--- _id: '12737' abstract: - lang: eng text: The substitution of heavier, more metallic atoms into classical organic ligand frameworks provides an important strategy for tuning ligand properties, such as ligand bite and donor character, and is the basis for the emerging area of main-group supramolecular chemistry. In this paper, we explore two new ligands [E(2-Me-8-qy)3] [E = Sb (1), Bi (2); qy = quinolyl], allowing a fundamental comparison of their coordination behavior with classical tris(2-pyridyl) ligands of the type [E′(2-py)3] (E = a range of bridgehead atoms and groups, py = pyridyl). A range of new coordination modes to Cu+, Ag+, and Au+ is seen for 1 and 2, in the absence of steric constraints at the bridgehead and with their more remote N-donor atoms. A particular feature is the adaptive nature of these new ligands, with the ability to adjust coordination mode in response to the hard–soft character of coordinated metal ions, influenced also by the character of the bridgehead atom (Sb or Bi). These features can be seen in a comparison between [Cu2{Sb(2-Me-8-qy)3}2](PF6)2 (1·CuPF6) and [Cu{Bi(2-Me-8-qy)3}](PF6) (2·CuPF6), the first containing a dimeric cation in which 1 adopts an unprecedented intramolecular N,N,Sb-coordination mode while in the second, 2 adopts an unusual N,N,(π-)C coordination mode. In contrast, the previously reported analogous ligands [E(6-Me-2-py)3] (E = Sb, Bi; 2-py = 2-pyridyl) show a tris-chelating mode in their complexes with CuPF6, which is typical for the extensive tris(2-pyridyl) family with a range of metals. The greater polarity of the Bi–C bond in 2 results in ligand transfer reactions with Au(I). Although this reactivity is not in itself unusual, the characterization of several products by single-crystal X-ray diffraction provides snapshots of the ligand transfer reaction involved, with one of the products (the bimetallic complex [(BiCl){ClAu2(2-Me-8-qy)3}] (8)) containing a Au2Bi core in which the shortest Au → Bi donor–acceptor bond to date is observed. acknowledgement: The authors thank the Walters-Kundert Studentship of Selwyn College (scholarship for J.E.W.), the Leverhulme Trust (R.G.-R. and D.S.W., grant RPG-2017-146), the Australian Research Council (A.L.C., DE200100450), the Spanish Ministry of Science and Innovation (MCI) and the Spanish Ministry of Science, Innovation and Universities (MCIU) (R.G.-R., PID2021-124691NB-I00, funded by MCIN/AEI/10.13039/501100011033/FEDER, UE and PGC2018-096880-A-I00, MCIU/AEI/FEDER), The University of Valladolid and Santander Bank (Fellowship for A.G.-R.), and the U.K. EPSRC and The Royal Dutch Shell plc. (I-Case award for R.B.J., EP/R511870/1) for financial support. Calculations were carried out on an in-house Odyssey HPC cluster (Cambridge), and the authors are grateful for the calculation time used. article_processing_charge: No article_type: original author: - first_name: Álvaro full_name: García-Romero, Álvaro last_name: García-Romero - first_name: Jessica E. full_name: Waters, Jessica E. last_name: Waters - first_name: Rajesh B full_name: Jethwa, Rajesh B id: 4cc538d5-803f-11ed-ab7e-8139573aad8f last_name: Jethwa orcid: 0000-0002-0404-4356 - first_name: Andrew D. full_name: Bond, Andrew D. last_name: Bond - first_name: Annie L. full_name: Colebatch, Annie L. last_name: Colebatch - first_name: Raúl full_name: García-Rodríguez, Raúl last_name: García-Rodríguez - first_name: Dominic S. full_name: Wright, Dominic S. last_name: Wright citation: ama: García-Romero Á, Waters JE, Jethwa RB, et al. Highly adaptive nature of group 15 tris(quinolyl) ligands─studies with coinage metals. Inorganic Chemistry. 2023;62(11):4625-4636. doi:10.1021/acs.inorgchem.3c00057 apa: García-Romero, Á., Waters, J. E., Jethwa, R. B., Bond, A. D., Colebatch, A. L., García-Rodríguez, R., & Wright, D. S. (2023). Highly adaptive nature of group 15 tris(quinolyl) ligands─studies with coinage metals. Inorganic Chemistry. American Chemical Society. https://doi.org/10.1021/acs.inorgchem.3c00057 chicago: García-Romero, Álvaro, Jessica E. Waters, Rajesh B Jethwa, Andrew D. Bond, Annie L. Colebatch, Raúl García-Rodríguez, and Dominic S. Wright. “Highly Adaptive Nature of Group 15 Tris(Quinolyl) Ligands─studies with Coinage Metals.” Inorganic Chemistry. American Chemical Society, 2023. https://doi.org/10.1021/acs.inorgchem.3c00057. ieee: Á. García-Romero et al., “Highly adaptive nature of group 15 tris(quinolyl) ligands─studies with coinage metals,” Inorganic Chemistry, vol. 62, no. 11. American Chemical Society, pp. 4625–4636, 2023. ista: García-Romero Á, Waters JE, Jethwa RB, Bond AD, Colebatch AL, García-Rodríguez R, Wright DS. 2023. Highly adaptive nature of group 15 tris(quinolyl) ligands─studies with coinage metals. Inorganic Chemistry. 62(11), 4625–4636. mla: García-Romero, Álvaro, et al. “Highly Adaptive Nature of Group 15 Tris(Quinolyl) Ligands─studies with Coinage Metals.” Inorganic Chemistry, vol. 62, no. 11, American Chemical Society, 2023, pp. 4625–36, doi:10.1021/acs.inorgchem.3c00057. short: Á. García-Romero, J.E. Waters, R.B. Jethwa, A.D. Bond, A.L. Colebatch, R. García-Rodríguez, D.S. Wright, Inorganic Chemistry 62 (2023) 4625–4636. date_created: 2023-03-19T23:00:59Z date_published: 2023-03-08T00:00:00Z date_updated: 2023-08-01T13:42:59Z day: '08' department: - _id: StFr doi: 10.1021/acs.inorgchem.3c00057 external_id: isi: - '000956110300001' pmid: - '36883367' intvolume: ' 62' isi: 1 issue: '11' language: - iso: eng month: '03' oa_version: None page: 4625-4636 pmid: 1 publication: Inorganic Chemistry publication_identifier: eissn: - 1520-510X issn: - 0020-1669 publication_status: published publisher: American Chemical Society quality_controlled: '1' scopus_import: '1' status: public title: Highly adaptive nature of group 15 tris(quinolyl) ligands─studies with coinage metals type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 62 year: '2023' ... --- _id: '13041' abstract: - lang: eng text: A series of triarylamines was synthesised and screened for their suitability as catholytes in redox flow batteries using cyclic voltammetry (CV). Tris(4-aminophenyl)amine was found to be the strongest candidate. Solubility and initial electrochemical performance were promising; however, polymerisation was observed during electrochemical cycling leading to rapid capacity fade prescribed to a loss of accessible active material and the limitation of ion transport processes within the cell. A mixed electrolyte system of H3PO4 and HCl was found to inhibit polymerisation producing oligomers that consumed less active material reducing rates of degradation in the redox flow battery. Under these conditions Coulombic efficiency improved by over 4 %, the maximum number of cycles more than quadrupled and an additional theoretical capacity of 20 % was accessed. This paper is, to our knowledge, the first example of triarylamines as catholytes in all-aqueous redox flow batteries and emphasises the impact supporting electrolytes can have on electrochemical performance. acknowledgement: The authors (N.L.F and R.B.J) would like to acknowledge the funding contributions of Shell and the EPRSC via I–Case studentships (grants no. EP/V519662/1 and EP/R511870/1 respectively). T.I would like to thank the ERC advanced Investigator Grant for CPG (EC H2020 835073). Thank you to Zhen Wang from the University of Cambridge for measuring GPC, the Yusuf Hamied Department of Chemistry's mass spectrometry service for MS measurements and analysis and Dr Andrew Bond from the University of Cambridge for XRD measurement and analysis. article_number: e202300128 article_processing_charge: Yes (in subscription journal) article_type: original author: - first_name: Nadia L. full_name: Farag, Nadia L. last_name: Farag - first_name: Rajesh B full_name: Jethwa, Rajesh B id: 4cc538d5-803f-11ed-ab7e-8139573aad8f last_name: Jethwa orcid: 0000-0002-0404-4356 - first_name: Alice E. full_name: Beardmore, Alice E. last_name: Beardmore - first_name: Teresa full_name: Insinna, Teresa last_name: Insinna - first_name: Christopher A. full_name: O'Keefe, Christopher A. last_name: O'Keefe - first_name: Peter A.A. full_name: Klusener, Peter A.A. last_name: Klusener - first_name: Clare P. full_name: Grey, Clare P. last_name: Grey - first_name: Dominic S. full_name: Wright, Dominic S. last_name: Wright citation: ama: Farag NL, Jethwa RB, Beardmore AE, et al. Triarylamines as catholytes in aqueous organic redox flow batteries. ChemSusChem. 2023;16(13). doi:10.1002/cssc.202300128 apa: Farag, N. L., Jethwa, R. B., Beardmore, A. E., Insinna, T., O’Keefe, C. A., Klusener, P. A. A., … Wright, D. S. (2023). Triarylamines as catholytes in aqueous organic redox flow batteries. ChemSusChem. Wiley. https://doi.org/10.1002/cssc.202300128 chicago: Farag, Nadia L., Rajesh B Jethwa, Alice E. Beardmore, Teresa Insinna, Christopher A. O’Keefe, Peter A.A. Klusener, Clare P. Grey, and Dominic S. Wright. “Triarylamines as Catholytes in Aqueous Organic Redox Flow Batteries.” ChemSusChem. Wiley, 2023. https://doi.org/10.1002/cssc.202300128. ieee: N. L. Farag et al., “Triarylamines as catholytes in aqueous organic redox flow batteries,” ChemSusChem, vol. 16, no. 13. Wiley, 2023. ista: Farag NL, Jethwa RB, Beardmore AE, Insinna T, O’Keefe CA, Klusener PAA, Grey CP, Wright DS. 2023. Triarylamines as catholytes in aqueous organic redox flow batteries. ChemSusChem. 16(13), e202300128. mla: Farag, Nadia L., et al. “Triarylamines as Catholytes in Aqueous Organic Redox Flow Batteries.” ChemSusChem, vol. 16, no. 13, e202300128, Wiley, 2023, doi:10.1002/cssc.202300128. short: N.L. Farag, R.B. Jethwa, A.E. Beardmore, T. Insinna, C.A. O’Keefe, P.A.A. Klusener, C.P. Grey, D.S. Wright, ChemSusChem 16 (2023). date_created: 2023-05-21T22:01:05Z date_published: 2023-07-06T00:00:00Z date_updated: 2023-11-14T11:28:23Z day: '06' ddc: - '540' department: - _id: StFr doi: 10.1002/cssc.202300128 external_id: isi: - '000985051300001' pmid: - '36970847' file: - access_level: open_access checksum: efa0713289995af83a2147b3e8e1d6a6 content_type: application/pdf creator: dernst date_created: 2023-11-14T11:27:16Z date_updated: 2023-11-14T11:27:16Z file_id: '14532' file_name: 2023_ChemSusChem_Farag.pdf file_size: 1168683 relation: main_file success: 1 file_date_updated: 2023-11-14T11:27:16Z has_accepted_license: '1' intvolume: ' 16' isi: 1 issue: '13' language: - iso: eng month: '07' oa: 1 oa_version: Published Version pmid: 1 publication: ChemSusChem publication_identifier: eissn: - 1864-564X issn: - 1864-5631 publication_status: published publisher: Wiley quality_controlled: '1' scopus_import: '1' status: public title: Triarylamines as catholytes in aqueous organic redox flow batteries tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: journal_article user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 volume: 16 year: '2023' ... --- _id: '14701' article_processing_charge: No article_type: review author: - first_name: Lynden A. full_name: Archer, Lynden A. last_name: Archer - first_name: Peter G. full_name: Bruce, Peter G. last_name: Bruce - first_name: Ernesto J. full_name: Calvo, Ernesto J. last_name: Calvo - first_name: Daniel full_name: Dewar, Daniel last_name: Dewar - first_name: James H. J. full_name: Ellison, James H. J. last_name: Ellison - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Xiangwen full_name: Gao, Xiangwen last_name: Gao - first_name: Laurence J. full_name: Hardwick, Laurence J. last_name: Hardwick - first_name: Gabriela full_name: Horwitz, Gabriela last_name: Horwitz - first_name: Jürgen full_name: Janek, Jürgen last_name: Janek - first_name: Lee R. full_name: Johnson, Lee R. last_name: Johnson - first_name: Jack W. full_name: Jordan, Jack W. last_name: Jordan - first_name: Shoichi full_name: Matsuda, Shoichi last_name: Matsuda - first_name: Svetlana full_name: Menkin, Svetlana last_name: Menkin - first_name: Soumyadip full_name: Mondal, Soumyadip id: d25d21ef-dc8d-11ea-abe3-ec4576307f48 last_name: Mondal - first_name: Qianyuan full_name: Qiu, Qianyuan last_name: Qiu - first_name: Thukshan full_name: Samarakoon, Thukshan last_name: Samarakoon - first_name: Israel full_name: Temprano, Israel last_name: Temprano - first_name: Kohei full_name: Uosaki, Kohei last_name: Uosaki - first_name: Ganesh full_name: Vailaya, Ganesh last_name: Vailaya - first_name: Eric D. full_name: Wachsman, Eric D. last_name: Wachsman - first_name: Yiying full_name: Wu, Yiying last_name: Wu - first_name: Shen full_name: Ye, Shen last_name: Ye citation: ama: 'Archer LA, Bruce PG, Calvo EJ, et al. Towards practical metal–oxygen batteries: General discussion. Faraday Discussions. 2023. doi:10.1039/d3fd90062b' apa: 'Archer, L. A., Bruce, P. G., Calvo, E. J., Dewar, D., Ellison, J. H. J., Freunberger, S. A., … Ye, S. (2023). Towards practical metal–oxygen batteries: General discussion. Faraday Discussions. Royal Society of Chemistry. https://doi.org/10.1039/d3fd90062b' chicago: 'Archer, Lynden A., Peter G. Bruce, Ernesto J. Calvo, Daniel Dewar, James H. J. Ellison, Stefan Alexander Freunberger, Xiangwen Gao, et al. “Towards Practical Metal–Oxygen Batteries: General Discussion.” Faraday Discussions. Royal Society of Chemistry, 2023. https://doi.org/10.1039/d3fd90062b.' ieee: 'L. A. Archer et al., “Towards practical metal–oxygen batteries: General discussion,” Faraday Discussions. Royal Society of Chemistry, 2023.' ista: 'Archer LA, Bruce PG, Calvo EJ, Dewar D, Ellison JHJ, Freunberger SA, Gao X, Hardwick LJ, Horwitz G, Janek J, Johnson LR, Jordan JW, Matsuda S, Menkin S, Mondal S, Qiu Q, Samarakoon T, Temprano I, Uosaki K, Vailaya G, Wachsman ED, Wu Y, Ye S. 2023. Towards practical metal–oxygen batteries: General discussion. Faraday Discussions.' mla: 'Archer, Lynden A., et al. “Towards Practical Metal–Oxygen Batteries: General Discussion.” Faraday Discussions, Royal Society of Chemistry, 2023, doi:10.1039/d3fd90062b.' short: L.A. Archer, P.G. Bruce, E.J. Calvo, D. Dewar, J.H.J. Ellison, S.A. Freunberger, X. Gao, L.J. Hardwick, G. Horwitz, J. Janek, L.R. Johnson, J.W. Jordan, S. Matsuda, S. Menkin, S. Mondal, Q. Qiu, T. Samarakoon, I. Temprano, K. Uosaki, G. Vailaya, E.D. Wachsman, Y. Wu, S. Ye, Faraday Discussions (2023). date_created: 2023-12-20T10:48:09Z date_published: 2023-12-19T00:00:00Z date_updated: 2023-12-20T11:54:06Z day: '19' department: - _id: StFr doi: 10.1039/d3fd90062b keyword: - Physical and Theoretical Chemistry language: - iso: eng month: '12' oa_version: None publication: Faraday Discussions publication_identifier: eissn: - 1364-5498 issn: - 1359-6640 publication_status: epub_ahead publisher: Royal Society of Chemistry quality_controlled: '1' status: public title: 'Towards practical metal–oxygen batteries: General discussion' type: journal_article user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 year: '2023' ... --- _id: '14702' article_processing_charge: No article_type: review author: - first_name: Gary A. full_name: Attard, Gary A. last_name: Attard - first_name: Ernesto J. full_name: Calvo, Ernesto J. last_name: Calvo - first_name: Larry A. full_name: Curtiss, Larry A. last_name: Curtiss - first_name: Daniel full_name: Dewar, Daniel last_name: Dewar - first_name: James H. J. full_name: Ellison, James H. J. last_name: Ellison - first_name: Xiangwen full_name: Gao, Xiangwen last_name: Gao - first_name: Clare P. full_name: Grey, Clare P. last_name: Grey - first_name: Laurence J. full_name: Hardwick, Laurence J. last_name: Hardwick - first_name: Gabriela full_name: Horwitz, Gabriela last_name: Horwitz - first_name: Juergen full_name: Janek, Juergen last_name: Janek - first_name: Lee R. full_name: Johnson, Lee R. last_name: Johnson - first_name: Jack W. full_name: Jordan, Jack W. last_name: Jordan - first_name: Shoichi full_name: Matsuda, Shoichi last_name: Matsuda - first_name: Soumyadip full_name: Mondal, Soumyadip id: d25d21ef-dc8d-11ea-abe3-ec4576307f48 last_name: Mondal - first_name: Alex R. full_name: Neale, Alex R. last_name: Neale - first_name: Nagore full_name: Ortiz-Vitoriano, Nagore last_name: Ortiz-Vitoriano - first_name: Israel full_name: Temprano, Israel last_name: Temprano - first_name: Ganesh full_name: Vailaya, Ganesh last_name: Vailaya - first_name: Eric D. full_name: Wachsman, Eric D. last_name: Wachsman - first_name: Hsien-Hau full_name: Wang, Hsien-Hau last_name: Wang - first_name: Yiying full_name: Wu, Yiying last_name: Wu - first_name: Shen full_name: Ye, Shen last_name: Ye citation: ama: 'Attard GA, Calvo EJ, Curtiss LA, et al. Materials for stable metal–oxygen battery cathodes: general discussion. Faraday Discussions. 2023. doi:10.1039/d3fd90059b' apa: 'Attard, G. A., Calvo, E. J., Curtiss, L. A., Dewar, D., Ellison, J. H. J., Gao, X., … Ye, S. (2023). Materials for stable metal–oxygen battery cathodes: general discussion. Faraday Discussions. Royal Society of Chemistry. https://doi.org/10.1039/d3fd90059b' chicago: 'Attard, Gary A., Ernesto J. Calvo, Larry A. Curtiss, Daniel Dewar, James H. J. Ellison, Xiangwen Gao, Clare P. Grey, et al. “Materials for Stable Metal–Oxygen Battery Cathodes: General Discussion.” Faraday Discussions. Royal Society of Chemistry, 2023. https://doi.org/10.1039/d3fd90059b.' ieee: 'G. A. Attard et al., “Materials for stable metal–oxygen battery cathodes: general discussion,” Faraday Discussions. Royal Society of Chemistry, 2023.' ista: 'Attard GA, Calvo EJ, Curtiss LA, Dewar D, Ellison JHJ, Gao X, Grey CP, Hardwick LJ, Horwitz G, Janek J, Johnson LR, Jordan JW, Matsuda S, Mondal S, Neale AR, Ortiz-Vitoriano N, Temprano I, Vailaya G, Wachsman ED, Wang H-H, Wu Y, Ye S. 2023. Materials for stable metal–oxygen battery cathodes: general discussion. Faraday Discussions.' mla: 'Attard, Gary A., et al. “Materials for Stable Metal–Oxygen Battery Cathodes: General Discussion.” Faraday Discussions, Royal Society of Chemistry, 2023, doi:10.1039/d3fd90059b.' short: G.A. Attard, E.J. Calvo, L.A. Curtiss, D. Dewar, J.H.J. Ellison, X. Gao, C.P. Grey, L.J. Hardwick, G. Horwitz, J. Janek, L.R. Johnson, J.W. Jordan, S. Matsuda, S. Mondal, A.R. Neale, N. Ortiz-Vitoriano, I. Temprano, G. Vailaya, E.D. Wachsman, H.-H. Wang, Y. Wu, S. Ye, Faraday Discussions (2023). date_created: 2023-12-20T10:49:43Z date_published: 2023-12-18T00:00:00Z date_updated: 2023-12-20T11:58:12Z day: '18' department: - _id: StFr doi: 10.1039/d3fd90059b keyword: - Physical and Theoretical Chemistry language: - iso: eng month: '12' oa_version: None publication: Faraday Discussions publication_identifier: eissn: - 1364-5498 issn: - 1359-6640 publication_status: epub_ahead publisher: Royal Society of Chemistry quality_controlled: '1' status: public title: 'Materials for stable metal–oxygen battery cathodes: general discussion' type: journal_article user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 year: '2023' ... --- _id: '14733' abstract: - lang: eng text: Redox flow batteries (RFBs) rely on the development of cheap, highly soluble, and high-energy-density electrolytes. Several candidate quinones have already been investigated in the literature as two-electron anolytes or catholytes, benefiting from fast kinetics, high tunability, and low cost. Here, an investigation of nitrogen-rich fused heteroaromatic quinones was carried out to explore avenues for electrolyte development. These quinones were synthesized and screened by using electrochemical techniques. The most promising candidate, 4,8-dioxo-4,8-dihydrobenzo[1,2-d:4,5-d′]bis([1,2,3]triazole)-1,5-diide (−0.68 V(SHE)), was tested in both an asymmetric and symmetric full-cell setup resulting in capacity fade rates of 0.35% per cycle and 0.0124% per cycle, respectively. In situ ultraviolet-visible spectroscopy (UV–Vis), nuclear magnetic resonance (NMR), and electron paramagnetic resonance (EPR) spectroscopies were used to investigate the electrochemical stability of the charged species during operation. UV–Vis spectroscopy, supported by density functional theory (DFT) modeling, reaffirmed that the two-step charging mechanism observed during battery operation consisted of two, single-electron transfers. The radical concentration during battery operation and the degree of delocalization of the unpaired electron were quantified with NMR and EPR spectroscopy. article_processing_charge: Yes (in subscription journal) article_type: original author: - first_name: Rajesh B full_name: Jethwa, Rajesh B id: 4cc538d5-803f-11ed-ab7e-8139573aad8f last_name: Jethwa orcid: 0000-0002-0404-4356 - first_name: Dominic full_name: Hey, Dominic last_name: Hey - first_name: Rachel N. full_name: Kerber, Rachel N. last_name: Kerber - first_name: Andrew D. full_name: Bond, Andrew D. last_name: Bond - first_name: Dominic S. full_name: Wright, Dominic S. last_name: Wright - first_name: Clare P. full_name: Grey, Clare P. last_name: Grey citation: ama: Jethwa RB, Hey D, Kerber RN, Bond AD, Wright DS, Grey CP. Exploring the landscape of heterocyclic quinones for redox flow batteries. ACS Applied Energy Materials. 2023. doi:10.1021/acsaem.3c02223 apa: Jethwa, R. B., Hey, D., Kerber, R. N., Bond, A. D., Wright, D. S., & Grey, C. P. (2023). Exploring the landscape of heterocyclic quinones for redox flow batteries. ACS Applied Energy Materials. American Chemical Society. https://doi.org/10.1021/acsaem.3c02223 chicago: Jethwa, Rajesh B, Dominic Hey, Rachel N. Kerber, Andrew D. Bond, Dominic S. Wright, and Clare P. Grey. “Exploring the Landscape of Heterocyclic Quinones for Redox Flow Batteries.” ACS Applied Energy Materials. American Chemical Society, 2023. https://doi.org/10.1021/acsaem.3c02223. ieee: R. B. Jethwa, D. Hey, R. N. Kerber, A. D. Bond, D. S. Wright, and C. P. Grey, “Exploring the landscape of heterocyclic quinones for redox flow batteries,” ACS Applied Energy Materials. American Chemical Society, 2023. ista: Jethwa RB, Hey D, Kerber RN, Bond AD, Wright DS, Grey CP. 2023. Exploring the landscape of heterocyclic quinones for redox flow batteries. ACS Applied Energy Materials. mla: Jethwa, Rajesh B., et al. “Exploring the Landscape of Heterocyclic Quinones for Redox Flow Batteries.” ACS Applied Energy Materials, American Chemical Society, 2023, doi:10.1021/acsaem.3c02223. short: R.B. Jethwa, D. Hey, R.N. Kerber, A.D. Bond, D.S. Wright, C.P. Grey, ACS Applied Energy Materials (2023). date_created: 2024-01-05T09:20:48Z date_published: 2023-12-28T00:00:00Z date_updated: 2024-01-08T09:03:01Z day: '28' ddc: - '540' department: - _id: StFr doi: 10.1021/acsaem.3c02223 ec_funded: 1 has_accepted_license: '1' keyword: - Electrical and Electronic Engineering - Materials Chemistry - Electrochemistry - Energy Engineering and Power Technology - Chemical Engineering (miscellaneous) language: - iso: eng main_file_link: - open_access: '1' url: https://doi.org/10.1021/acsaem.3c02223 month: '12' oa: 1 oa_version: Published Version project: - _id: fc2ed2f7-9c52-11eb-aca3-c01059dda49c call_identifier: H2020 grant_number: '101034413' name: 'IST-BRIDGE: International postdoctoral program' publication: ACS Applied Energy Materials publication_identifier: eissn: - 2574-0962 publication_status: epub_ahead publisher: American Chemical Society quality_controlled: '1' status: public title: Exploring the landscape of heterocyclic quinones for redox flow batteries tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: journal_article user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 year: '2023' ... --- _id: '14687' abstract: - lang: eng text: The short history of research on Li-O2 batteries has seen a remarkable number of mechanistic U-turns over the years. From the initial use of carbonate electrolytes, that were then found to be entirely unsuitable, to the belief that (su)peroxide was solely responsible for degradation, before the more reactive singlet oxygen was found to form, to the hypothesis that capacity depends on a competing surface/solution mechanism before a practically exclusive solution mechanism was identified. Herein, we argue for an ever-fresh look at the reported data without bias towards supposedly established explanations. We explain how the latest findings on rate and capacity limits, as well as the origin of side reactions, are connected via the disproportionation (DISP) step in the (dis)charge mechanism. Therefrom, directions emerge for the design of electrolytes and mediators on how to suppress side reactions and to enable high rate and high reversible capacity. article_number: e202316476 article_processing_charge: Yes (via OA deal) article_type: review author: - first_name: Rajesh B full_name: Jethwa, Rajesh B id: 4cc538d5-803f-11ed-ab7e-8139573aad8f last_name: Jethwa orcid: 0000-0002-0404-4356 - first_name: Soumyadip full_name: Mondal, Soumyadip id: d25d21ef-dc8d-11ea-abe3-ec4576307f48 last_name: Mondal - first_name: Bhargavi full_name: Pant, Bhargavi id: 50c64d4d-eb97-11eb-a6c2-d33e5e14f112 last_name: Pant - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Jethwa RB, Mondal S, Pant B, Freunberger SA. To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries. Angewandte Chemie International Edition. 2023. doi:10.1002/anie.202316476 apa: Jethwa, R. B., Mondal, S., Pant, B., & Freunberger, S. A. (2023). To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries. Angewandte Chemie International Edition. Wiley. https://doi.org/10.1002/anie.202316476 chicago: Jethwa, Rajesh B, Soumyadip Mondal, Bhargavi Pant, and Stefan Alexander Freunberger. “To DISP or Not? The Far‐reaching Reaction Mechanisms Underpinning Lithium‐air Batteries.” Angewandte Chemie International Edition. Wiley, 2023. https://doi.org/10.1002/anie.202316476. ieee: R. B. Jethwa, S. Mondal, B. Pant, and S. A. Freunberger, “To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries,” Angewandte Chemie International Edition. Wiley, 2023. ista: Jethwa RB, Mondal S, Pant B, Freunberger SA. 2023. To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries. Angewandte Chemie International Edition., e202316476. mla: Jethwa, Rajesh B., et al. “To DISP or Not? The Far‐reaching Reaction Mechanisms Underpinning Lithium‐air Batteries.” Angewandte Chemie International Edition, e202316476, Wiley, 2023, doi:10.1002/anie.202316476. short: R.B. Jethwa, S. Mondal, B. Pant, S.A. Freunberger, Angewandte Chemie International Edition (2023). date_created: 2023-12-15T16:10:13Z date_published: 2023-12-14T00:00:00Z date_updated: 2024-02-15T14:43:05Z day: '14' department: - _id: StFr - _id: GradSch doi: 10.1002/anie.202316476 keyword: - General Chemistry - Catalysis language: - iso: eng main_file_link: - open_access: '1' url: ' https://doi.org/10.1002/anie.202316476' month: '12' oa: 1 oa_version: Published Version publication: Angewandte Chemie International Edition publication_identifier: eissn: - 1521-3773 issn: - 1433-7851 publication_status: epub_ahead publisher: Wiley quality_controlled: '1' scopus_import: '1' status: public title: To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries type: journal_article user_id: 3E5EF7F0-F248-11E8-B48F-1D18A9856A87 year: '2023' ... --- _id: '13044' abstract: - lang: eng text: Singlet oxygen (1O2) formation is now recognised as a key aspect of non-aqueous oxygen redox chemistry. For identifying 1O2, chemical trapping via 9,10-dimethylanthracene (DMA) to form the endoperoxide (DMA-O2) has become the mainstay method due to its sensitivity, selectivity, and ease of use. While DMA has been shown to be selective for 1O2, rather than forming DMA-O2 with a wide variety of potentially reactive O-containing species, false positives might hypothetically be obtained in the presence of previously overlooked species. Here, we first give unequivocal direct spectroscopic proof by the 1O2-specific near infrared (NIR) emission at 1270 nm for the previously proposed 1O2 formation pathways, which centre around superoxide disproportionation. We then show that peroxocarbonates, common intermediates in metal-O2 and metal carbonate electrochemistry, do not produce false-positive DMA-O2. Moreover, we identify a previously unreported 1O2-forming pathway through the reaction of CO2 with superoxide. Overall, we give unequivocal proof for 1O2 formation in non-aqueous oxygen redox and show that chemical trapping with DMA is a reliable method to assess 1O2 formation. article_processing_charge: Yes (via OA deal) article_type: original author: - first_name: Soumyadip full_name: Mondal, Soumyadip id: d25d21ef-dc8d-11ea-abe3-ec4576307f48 last_name: Mondal - first_name: Rajesh B full_name: Jethwa, Rajesh B id: 4cc538d5-803f-11ed-ab7e-8139573aad8f last_name: Jethwa orcid: 0000-0002-0404-4356 - first_name: Bhargavi full_name: Pant, Bhargavi id: 50c64d4d-eb97-11eb-a6c2-d33e5e14f112 last_name: Pant - first_name: Robert full_name: Hauschild, Robert id: 4E01D6B4-F248-11E8-B48F-1D18A9856A87 last_name: Hauschild orcid: 0000-0001-9843-3522 - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: 'Mondal S, Jethwa RB, Pant B, Hauschild R, Freunberger SA. Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways and reliability of chemical probes. Faraday Discussions. 2023. doi:10.1039/d3fd00088e' apa: 'Mondal, S., Jethwa, R. B., Pant, B., Hauschild, R., & Freunberger, S. A. (2023). Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways and reliability of chemical probes. Faraday Discussions. Royal Society of Chemistry. https://doi.org/10.1039/d3fd00088e' chicago: 'Mondal, Soumyadip, Rajesh B Jethwa, Bhargavi Pant, Robert Hauschild, and Stefan Alexander Freunberger. “Singlet Oxygen in Non-Aqueous Oxygen Redox: Direct Spectroscopic Evidence for Formation Pathways and Reliability of Chemical Probes.” Faraday Discussions. Royal Society of Chemistry, 2023. https://doi.org/10.1039/d3fd00088e.' ieee: 'S. Mondal, R. B. Jethwa, B. Pant, R. Hauschild, and S. A. Freunberger, “Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways and reliability of chemical probes,” Faraday Discussions. Royal Society of Chemistry, 2023.' ista: 'Mondal S, Jethwa RB, Pant B, Hauschild R, Freunberger SA. 2023. Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways and reliability of chemical probes. Faraday Discussions.' mla: 'Mondal, Soumyadip, et al. “Singlet Oxygen in Non-Aqueous Oxygen Redox: Direct Spectroscopic Evidence for Formation Pathways and Reliability of Chemical Probes.” Faraday Discussions, Royal Society of Chemistry, 2023, doi:10.1039/d3fd00088e.' short: S. Mondal, R.B. Jethwa, B. Pant, R. Hauschild, S.A. Freunberger, Faraday Discussions (2023). date_created: 2023-05-22T06:53:34Z date_published: 2023-05-17T00:00:00Z date_updated: 2024-03-20T13:10:00Z day: '17' department: - _id: StFr - _id: Bio doi: 10.1039/d3fd00088e external_id: isi: - '001070423500001' isi: 1 keyword: - Physical and Theoretical Chemistry language: - iso: eng main_file_link: - open_access: '1' url: https://doi.org/10.1039/d3fd00088e month: '05' oa: 1 oa_version: Published Version publication: Faraday Discussions publication_identifier: eissn: - 1364-5498 issn: - 1359-6640 publication_status: epub_ahead publisher: Royal Society of Chemistry quality_controlled: '1' status: public title: 'Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways and reliability of chemical probes' tmp: image: /images/cc_by_nc.png legal_code_url: https://creativecommons.org/licenses/by-nc/4.0/legalcode name: Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0) short: CC BY-NC (4.0) type: journal_article user_id: 3E5EF7F0-F248-11E8-B48F-1D18A9856A87 year: '2023' ... --- _id: '12065' abstract: - lang: eng text: Capacity, rate performance, and cycle life of aprotic Li–O2 batteries critically depend on reversible electrodeposition of Li2O2. Current understanding states surface-adsorbed versus solvated LiO2 controls Li2O2 growth as surface film or as large particles. Herein, we show that Li2O2 forms across a wide range of electrolytes, carbons, and current densities as particles via solution-mediated LiO2 disproportionation, bringing into question the prevalence of any surface growth under practical conditions. We describe a unified O2 reduction mechanism, which can explain all found capacity relations and Li2O2 morphologies with exclusive solution discharge. Determining particle morphology and achievable capacities are species mobilities, true areal rate, and the degree of LiO2 association in solution. Capacity is conclusively limited by mass transport through the tortuous Li2O2 rather than electron transport through a passivating Li2O2 film. Provided that species mobilities and surface growth are high, high capacities are also achieved with weakly solvating electrolytes, which were previously considered prototypical for low capacity via surface growth. acknowledged_ssus: - _id: EM-Fac - _id: M-Shop acknowledgement: S.A.F. and C.P. are indebted to the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 636069). This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant NanoEvolution, Grant Agreement No. 894042. S.A.F. and S.M. are indebted to Institute of Science and Technology Austria (ISTA) for support. This research was supported by the Scientific Service Units of ISTA through resources provided by the Electron Microscopy Facility and the Miba Machine Shop. C.P. thanks Vanessa Wood (ETH Zürich) for her continuing support. article_processing_charge: Yes (via OA deal) article_type: original author: - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Soumyadip full_name: Mondal, Soumyadip id: d25d21ef-dc8d-11ea-abe3-ec4576307f48 last_name: Mondal - first_name: Ludek full_name: Lovicar, Ludek id: 36DB3A20-F248-11E8-B48F-1D18A9856A87 last_name: Lovicar - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Prehal C, Mondal S, Lovicar L, Freunberger SA. Exclusive solution discharge in Li-O₂ batteries? ACS Energy Letters. 2022;7(9):3112-3119. doi:10.1021/acsenergylett.2c01711 apa: Prehal, C., Mondal, S., Lovicar, L., & Freunberger, S. A. (2022). Exclusive solution discharge in Li-O₂ batteries? ACS Energy Letters. American Chemical Society. https://doi.org/10.1021/acsenergylett.2c01711 chicago: Prehal, Christian, Soumyadip Mondal, Ludek Lovicar, and Stefan Alexander Freunberger. “Exclusive Solution Discharge in Li-O₂ Batteries?” ACS Energy Letters. American Chemical Society, 2022. https://doi.org/10.1021/acsenergylett.2c01711. ieee: C. Prehal, S. Mondal, L. Lovicar, and S. A. Freunberger, “Exclusive solution discharge in Li-O₂ batteries?,” ACS Energy Letters, vol. 7, no. 9. American Chemical Society, pp. 3112–3119, 2022. ista: Prehal C, Mondal S, Lovicar L, Freunberger SA. 2022. Exclusive solution discharge in Li-O₂ batteries? ACS Energy Letters. 7(9), 3112–3119. mla: Prehal, Christian, et al. “Exclusive Solution Discharge in Li-O₂ Batteries?” ACS Energy Letters, vol. 7, no. 9, American Chemical Society, 2022, pp. 3112–19, doi:10.1021/acsenergylett.2c01711. short: C. Prehal, S. Mondal, L. Lovicar, S.A. Freunberger, ACS Energy Letters 7 (2022) 3112–3119. date_created: 2022-09-08T09:51:09Z date_published: 2022-08-29T00:00:00Z date_updated: 2023-08-03T13:47:56Z day: '29' ddc: - '540' department: - _id: StFr - _id: EM-Fac doi: 10.1021/acsenergylett.2c01711 external_id: isi: - '000860787000001' file: - access_level: open_access checksum: cf0bed3a2535c11d27244cd029dbc1d0 content_type: application/pdf creator: dernst date_created: 2023-01-20T08:43:51Z date_updated: 2023-01-20T08:43:51Z file_id: '12319' file_name: 2022_ACSEnergyLetters_Prehal.pdf file_size: 3827583 relation: main_file success: 1 file_date_updated: 2023-01-20T08:43:51Z has_accepted_license: '1' intvolume: ' 7' isi: 1 issue: '9' language: - iso: eng month: '08' oa: 1 oa_version: Published Version page: 3112-3119 publication: ACS Energy Letters publication_identifier: eissn: - 2380-8195 publication_status: published publisher: American Chemical Society quality_controlled: '1' scopus_import: '1' status: public title: Exclusive solution discharge in Li-O₂ batteries? tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 7 year: '2022' ... --- _id: '12208' abstract: - lang: eng text: The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li2S) via soluble polysulfides (PSs) formation impedes the development of high-performance lithium-sulfur (Li-S) batteries with non-aqueous electrolyte solutions. Here, we use operando small and wide angle X-ray scattering and operando small angle neutron scattering (SANS) measurements to track the nucleation, growth and dissolution of solid deposits from atomic to sub-micron scales during real-time Li-S cell operation. In particular, stochastic modelling based on the SANS data allows quantifying the nanoscale phase evolution during battery cycling. We show that next to nano-crystalline Li2S the deposit comprises solid short-chain PSs particles. The analysis of the experimental data suggests that initially, Li2S2 precipitates from the solution and then is partially converted via solid-state electroreduction to Li2S. We further demonstrate that mass transport, rather than electron transport through a thin passivating film, limits the discharge capacity and rate performance in Li-S cells. acknowledgement: "This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant NanoEvolution, grant agreement No 894042. The authors acknowledge the CERIC-ERIC Consortium for the access to the Austrian SAXS beamline and TU Graz for support through the Lead Project LP-03.\r\nLikewise, the use of SOMAPP Lab, a core facility supported by the Austrian Federal Ministry of Education, Science and Research, the Graz University of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. In addition, the authors acknowledge access to the D-22SANS beamline at the ILL neutron source. Electron microscopy measurements were performed at the Scientific Scenter for Optical and Electron Microscopy (ScopeM) of the Swiss Federal Institute of Technology. C.P. and J.M.M. thank A. Senol for her support with the SANS\r\nbeamtime preparation. S.D.T, A.V. and R.D. acknowledge the financial support by the Slovenian Research Agency (ARRS) research core funding P2-0393 and P2-0423. Furthermore, A.V. acknowledge the funding from the Slovenian Research Agency, research project Z2−1863.\r\nS.A.F. is indebted to IST Austria for support. " article_number: '6326' article_processing_charge: No article_type: original author: - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Jean-Marc full_name: von Mentlen, Jean-Marc last_name: von Mentlen - first_name: Sara full_name: Drvarič Talian, Sara last_name: Drvarič Talian - first_name: Alen full_name: Vizintin, Alen last_name: Vizintin - first_name: Robert full_name: Dominko, Robert last_name: Dominko - first_name: Heinz full_name: Amenitsch, Heinz last_name: Amenitsch - first_name: Lionel full_name: Porcar, Lionel last_name: Porcar - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Vanessa full_name: Wood, Vanessa last_name: Wood citation: ama: Prehal C, von Mentlen J-M, Drvarič Talian S, et al. On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering. Nature Communications. 2022;13. doi:10.1038/s41467-022-33931-4 apa: Prehal, C., von Mentlen, J.-M., Drvarič Talian, S., Vizintin, A., Dominko, R., Amenitsch, H., … Wood, V. (2022). On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering. Nature Communications. Springer Nature. https://doi.org/10.1038/s41467-022-33931-4 chicago: Prehal, Christian, Jean-Marc von Mentlen, Sara Drvarič Talian, Alen Vizintin, Robert Dominko, Heinz Amenitsch, Lionel Porcar, Stefan Alexander Freunberger, and Vanessa Wood. “On the Nanoscale Structural Evolution of Solid Discharge Products in Lithium-Sulfur Batteries Using Operando Scattering.” Nature Communications. Springer Nature, 2022. https://doi.org/10.1038/s41467-022-33931-4. ieee: C. Prehal et al., “On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering,” Nature Communications, vol. 13. Springer Nature, 2022. ista: Prehal C, von Mentlen J-M, Drvarič Talian S, Vizintin A, Dominko R, Amenitsch H, Porcar L, Freunberger SA, Wood V. 2022. On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering. Nature Communications. 13, 6326. mla: Prehal, Christian, et al. “On the Nanoscale Structural Evolution of Solid Discharge Products in Lithium-Sulfur Batteries Using Operando Scattering.” Nature Communications, vol. 13, 6326, Springer Nature, 2022, doi:10.1038/s41467-022-33931-4. short: C. Prehal, J.-M. von Mentlen, S. Drvarič Talian, A. Vizintin, R. Dominko, H. Amenitsch, L. Porcar, S.A. Freunberger, V. Wood, Nature Communications 13 (2022). date_created: 2023-01-16T09:45:09Z date_published: 2022-10-24T00:00:00Z date_updated: 2023-08-04T09:15:31Z day: '24' ddc: - '540' department: - _id: StFr doi: 10.1038/s41467-022-33931-4 external_id: isi: - '000871563700006' pmid: - '36280671' file: - access_level: open_access checksum: 5034336dbf0f860030ef745c08df9e0e content_type: application/pdf creator: dernst date_created: 2023-01-27T07:19:11Z date_updated: 2023-01-27T07:19:11Z file_id: '12411' file_name: 2022_NatureCommunications_Prehal.pdf file_size: 4216931 relation: main_file success: 1 file_date_updated: 2023-01-27T07:19:11Z has_accepted_license: '1' intvolume: ' 13' isi: 1 keyword: - General Physics and Astronomy - General Biochemistry - Genetics and Molecular Biology - General Chemistry - Multidisciplinary language: - iso: eng month: '10' oa: 1 oa_version: Published Version pmid: 1 publication: Nature Communications publication_identifier: issn: - 2041-1723 publication_status: published publisher: Springer Nature quality_controlled: '1' scopus_import: '1' status: public title: On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 13 year: '2022' ... --- _id: '12227' abstract: - lang: eng text: Polydicyclopentadiene (pDCPD), a thermoset with excellent mechanical properties, has enormous potential as a lightweight, tough, and stable matrix material owing to its highly cross-linked macromolecular network. This work describes generating pDCPD-based foams and hierarchically porous carbons derived therefrom by combining ring-opening metathesis polymerization (ROMP) of DCPD, high internal phase emulsions (HIPEs) as structural templates, and subsequent carbonization. The structure and function of the carbon foams were characterized and discussed in detail using scanning electron, transmission electron, or atomic force microscopy (SEM, TEM, AFM), electron energy-loss spectroscopy (TEM-EELS), N2 sorption, and analyses of electrical conductivity as well as mechanical properties. The resulting materials exhibited uniform, shape-retaining shrinkage of only ∼1/3 after carbonization. No structural failure was observed even when the pDCPD precursor foams were heated to 1400 °C. Instead, the high porosity, void size, and 3D interconnectivity were fully preserved, and the void diameters could be adjusted between 87 and 2.5 μm. Moreover, foams have a carbon content >97%, an electronic conductivity of up to 2800 S·m–1, a Young’s modulus of up to 2.1 GPa, and a specific surface area of up to 1200 m2·g–1. Surprisingly, the pDCPD foams were carbonized into shapes other than monoliths, such as 10’s of micron thick membranes or foamy coatings adhered to a metal foil or grid substrate. The latter coatings even adhere upon bending. Finally, as a use case, carbonized foams were applied as porous cathodes for Li–O2 batteries where the foams show a favorable combination of porosity, active surface area, and pore size for outstanding capacity. acknowledgement: S.K. acknowledges the financial support from the Slovenian Research Agency (grants P1-0021, P2-0150). Support by Graz University of Technology (LP-03 – Porous Materials@Work) and from VARTA Innovation GmbH is kindly acknowledged. We thank Umicore for providing the initiator and Matjaž Mazaj (National Institute of Chemistry, Ljubljana) and Karel Jerabek (Czech Academy of Sciences) for measurements and fruitful discussions. S.A.F. is indebted to the Austrian Federal Ministry of Science, Research and Economy; the Austrian Research Promotion Agency (Grant No. 845364); and ISTA for support. article_processing_charge: No article_type: original author: - first_name: Sebastijan full_name: Kovačič, Sebastijan last_name: Kovačič - first_name: Bettina full_name: Schafzahl, Bettina last_name: Schafzahl - first_name: Nadejda B. full_name: Matsko, Nadejda B. last_name: Matsko - first_name: Katharina full_name: Gruber, Katharina last_name: Gruber - first_name: Martin full_name: Schmuck, Martin last_name: Schmuck - first_name: Stefan full_name: Koller, Stefan last_name: Koller - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Christian full_name: Slugovc, Christian last_name: Slugovc citation: ama: 'Kovačič S, Schafzahl B, Matsko NB, et al. Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications. ACS Applied Energy Materials. 2022;5(11):14381-14390. doi:10.1021/acsaem.2c02787' apa: 'Kovačič, S., Schafzahl, B., Matsko, N. B., Gruber, K., Schmuck, M., Koller, S., … Slugovc, C. (2022). Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications. ACS Applied Energy Materials. American Chemical Society. https://doi.org/10.1021/acsaem.2c02787' chicago: 'Kovačič, Sebastijan, Bettina Schafzahl, Nadejda B. Matsko, Katharina Gruber, Martin Schmuck, Stefan Koller, Stefan Alexander Freunberger, and Christian Slugovc. “Carbon Foams via Ring-Opening Metathesis Polymerization of Emulsion Templates: A Facile Method to Make Carbon Current Collectors for Battery Applications.” ACS Applied Energy Materials. American Chemical Society, 2022. https://doi.org/10.1021/acsaem.2c02787.' ieee: 'S. Kovačič et al., “Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications,” ACS Applied Energy Materials, vol. 5, no. 11. American Chemical Society, pp. 14381–14390, 2022.' ista: 'Kovačič S, Schafzahl B, Matsko NB, Gruber K, Schmuck M, Koller S, Freunberger SA, Slugovc C. 2022. Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications. ACS Applied Energy Materials. 5(11), 14381–14390.' mla: 'Kovačič, Sebastijan, et al. “Carbon Foams via Ring-Opening Metathesis Polymerization of Emulsion Templates: A Facile Method to Make Carbon Current Collectors for Battery Applications.” ACS Applied Energy Materials, vol. 5, no. 11, American Chemical Society, 2022, pp. 14381–90, doi:10.1021/acsaem.2c02787.' short: S. Kovačič, B. Schafzahl, N.B. Matsko, K. Gruber, M. Schmuck, S. Koller, S.A. Freunberger, C. Slugovc, ACS Applied Energy Materials 5 (2022) 14381–14390. date_created: 2023-01-16T09:48:53Z date_published: 2022-10-16T00:00:00Z date_updated: 2023-08-04T09:27:32Z day: '16' ddc: - '540' department: - _id: StFr doi: 10.1021/acsaem.2c02787 external_id: isi: - '000875635900001' file: - access_level: open_access checksum: 572d15c250ab83d44f4e2c3aeb5f7388 content_type: application/pdf creator: dernst date_created: 2023-01-27T09:09:15Z date_updated: 2023-01-27T09:09:15Z file_id: '12420' file_name: 2022_AppliedEnergyMaterials_Kovacic.pdf file_size: 13105589 relation: main_file success: 1 file_date_updated: 2023-01-27T09:09:15Z has_accepted_license: '1' intvolume: ' 5' isi: 1 issue: '11' keyword: - Electrical and Electronic Engineering - Materials Chemistry - Electrochemistry - Energy Engineering and Power Technology - Chemical Engineering (miscellaneous) language: - iso: eng month: '10' oa: 1 oa_version: Published Version page: 14381-14390 publication: ACS Applied Energy Materials publication_identifier: issn: - 2574-0962 publication_status: published publisher: American Chemical Society quality_controlled: '1' scopus_import: '1' status: public title: 'Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications' tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 5 year: '2022' ... --- _id: '10813' abstract: - lang: eng text: Redox mediators could catalyse otherwise slow and energy-inefficient cycling of Li–S and Li–O2 batteries by shuttling electrons or holes between the electrode and the solid insulating storage materials. For mediators to work efficiently they need to oxidize the solid with fast kinetics but with the lowest possible overpotential. However, the dependence of kinetics and overpotential is unclear, which hinders informed improvement. Here, we find that when the redox potentials of mediators are tuned via, for example, Li+ concentration in the electrolyte, they exhibit distinct threshold potentials, where the kinetics accelerate several-fold within a range as small as 10 mV. This phenomenon is independent of types of mediator and electrolyte. The acceleration originates from the overpotentials required to activate fast Li+/e− extraction and the following chemical step at specific abundant surface facets. Efficient redox catalysis at insulating solids therefore requires careful consideration of the surface conditions of the storage materials and electrolyte-dependent redox potentials, which may be tuned by salt concentrations or solvents. acknowledgement: This work was financially supported by the National Natural Science Foundation of China (grant nos. 51773092, 21975124, 11874254, 51802187 and U2030206). It was further supported by Fujian science & technology innovation laboratory for energy devices of China (21C-LAB), Key Research Project of Zhejiang Laboratory (grant no. 2021PE0AC02) and the Cultivation Program for the Excellent Doctoral Dissertation of Nanjing Tech University. S.A.F. is indebted to IST Austria for support. article_processing_charge: No article_type: original author: - first_name: Deqing full_name: Cao, Deqing last_name: Cao - first_name: Xiaoxiao full_name: Shen, Xiaoxiao last_name: Shen - first_name: Aiping full_name: Wang, Aiping last_name: Wang - first_name: Fengjiao full_name: Yu, Fengjiao last_name: Yu - first_name: Yuping full_name: Wu, Yuping last_name: Wu - first_name: Siqi full_name: Shi, Siqi last_name: Shi - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Yuhui full_name: Chen, Yuhui last_name: Chen citation: ama: Cao D, Shen X, Wang A, et al. Threshold potentials for fast kinetics during mediated redox catalysis of insulators in Li–O2 and Li–S batteries. Nature Catalysis. 2022;5:193-201. doi:10.1038/s41929-022-00752-z apa: Cao, D., Shen, X., Wang, A., Yu, F., Wu, Y., Shi, S., … Chen, Y. (2022). Threshold potentials for fast kinetics during mediated redox catalysis of insulators in Li–O2 and Li–S batteries. Nature Catalysis. Springer Nature. https://doi.org/10.1038/s41929-022-00752-z chicago: Cao, Deqing, Xiaoxiao Shen, Aiping Wang, Fengjiao Yu, Yuping Wu, Siqi Shi, Stefan Alexander Freunberger, and Yuhui Chen. “Threshold Potentials for Fast Kinetics during Mediated Redox Catalysis of Insulators in Li–O2 and Li–S Batteries.” Nature Catalysis. Springer Nature, 2022. https://doi.org/10.1038/s41929-022-00752-z. ieee: D. Cao et al., “Threshold potentials for fast kinetics during mediated redox catalysis of insulators in Li–O2 and Li–S batteries,” Nature Catalysis, vol. 5. Springer Nature, pp. 193–201, 2022. ista: Cao D, Shen X, Wang A, Yu F, Wu Y, Shi S, Freunberger SA, Chen Y. 2022. Threshold potentials for fast kinetics during mediated redox catalysis of insulators in Li–O2 and Li–S batteries. Nature Catalysis. 5, 193–201. mla: Cao, Deqing, et al. “Threshold Potentials for Fast Kinetics during Mediated Redox Catalysis of Insulators in Li–O2 and Li–S Batteries.” Nature Catalysis, vol. 5, Springer Nature, 2022, pp. 193–201, doi:10.1038/s41929-022-00752-z. short: D. Cao, X. Shen, A. Wang, F. Yu, Y. Wu, S. Shi, S.A. Freunberger, Y. Chen, Nature Catalysis 5 (2022) 193–201. date_created: 2022-03-04T07:50:10Z date_published: 2022-03-03T00:00:00Z date_updated: 2023-10-17T13:06:28Z day: '03' department: - _id: StFr doi: 10.1038/s41929-022-00752-z external_id: isi: - '000763879400001' intvolume: ' 5' isi: 1 keyword: - Process Chemistry and Technology - Biochemistry - Bioengineering - Catalysis language: - iso: eng main_file_link: - open_access: '1' url: https://doi.org/10.21203/rs.3.rs-750965/v1 month: '03' oa: 1 oa_version: Preprint page: 193-201 publication: Nature Catalysis publication_identifier: issn: - 2520-1158 publication_status: published publisher: Springer Nature quality_controlled: '1' related_material: record: - id: '9978' relation: earlier_version status: public scopus_import: '1' status: public title: Threshold potentials for fast kinetics during mediated redox catalysis of insulators in Li–O2 and Li–S batteries type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 5 year: '2022' ... --- _id: '9980' abstract: - lang: eng text: Insufficient understanding of the mechanism that reversibly converts sulphur into lithium sulphide (Li2S) via soluble polysulphides (PS) hampers the realization of high performance lithium-sulphur cells. Typically Li2S formation is explained by direct electroreduction of a PS to Li2S; however, this is not consistent with the size of the insulating Li2S deposits. Here, we use in situ small and wide angle X-ray scattering (SAXS/WAXS) to track the growth and dissolution of crystalline and amorphous deposits from atomic to sub-micron scales during charge and discharge. Stochastic modelling based on the SAXS data allows quantification of the chemical phase evolution during discharge and charge. We show that Li2S deposits predominantly via disproportionation of transient, solid Li2S2 to form primary Li2S crystallites and solid Li2S4 particles. We further demonstrate that this process happens in reverse during charge. These findings show that the discharge capacity and rate capability in Li-S battery cathodes are therefore limited by mass transport through the increasingly tortuous network of Li2S / Li2S4 / carbon pores rather than electron transport through a passivating surface film. acknowledgement: "This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant NanoEvolution, grant agreement No 894042. The authors acknowledge TU Graz for support through the Lead Project LP-03. Likewise, the use of SOMAPP Lab, a core facility supported by the Austrian Federal Ministry of Education, Science and Research, the Graz University\r\n6 of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. S.D.T, A.V. and R.D. acknowledge the financial support by the Slovenian Research Agency (ARRS) research core funding P2-0393. Furthermore, A.V. acknowledge the funding from the Slovenian Research Agency, research project Z2-1863. S.A.F. is indebted to IST Austria for support. " article_processing_charge: No author: - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Sara Drvarič full_name: Talian, Sara Drvarič last_name: Talian - first_name: Alen full_name: Vizintin, Alen last_name: Vizintin - first_name: Heinz full_name: Amenitsch, Heinz last_name: Amenitsch - first_name: Robert full_name: Dominko, Robert last_name: Dominko - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Vanessa full_name: Wood, Vanessa last_name: Wood citation: ama: Prehal C, Talian SD, Vizintin A, et al. Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries. Research Square. doi:10.21203/rs.3.rs-818607/v1 apa: Prehal, C., Talian, S. D., Vizintin, A., Amenitsch, H., Dominko, R., Freunberger, S. A., & Wood, V. (n.d.). Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries. Research Square. https://doi.org/10.21203/rs.3.rs-818607/v1 chicago: Prehal, Christian, Sara Drvarič Talian, Alen Vizintin, Heinz Amenitsch, Robert Dominko, Stefan Alexander Freunberger, and Vanessa Wood. “Mechanism of Li2S Formation and Dissolution in Lithium-Sulphur Batteries.” Research Square, n.d. https://doi.org/10.21203/rs.3.rs-818607/v1. ieee: C. Prehal et al., “Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries,” Research Square. . ista: Prehal C, Talian SD, Vizintin A, Amenitsch H, Dominko R, Freunberger SA, Wood V. Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries. Research Square, 10.21203/rs.3.rs-818607/v1. mla: Prehal, Christian, et al. “Mechanism of Li2S Formation and Dissolution in Lithium-Sulphur Batteries.” Research Square, doi:10.21203/rs.3.rs-818607/v1. short: C. Prehal, S.D. Talian, A. Vizintin, H. Amenitsch, R. Dominko, S.A. Freunberger, V. Wood, Research Square (n.d.). date_created: 2021-09-02T08:45:00Z date_published: 2021-08-16T00:00:00Z date_updated: 2021-12-03T10:35:42Z day: '16' ddc: - '621' department: - _id: StFr doi: 10.21203/rs.3.rs-818607/v1 keyword: - Li2S - Lithium Sulphur Batteries - SAXS - WAXS language: - iso: eng main_file_link: - open_access: '1' url: https://www.researchsquare.com/article/rs-818607/v1 month: '08' oa: 1 oa_version: Preprint page: '21' publication: Research Square publication_status: submitted status: public title: Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: preprint user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9 year: '2021' ... --- _id: '9113' abstract: - lang: eng text: “Hydrogen economy” could enable a carbon-neutral sustainable energy chain. However, issues with safety, storage, and transport of molecular hydrogen impede its realization. Alcohols as liquid H2 carriers could be enablers, but state-of-the-art reforming is difficult, requiring high temperatures >200 °C and pressures >25 bar, and the resulting H2 is carbonized beyond tolerance levels for direct use in fuel cells. Here, we demonstrate ambient temperature and pressure alcohol reforming in a fuel cell (ARFC) with a simultaneous electrical power output. The alcohol is oxidized at the alkaline anode, where the resulting CO2 is sequestrated as carbonate. Carbon-free H2 is liberated at the acidic cathode. The neutralization energy between the alkaline anode and the acidic cathode drives the process, particularly the unusually high entropy gain (1.27-fold ΔH). The significantly positive temperature coefficient of the resulting electromotive force allows us to harvest a large fraction of the output energy from the surrounding, achieving a thermodynamic efficiency as high as 2.27. MoS2 as the cathode catalyst allows alcohol reforming even under open-air conditions, a challenge that state-of-the-art alcohol reforming failed to overcome. We further show reforming of a wide range of alcohols. The ARFC offers an unprecedented route toward hydrogen economy as CO2 is simultaneously captured and pure H2 produced at mild conditions. acknowledgement: M.O.T. acknowledges DST/TMD/HFC/2 K18/58, DST-SERB, MHRD fast track, and DST Nanomission forfinancialassistance. Z.M.B. acknowledges CSIR-SRF fellowship fromMHRD, India. S.A.F. acknowledges support from IST Austria. article_processing_charge: No article_type: original author: - first_name: Zahid Manzoor full_name: Manzoor Bhat, Zahid Manzoor last_name: Manzoor Bhat - first_name: Ravikumar full_name: Thimmappa, Ravikumar last_name: Thimmappa - first_name: 'Neethu Christudas ' full_name: 'Dargily, Neethu Christudas ' last_name: Dargily - first_name: 'Abdul ' full_name: 'Raafik, Abdul ' last_name: Raafik - first_name: 'Alagar Raja ' full_name: 'Kottaichamy, Alagar Raja ' last_name: Kottaichamy - first_name: 'Mruthyunjayachari Chattanahalli ' full_name: 'Devendrachari, Mruthyunjayachari Chattanahalli ' last_name: Devendrachari - first_name: Mahesh full_name: Itagi, Mahesh last_name: Itagi - first_name: Harish full_name: ' Makri Nimbegondi Kotresh, Harish' last_name: ' Makri Nimbegondi Kotresh' - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: 'Musthafa ' full_name: 'Ottakam Thotiyl, Musthafa ' last_name: Ottakam Thotiyl citation: ama: Manzoor Bhat ZM, Thimmappa R, Dargily NC, et al. Ambient condition alcohol reforming to hydrogen with electricity output. ACS Sustainable Chemistry and Engineering. 2021;9(8):3104-3111. doi:10.1021/acssuschemeng.0c07547 apa: Manzoor Bhat, Z. M., Thimmappa, R., Dargily, N. C., Raafik, A., Kottaichamy, A. R., Devendrachari, M. C., … Ottakam Thotiyl, M. (2021). Ambient condition alcohol reforming to hydrogen with electricity output. ACS Sustainable Chemistry and Engineering. American Chemical Society. https://doi.org/10.1021/acssuschemeng.0c07547 chicago: Manzoor Bhat, Zahid Manzoor, Ravikumar Thimmappa, Neethu Christudas Dargily, Abdul Raafik, Alagar Raja Kottaichamy, Mruthyunjayachari Chattanahalli Devendrachari, Mahesh Itagi, Harish Makri Nimbegondi Kotresh, Stefan Alexander Freunberger, and Musthafa Ottakam Thotiyl. “Ambient Condition Alcohol Reforming to Hydrogen with Electricity Output.” ACS Sustainable Chemistry and Engineering. American Chemical Society, 2021. https://doi.org/10.1021/acssuschemeng.0c07547. ieee: Z. M. Manzoor Bhat et al., “Ambient condition alcohol reforming to hydrogen with electricity output,” ACS Sustainable Chemistry and Engineering, vol. 9, no. 8. American Chemical Society, pp. 3104–3111, 2021. ista: Manzoor Bhat ZM, Thimmappa R, Dargily NC, Raafik A, Kottaichamy AR, Devendrachari MC, Itagi M, Makri Nimbegondi Kotresh H, Freunberger SA, Ottakam Thotiyl M. 2021. Ambient condition alcohol reforming to hydrogen with electricity output. ACS Sustainable Chemistry and Engineering. 9(8), 3104–3111. mla: Manzoor Bhat, Zahid Manzoor, et al. “Ambient Condition Alcohol Reforming to Hydrogen with Electricity Output.” ACS Sustainable Chemistry and Engineering, vol. 9, no. 8, American Chemical Society, 2021, pp. 3104–11, doi:10.1021/acssuschemeng.0c07547. short: Z.M. Manzoor Bhat, R. Thimmappa, N.C. Dargily, A. Raafik, A.R. Kottaichamy, M.C. Devendrachari, M. Itagi, H. Makri Nimbegondi Kotresh, S.A. Freunberger, M. Ottakam Thotiyl, ACS Sustainable Chemistry and Engineering 9 (2021) 3104–3111. date_created: 2021-02-12T09:20:18Z date_published: 2021-02-11T00:00:00Z date_updated: 2023-08-07T13:43:19Z day: '11' department: - _id: StFr doi: 10.1021/acssuschemeng.0c07547 external_id: isi: - '000625460400010' intvolume: ' 9' isi: 1 issue: '8' language: - iso: eng month: '02' oa_version: None page: 3104-3111 publication: ACS Sustainable Chemistry and Engineering publication_identifier: eissn: - 2168-0485 publication_status: published publisher: American Chemical Society quality_controlled: '1' scopus_import: '1' status: public title: Ambient condition alcohol reforming to hydrogen with electricity output type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 9 year: '2021' ... --- _id: '9301' abstract: - lang: eng text: Electrodepositing insulating lithium peroxide (Li2O2) is the key process during discharge of aprotic Li–O2 batteries and determines rate, capacity, and reversibility. Current understanding states that the partition between surface adsorbed and dissolved lithium superoxide governs whether Li2O2 grows as a conformal surface film or larger particles, leading to low or high capacities, respectively. However, better understanding governing factors for Li2O2 packing density and capacity requires structural sensitive in situ metrologies. Here, we establish in situ small- and wide-angle X-ray scattering (SAXS/WAXS) as a suitable method to record the Li2O2 phase evolution with atomic to submicrometer resolution during cycling a custom-built in situ Li–O2 cell. Combined with sophisticated data analysis, SAXS allows retrieving rich quantitative structural information from complex multiphase systems. Surprisingly, we find that features are absent that would point at a Li2O2 surface film formed via two consecutive electron transfers, even in poorly solvating electrolytes thought to be prototypical for surface growth. All scattering data can be modeled by stacks of thin Li2O2 platelets potentially forming large toroidal particles. Li2O2 solution growth is further justified by rotating ring-disk electrode measurements and electron microscopy. Higher discharge overpotentials lead to smaller Li2O2 particles, but there is no transition to an electronically passivating, conformal Li2O2 coating. Hence, mass transport of reactive species rather than electronic transport through a Li2O2 film limits the discharge capacity. Provided that species mobilities and carbon surface areas are high, this allows for high discharge capacities even in weakly solvating electrolytes. The currently accepted Li–O2 reaction mechanism ought to be reconsidered. acknowledged_ssus: - _id: EM-Fac acknowledgement: S.A.F. and C.P. are indebted to the European Research Council under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 636069), the Austrian Federal Ministry of Science, Research and Economy, and the Austrian Research Promotion Agency (Grant No. 845364). We acknowledge A. Zankel and H. Schroettner for support with SEM measurements. C.P. thanks N. Kostoglou, C. Koczwara, M. Hartmann, and M. Burian for discussions on gas sorption analysis, C++ programming, Monte Carlo modeling, and in situ SAXS experiments, respectively. We thank S. Stadlbauer for help with Karl Fischer titration, R. Riccò for gas sorption measurements, and acknowledge Graz University of Technology for support through the Lead Project LP-03. Likewise, the use of SOMAPP Lab, a core facility supported by the Austrian Federal Ministry of Education, Science and Research, the Graz University of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. S.A.F. is indebted to Institute of Science and Technology Austria (IST Austria) for support. This research was supported by the Scientific Service Units of IST Austria through resources provided by the Electron Microscopy Facility. article_number: e2021893118 article_processing_charge: No article_type: original author: - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Aleksej full_name: Samojlov, Aleksej last_name: Samojlov - first_name: Manfred full_name: Nachtnebel, Manfred last_name: Nachtnebel - first_name: Ludek full_name: Lovicar, Ludek id: 36DB3A20-F248-11E8-B48F-1D18A9856A87 last_name: Lovicar orcid: 0000-0001-6206-4200 - first_name: Manfred full_name: Kriechbaum, Manfred last_name: Kriechbaum - first_name: Heinz full_name: Amenitsch, Heinz last_name: Amenitsch - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Prehal C, Samojlov A, Nachtnebel M, et al. In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes. Proceedings of the National Academy of Sciences. 2021;118(14). doi:10.1073/pnas.2021893118 apa: Prehal, C., Samojlov, A., Nachtnebel, M., Lovicar, L., Kriechbaum, M., Amenitsch, H., & Freunberger, S. A. (2021). In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes. Proceedings of the National Academy of Sciences. National Academy of Sciences. https://doi.org/10.1073/pnas.2021893118 chicago: Prehal, Christian, Aleksej Samojlov, Manfred Nachtnebel, Ludek Lovicar, Manfred Kriechbaum, Heinz Amenitsch, and Stefan Alexander Freunberger. “In Situ Small-Angle X-Ray Scattering Reveals Solution Phase Discharge of Li–O2 Batteries with Weakly Solvating Electrolytes.” Proceedings of the National Academy of Sciences. National Academy of Sciences, 2021. https://doi.org/10.1073/pnas.2021893118. ieee: C. Prehal et al., “In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes,” Proceedings of the National Academy of Sciences, vol. 118, no. 14. National Academy of Sciences, 2021. ista: Prehal C, Samojlov A, Nachtnebel M, Lovicar L, Kriechbaum M, Amenitsch H, Freunberger SA. 2021. In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes. Proceedings of the National Academy of Sciences. 118(14), e2021893118. mla: Prehal, Christian, et al. “In Situ Small-Angle X-Ray Scattering Reveals Solution Phase Discharge of Li–O2 Batteries with Weakly Solvating Electrolytes.” Proceedings of the National Academy of Sciences, vol. 118, no. 14, e2021893118, National Academy of Sciences, 2021, doi:10.1073/pnas.2021893118. short: C. Prehal, A. Samojlov, M. Nachtnebel, L. Lovicar, M. Kriechbaum, H. Amenitsch, S.A. Freunberger, Proceedings of the National Academy of Sciences 118 (2021). date_created: 2021-03-31T07:00:01Z date_published: 2021-04-06T00:00:00Z date_updated: 2023-09-05T13:27:18Z day: '06' department: - _id: StFr - _id: EM-Fac doi: 10.1073/pnas.2021893118 external_id: isi: - '000637398300050' intvolume: ' 118' isi: 1 issue: '14' keyword: - small-angle X-ray scattering - oxygen reduction - disproportionation - Li-air battery language: - iso: eng main_file_link: - open_access: '1' url: https://doi.org/10.26434/chemrxiv.11447775 month: '04' oa: 1 oa_version: Preprint publication: Proceedings of the National Academy of Sciences publication_identifier: eissn: - 1091-6490 issn: - 0027-8424 publication_status: published publisher: National Academy of Sciences quality_controlled: '1' status: public title: In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes type: journal_article user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1 volume: 118 year: '2021' ... --- _id: '9447' abstract: - lang: eng text: 'Lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) based water-in-salt electrolytes (WiSEs) has recently emerged as a new promising class of electrolytes, primarily owing to their wide electrochemical stability windows (~3–4 V), that by far exceed the thermodynamic stability window of water (1.23 V). Upon increasing the salt concentration towards superconcentration the onset of the oxygen evolution reaction (OER) shifts more significantly than the hydrogen evolution reaction (HER) does. The OER shift has been explained by the accumulation of hydrophobic anions blocking water access to the electrode surface, hence by double layer theory. Here we demonstrate that the processes during oxidation are much more complex, involving OER, carbon and salt decomposition by OER intermediates, and salt precipitation upon local oversaturation. The positive shift in the onset potential of oxidation currents was elucidated by combining several advanced analysis techniques: rotating ring-disk electrode voltammetry, online electrochemical mass spectrometry, and X-ray photoelectron spectroscopy, using both dilute and superconcentrated electrolytes. The results demonstrate the importance of reactive OER intermediates and surface films for electrolyte and electrode stability and motivate further studies of the nature of the electrode.' article_number: '050550' article_processing_charge: No author: - first_name: Marion full_name: Maffre, Marion last_name: Maffre - first_name: Roza full_name: Bouchal, Roza last_name: Bouchal - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Niklas full_name: Lindahl, Niklas last_name: Lindahl - first_name: Patrik full_name: Johansson, Patrik last_name: Johansson - first_name: Frédéric full_name: Favier, Frédéric last_name: Favier - first_name: Olivier full_name: Fontaine, Olivier last_name: Fontaine - first_name: Daniel full_name: Bélanger, Daniel last_name: Bélanger citation: ama: Maffre M, Bouchal R, Freunberger SA, et al. Investigation of electrochemical and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes. Journal of The Electrochemical Society. 2021;168(5). doi:10.1149/1945-7111/ac0300 apa: Maffre, M., Bouchal, R., Freunberger, S. A., Lindahl, N., Johansson, P., Favier, F., … Bélanger, D. (2021). Investigation of electrochemical and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes. Journal of The Electrochemical Society. IOP Publishing. https://doi.org/10.1149/1945-7111/ac0300 chicago: Maffre, Marion, Roza Bouchal, Stefan Alexander Freunberger, Niklas Lindahl, Patrik Johansson, Frédéric Favier, Olivier Fontaine, and Daniel Bélanger. “Investigation of Electrochemical and Chemical Processes Occurring at Positive Potentials in ‘Water-in-Salt’ Electrolytes.” Journal of The Electrochemical Society. IOP Publishing, 2021. https://doi.org/10.1149/1945-7111/ac0300. ieee: M. Maffre et al., “Investigation of electrochemical and chemical processes occurring at positive potentials in ‘Water-in-Salt’ electrolytes,” Journal of The Electrochemical Society, vol. 168, no. 5. IOP Publishing, 2021. ista: Maffre M, Bouchal R, Freunberger SA, Lindahl N, Johansson P, Favier F, Fontaine O, Bélanger D. 2021. Investigation of electrochemical and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes. Journal of The Electrochemical Society. 168(5), 050550. mla: Maffre, Marion, et al. “Investigation of Electrochemical and Chemical Processes Occurring at Positive Potentials in ‘Water-in-Salt’ Electrolytes.” Journal of The Electrochemical Society, vol. 168, no. 5, 050550, IOP Publishing, 2021, doi:10.1149/1945-7111/ac0300. short: M. Maffre, R. Bouchal, S.A. Freunberger, N. Lindahl, P. Johansson, F. Favier, O. Fontaine, D. Bélanger, Journal of The Electrochemical Society 168 (2021). date_created: 2021-06-03T09:58:38Z date_published: 2021-05-01T00:00:00Z date_updated: 2023-09-05T13:25:30Z day: '01' department: - _id: StFr doi: 10.1149/1945-7111/ac0300 external_id: isi: - '000657724200001' intvolume: ' 168' isi: 1 issue: '5' keyword: - Renewable Energy - Sustainability and the Environment - Electrochemistry - Materials Chemistry - Electronic - Optical and Magnetic Materials - Surfaces - Coatings and Films - Condensed Matter Physics language: - iso: eng month: '05' oa_version: None publication: Journal of The Electrochemical Society publication_identifier: eissn: - 1945-7111 issn: - 0013-4651 publication_status: published publisher: IOP Publishing quality_controlled: '1' status: public title: Investigation of electrochemical and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes type: journal_article user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1 volume: 168 year: '2021' ... --- _id: '9978' abstract: - lang: eng text: Redox mediators could catalyse otherwise slow and energy-inefficient cycling of Li-S and Li-O 2 batteries by shuttling electrons/holes between the electrode and the solid insulating storage materials. For mediators to work efficiently they need to oxidize the solid with fast kinetics yet the lowest possible overpotential. Here, we found that when the redox potentials of mediators are tuned via, e.g., Li + concentration in the electrolyte, they exhibit distinct threshold potentials, where the kinetics accelerate several-fold within a range as small as 10 mV. This phenomenon is independent of types of mediators and electrolyte. The acceleration originates from the overpotentials required to activate fast Li + /e – extraction and the following chemical step at specific abundant surface facets. Efficient redox catalysis at insulating solids requires therefore carefully considering the surface conditions of the storage materials and electrolyte-dependent redox potentials, which may be tuned by salt concentrations or solvents. acknowledgement: 'This work was financially supported by the National Natural Science Foundation of China (51773092, 21975124, 11874254, 51802187, U2030206). S.A.F. is indebted to IST Austria for support. ' article_processing_charge: No author: - first_name: Deqing full_name: Cao, Deqing last_name: Cao - first_name: Xiaoxiao full_name: Shen, Xiaoxiao last_name: Shen - first_name: Aiping full_name: Wang, Aiping last_name: Wang - first_name: Fengjiao full_name: Yu, Fengjiao last_name: Yu - first_name: Yuping full_name: Wu, Yuping last_name: Wu - first_name: Siqi full_name: Shi, Siqi last_name: Shi - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: Yuhui full_name: Chen, Yuhui last_name: Chen citation: ama: Cao D, Shen X, Wang A, et al. Sharp kinetic acceleration potentials during mediated redox catalysis of insulators. Research Square. doi:10.21203/rs.3.rs-750965/v1 apa: Cao, D., Shen, X., Wang, A., Yu, F., Wu, Y., Shi, S., … Chen, Y. (n.d.). Sharp kinetic acceleration potentials during mediated redox catalysis of insulators. Research Square. Research Square. https://doi.org/10.21203/rs.3.rs-750965/v1 chicago: Cao, Deqing, Xiaoxiao Shen, Aiping Wang, Fengjiao Yu, Yuping Wu, Siqi Shi, Stefan Alexander Freunberger, and Yuhui Chen. “Sharp Kinetic Acceleration Potentials during Mediated Redox Catalysis of Insulators.” Research Square. Research Square, n.d. https://doi.org/10.21203/rs.3.rs-750965/v1. ieee: D. Cao et al., “Sharp kinetic acceleration potentials during mediated redox catalysis of insulators,” Research Square. Research Square. ista: Cao D, Shen X, Wang A, Yu F, Wu Y, Shi S, Freunberger SA, Chen Y. Sharp kinetic acceleration potentials during mediated redox catalysis of insulators. Research Square, 10.21203/rs.3.rs-750965/v1. mla: Cao, Deqing, et al. “Sharp Kinetic Acceleration Potentials during Mediated Redox Catalysis of Insulators.” Research Square, Research Square, doi:10.21203/rs.3.rs-750965/v1. short: D. Cao, X. Shen, A. Wang, F. Yu, Y. Wu, S. Shi, S.A. Freunberger, Y. Chen, Research Square (n.d.). date_created: 2021-08-31T12:54:16Z date_published: 2021-08-18T00:00:00Z date_updated: 2023-10-17T13:06:29Z day: '18' ddc: - '541' department: - _id: StFr doi: 10.21203/rs.3.rs-750965/v1 file: - access_level: open_access checksum: 1878e91c29d5769ed5a827b0b7addf00 content_type: application/pdf creator: cchlebak date_created: 2021-08-31T14:02:19Z date_updated: 2021-08-31T14:02:19Z file_id: '9979' file_name: 2021_ResearchSquare_Cao.pdf file_size: 1019662 relation: main_file success: 1 file_date_updated: 2021-08-31T14:02:19Z has_accepted_license: '1' keyword: - Catalysis - Energy engineering - Materials theory and modeling language: - iso: eng month: '08' oa: 1 oa_version: Preprint page: '21' publication: Research Square publication_identifier: eissn: - 2693-5015 publication_status: submitted publisher: Research Square related_material: record: - id: '10813' relation: later_version status: public status: public title: Sharp kinetic acceleration potentials during mediated redox catalysis of insulators tmp: image: /images/cc_by.png legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0) short: CC BY (4.0) type: preprint user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 year: '2021' ... --- _id: '9250' abstract: - lang: eng text: Aprotic alkali metal–O2 batteries face two major obstacles to their chemistry occurring efficiently, the insulating nature of the formed alkali superoxides/peroxides and parasitic reactions that are caused by the highly reactive singlet oxygen (1O2). Redox mediators are recognized to be key for improving rechargeability. However, it is unclear how they affect 1O2 formation, which hinders strategies for their improvement. Here we clarify the mechanism of mediated peroxide and superoxide oxidation and thus explain how redox mediators either enhance or suppress 1O2 formation. We show that charging commences with peroxide oxidation to a superoxide intermediate and that redox potentials above ~3.5 V versus Li/Li+ drive 1O2 evolution from superoxide oxidation, while disproportionation always generates some 1O2. We find that 1O2 suppression requires oxidation to be faster than the generation of 1O2 from disproportionation. Oxidation rates decrease with growing driving force following Marcus inverted-region behaviour, establishing a region of maximum rate. acknowledged_ssus: - _id: M-Shop acknowledgement: S.A.F. is indebted to the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 636069) as well as IST Austria. O.F thanks the French National Research Agency (STORE-EX Labex Project ANR-10-LABX-76-01). We thank EL-Cell GmbH (Hamburg, Germany) for the pressure test cell. We thank R. Saf for help with the mass spectrometry, J. Schlegl for manufacturing instrumentation, M. Winkler of Acib GmbH, G. Strohmeier and R. Fürst for HPLC measurements and S. Mondal and S. Stadlbauer for kinetic measurements. article_processing_charge: No article_type: original author: - first_name: Yann K. full_name: Petit, Yann K. last_name: Petit - first_name: Eléonore full_name: Mourad, Eléonore last_name: Mourad - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Christian full_name: Leypold, Christian last_name: Leypold - first_name: Andreas full_name: Windischbacher, Andreas last_name: Windischbacher - first_name: Daniel full_name: Mijailovic, Daniel last_name: Mijailovic - first_name: Christian full_name: Slugovc, Christian last_name: Slugovc - first_name: Sergey M. full_name: Borisov, Sergey M. last_name: Borisov - first_name: Egbert full_name: Zojer, Egbert last_name: Zojer - first_name: Sergio full_name: Brutti, Sergio last_name: Brutti - first_name: Olivier full_name: Fontaine, Olivier last_name: Fontaine - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Petit YK, Mourad E, Prehal C, et al. Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation. Nature Chemistry. 2021;13(5):465-471. doi:10.1038/s41557-021-00643-z apa: Petit, Y. K., Mourad, E., Prehal, C., Leypold, C., Windischbacher, A., Mijailovic, D., … Freunberger, S. A. (2021). Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation. Nature Chemistry. Springer Nature. https://doi.org/10.1038/s41557-021-00643-z chicago: Petit, Yann K., Eléonore Mourad, Christian Prehal, Christian Leypold, Andreas Windischbacher, Daniel Mijailovic, Christian Slugovc, et al. “Mechanism of Mediated Alkali Peroxide Oxidation and Triplet versus Singlet Oxygen Formation.” Nature Chemistry. Springer Nature, 2021. https://doi.org/10.1038/s41557-021-00643-z. ieee: Y. K. Petit et al., “Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation,” Nature Chemistry, vol. 13, no. 5. Springer Nature, pp. 465–471, 2021. ista: Petit YK, Mourad E, Prehal C, Leypold C, Windischbacher A, Mijailovic D, Slugovc C, Borisov SM, Zojer E, Brutti S, Fontaine O, Freunberger SA. 2021. Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation. Nature Chemistry. 13(5), 465–471. mla: Petit, Yann K., et al. “Mechanism of Mediated Alkali Peroxide Oxidation and Triplet versus Singlet Oxygen Formation.” Nature Chemistry, vol. 13, no. 5, Springer Nature, 2021, pp. 465–71, doi:10.1038/s41557-021-00643-z. short: Y.K. Petit, E. Mourad, C. Prehal, C. Leypold, A. Windischbacher, D. Mijailovic, C. Slugovc, S.M. Borisov, E. Zojer, S. Brutti, O. Fontaine, S.A. Freunberger, Nature Chemistry 13 (2021) 465–471. date_created: 2021-03-16T11:12:20Z date_published: 2021-03-15T00:00:00Z date_updated: 2023-09-05T15:34:44Z day: '15' ddc: - '540' department: - _id: StFr doi: 10.1038/s41557-021-00643-z external_id: isi: - '000629296400001' pmid: - '33723377' file: - access_level: open_access checksum: 3ee3f8dd79ed1b7bb0929fce184c8012 content_type: application/pdf creator: dernst date_created: 2021-03-22T11:46:00Z date_updated: 2021-09-16T22:30:03Z embargo: 2021-09-15 file_id: '9276' file_name: 2021_NatureChem_Petit_acceptedVersion.pdf file_size: 1811448 relation: main_file file_date_updated: 2021-09-16T22:30:03Z has_accepted_license: '1' intvolume: ' 13' isi: 1 issue: '5' keyword: - General Chemistry - General Chemical Engineering language: - iso: eng month: '03' oa: 1 oa_version: Submitted Version page: 465-471 pmid: 1 publication: Nature Chemistry publication_identifier: eissn: - 1755-4349 issn: - 1755-4330 publication_status: published publisher: Springer Nature quality_controlled: '1' scopus_import: '1' status: public title: Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation type: journal_article user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1 volume: 13 year: '2021' ... --- _id: '8081' abstract: - lang: eng text: "Here, we employ micro- and nanosized cellulose particles, namely paper fines and cellulose\r\nnanocrystals, to induce hierarchical organization over a wide length scale. After processing\r\nthem into carbonaceous materials, we demonstrate that these hierarchically organized materials\r\noutperform the best materials for supercapacitors operating with organic electrolytes reported\r\nin literature in terms of specific energy/power (Ragone plot) while showing hardly any capacity\r\nfade over 4,000 cycles. The highly porous materials feature a specific surface area as high as\r\n2500 m2ˑg-1 and exhibit pore sizes in the range of 0.5 to 200 nm as proven by scanning electron\r\nmicroscopy and N2 physisorption. The carbonaceous materials have been further investigated\r\nby X-ray photoelectron spectroscopy and RAMAN spectroscopy. Since paper fines are an\r\nunderutilized side stream in any paper production process, they are a cheap and highly available\r\nfeedstock to prepare carbonaceous materials with outstanding performance in electrochemical\r\napplications. " acknowledgement: 'The authors M.A.H., S.S., R.E., and W.B. acknowledge the industrial partners Sappi Gratkorn, Zellstoff Pöls and Mondi Frantschach, the Austrian Research Promotion Agency (FFG), COMET, BMVIT, BMWFJ, the Province of Styria and Carinthia for their financial support of the K-project Flippr²-Process Integration. E.M. and S.A.F. are indebted to the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No 636069). W. T. and S. E. thank FWO (G.0C60.13N) and the European Union’s European Fund for Regional Development and Flanders Innovation & Entrepreneurship (Accelerate3 project, Interreg Vlaanderen-Nederland program) for financial support. W. T. also thanks the Provincie West-Vlaanderen (Belgium) for his Provincial Chair in Advanced Materials. S. B. thanks the European Regional Development Fund (EFRE) and the province of Upper Austria for financial support through the program IWB 2014-2020 (project BioCarb-K). AMR gratefully acknowledges funding support through the SC EPSCoR/IDeAProgram under Award #18-SR03, and the NASA EPSCoR Program under Award #NNH17ZHA002C. Icons in Scheme 1 were provided by Good Ware, monkik, photo3idea_studio, and OCHA from www.flaticon.com.' article_processing_charge: No author: - first_name: 'Mathias A. ' full_name: 'Hobisch, Mathias A. ' last_name: Hobisch - first_name: 'Eléonore ' full_name: 'Mourad, Eléonore ' last_name: Mourad - first_name: 'Wolfgang J. ' full_name: 'Fischer, Wolfgang J. ' last_name: Fischer - first_name: 'Christian ' full_name: 'Prehal, Christian ' last_name: Prehal - first_name: 'Samuel ' full_name: 'Eyley, Samuel ' last_name: Eyley - first_name: 'Anthony ' full_name: 'Childress, Anthony ' last_name: Childress - first_name: 'Armin ' full_name: 'Zankel, Armin ' last_name: Zankel - first_name: 'Andreas ' full_name: 'Mautner, Andreas ' last_name: Mautner - first_name: 'Stefan ' full_name: 'Breitenbach, Stefan ' last_name: Breitenbach - first_name: 'Apparao M. ' full_name: 'Rao, Apparao M. ' last_name: Rao - first_name: 'Wim ' full_name: 'Thielemans, Wim ' last_name: Thielemans - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 - first_name: 'Rene ' full_name: 'Eckhart, Rene ' last_name: Eckhart - first_name: 'Wolfgang ' full_name: 'Bauer, Wolfgang ' last_name: Bauer - first_name: 'Stefan ' full_name: 'Spirk, Stefan ' last_name: Spirk citation: ama: Hobisch MA, Mourad E, Fischer WJ, et al. High specific capacitance supercapacitors from hierarchically organized all-cellulose composites. apa: Hobisch, M. A., Mourad, E., Fischer, W. J., Prehal, C., Eyley, S., Childress, A., … Spirk, S. (n.d.). High specific capacitance supercapacitors from hierarchically organized all-cellulose composites. chicago: Hobisch, Mathias A. , Eléonore Mourad, Wolfgang J. Fischer, Christian Prehal, Samuel Eyley, Anthony Childress, Armin Zankel, et al. “High Specific Capacitance Supercapacitors from Hierarchically Organized All-Cellulose Composites,” n.d. ieee: M. A. Hobisch et al., “High specific capacitance supercapacitors from hierarchically organized all-cellulose composites.” . ista: Hobisch MA, Mourad E, Fischer WJ, Prehal C, Eyley S, Childress A, Zankel A, Mautner A, Breitenbach S, Rao AM, Thielemans W, Freunberger SA, Eckhart R, Bauer W, Spirk S. High specific capacitance supercapacitors from hierarchically organized all-cellulose composites. mla: Hobisch, Mathias A., et al. High Specific Capacitance Supercapacitors from Hierarchically Organized All-Cellulose Composites. short: M.A. Hobisch, E. Mourad, W.J. Fischer, C. Prehal, S. Eyley, A. Childress, A. Zankel, A. Mautner, S. Breitenbach, A.M. Rao, W. Thielemans, S.A. Freunberger, R. Eckhart, W. Bauer, S. Spirk, (n.d.). date_created: 2020-07-02T20:24:42Z date_published: 2020-07-13T00:00:00Z date_updated: 2022-06-17T08:39:49Z day: '13' ddc: - '540' department: - _id: StFr file: - access_level: open_access checksum: 6970d621984c03ebc2eee71adfe706dd content_type: application/pdf creator: sfreunbe date_created: 2020-07-02T20:21:59Z date_updated: 2020-07-14T12:48:09Z file_id: '8082' file_name: AM.pdf file_size: 1129852 relation: main_file - access_level: open_access checksum: cd74c7bd47d6e7163d54d67f074dcc36 content_type: application/pdf creator: cziletti date_created: 2020-07-08T12:14:04Z date_updated: 2020-07-14T12:48:09Z file_id: '8102' file_name: Supporting_Information.pdf file_size: 945565 relation: supplementary_material file_date_updated: 2020-07-14T12:48:09Z has_accepted_license: '1' language: - iso: eng month: '07' oa: 1 oa_version: Submitted Version publication_status: submitted status: public title: High specific capacitance supercapacitors from hierarchically organized all-cellulose composites type: preprint user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87 year: '2020' ... --- _id: '7672' abstract: - lang: eng text: Large overpotentials upon discharge and charge of Li-O2 cells have motivated extensive research into heterogeneous solid electrocatalysts or non-carbon electrodes with the aim to improve rate capability, round-trip efficiency and cycle life. These features are equally governed by parasitic reactions, which are now recognized to be caused by the highly reactive singlet oxygen (1O2). However, the link between the presence of electrocatalysts and 1O2 formation in metal-O2 cells is unknown. Here, we show that, compared to pristine carbon black electrodes, a representative selection of electrocatalysts or non-carbon electrodes (noble metal, transition metal compounds) may both slightly reduce or severely increase the 1O2 formation. The individual reaction steps, where the surfaces impact the 1O2 yield are deciphered, showing that 1O2 yield from superoxide disproportionation as well as the decomposition of trace H2O2 are sensitive to catalysts. Transition metal compounds in general are prone to increase 1O2. acknowledgement: S.A.F. thanks the International Society of Electrochemistry for awarding the Tajima Prize 2019 “in recognition of outstanding re- searches on Li-Air batteries by the use of a range of in-situ elec- trochemical methods to achieve comprehensive understanding of the reactions taking place at the oxygen electrode”. This article is dedicated to the special issue of Electrochmica Acta associated with the awarding conference. S.A.F. is indebted to and the Austrian Federal Ministry of Science, Research and Economy and the Austrian Research Promotion Agency (grant No. 845364 ) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 636069). The authors thank J. Schlegl for manufacturing instrumentation, M. Winkler of Acib GmbH and G. Strohmeier for help with HPLC measurements, S. Eder for cyclic voltammetry measurements, and C. Slugovc for discussions and continuous support. We thank S. Borisov for access and advice with fluorescence measurements. We thank EL-Cell GmbH, Hamburg, Germany for providing the PAT-Cell-Press electrochemical cell. article_number: '137175' article_processing_charge: Yes (via OA deal) article_type: original author: - first_name: Aleksej full_name: Samojlov, Aleksej last_name: Samojlov - first_name: David full_name: Schuster, David last_name: Schuster - first_name: Jürgen full_name: Kahr, Jürgen last_name: Kahr - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Samojlov A, Schuster D, Kahr J, Freunberger SA. Surface and catalyst driven singlet oxygen formation in Li-O2 cells. Electrochimica Acta. 2020;362(12). doi:10.1016/j.electacta.2020.137175 apa: Samojlov, A., Schuster, D., Kahr, J., & Freunberger, S. A. (2020). Surface and catalyst driven singlet oxygen formation in Li-O2 cells. Electrochimica Acta. Elsevier. https://doi.org/10.1016/j.electacta.2020.137175 chicago: Samojlov, Aleksej, David Schuster, Jürgen Kahr, and Stefan Alexander Freunberger. “Surface and Catalyst Driven Singlet Oxygen Formation in Li-O2 Cells.” Electrochimica Acta. Elsevier, 2020. https://doi.org/10.1016/j.electacta.2020.137175. ieee: A. Samojlov, D. Schuster, J. Kahr, and S. A. Freunberger, “Surface and catalyst driven singlet oxygen formation in Li-O2 cells,” Electrochimica Acta, vol. 362, no. 12. Elsevier, 2020. ista: Samojlov A, Schuster D, Kahr J, Freunberger SA. 2020. Surface and catalyst driven singlet oxygen formation in Li-O2 cells. Electrochimica Acta. 362(12), 137175. mla: Samojlov, Aleksej, et al. “Surface and Catalyst Driven Singlet Oxygen Formation in Li-O2 Cells.” Electrochimica Acta, vol. 362, no. 12, 137175, Elsevier, 2020, doi:10.1016/j.electacta.2020.137175. short: A. Samojlov, D. Schuster, J. Kahr, S.A. Freunberger, Electrochimica Acta 362 (2020). date_created: 2020-04-20T19:29:31Z date_published: 2020-12-01T00:00:00Z date_updated: 2023-08-21T06:14:21Z day: '01' ddc: - '540' department: - _id: StFr doi: 10.1016/j.electacta.2020.137175 external_id: isi: - '000582869700060' file: - access_level: open_access checksum: 1ab1aa2024d431e2a089ea336bc08298 content_type: application/pdf creator: dernst date_created: 2020-10-01T13:20:45Z date_updated: 2020-10-01T13:20:45Z file_id: '8593' file_name: 2020_ElectrochimicaActa_Samojlov.pdf file_size: 1404030 relation: main_file success: 1 file_date_updated: 2020-10-01T13:20:45Z has_accepted_license: '1' intvolume: ' 362' isi: 1 issue: '12' language: - iso: eng license: https://creativecommons.org/licenses/by-nc-nd/4.0/ month: '12' oa: 1 oa_version: Published Version publication: Electrochimica Acta publication_status: published publisher: Elsevier quality_controlled: '1' scopus_import: '1' status: public title: Surface and catalyst driven singlet oxygen formation in Li-O2 cells tmp: image: /images/cc_by_nc_nd.png legal_code_url: https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode name: Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) short: CC BY-NC-ND (4.0) type: journal_article user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8 volume: 362 year: '2020' ... --- _id: '8067' abstract: - lang: eng text: "With the lithium-ion technology approaching its intrinsic limit with graphite-based anodes, lithium metal is recently receiving renewed interest from the battery community as potential high capacity anode for next-generation rechargeable batteries. In this focus paper, we review the main advances in this field since the first attempts in the\r\nmid-1970s. Strategies for enabling reversible cycling and avoiding dendrite growth are thoroughly discussed, including specific applications in all-solid-state (polymeric and inorganic), Lithium-sulphur and Li-O2 (air) batteries. A particular attention is paid to review recent developments in regard of prototype manufacturing and current state-ofthe-art of these battery technologies with respect to the 2030 targets of the EU Integrated Strategic Energy Technology Plan (SET-Plan) Action 7." alternative_title: - IST Austria Technical Report article_processing_charge: No author: - first_name: Alberto full_name: Varzi, Alberto last_name: Varzi - first_name: Katharina full_name: Thanner, Katharina last_name: Thanner - first_name: Roberto full_name: Scipioni, Roberto last_name: Scipioni - first_name: Daniele full_name: Di Lecce, Daniele last_name: Di Lecce - first_name: Jusef full_name: Hassoun, Jusef last_name: Hassoun - first_name: Susanne full_name: Dörfler, Susanne last_name: Dörfler - first_name: Holger full_name: Altheus, Holger last_name: Altheus - first_name: Stefan full_name: Kaskel, Stefan last_name: Kaskel - first_name: Christian full_name: Prehal, Christian last_name: Prehal - first_name: Stefan Alexander full_name: Freunberger, Stefan Alexander id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425 last_name: Freunberger orcid: 0000-0003-2902-5319 citation: ama: Varzi A, Thanner K, Scipioni R, et al. Current Status and Future Perspectives of Lithium Metal Batteries. IST Austria doi:10.15479/AT:ISTA:8067 apa: Varzi, A., Thanner, K., Scipioni, R., Di Lecce, D., Hassoun, J., Dörfler, S., … Freunberger, S. A. (n.d.). Current status and future perspectives of Lithium metal batteries. IST Austria. https://doi.org/10.15479/AT:ISTA:8067 chicago: Varzi, Alberto, Katharina Thanner, Roberto Scipioni, Daniele Di Lecce, Jusef Hassoun, Susanne Dörfler, Holger Altheus, Stefan Kaskel, Christian Prehal, and Stefan Alexander Freunberger. Current Status and Future Perspectives of Lithium Metal Batteries. IST Austria, n.d. https://doi.org/10.15479/AT:ISTA:8067. ieee: A. Varzi et al., Current status and future perspectives of Lithium metal batteries. IST Austria. ista: Varzi A, Thanner K, Scipioni R, Di Lecce D, Hassoun J, Dörfler S, Altheus H, Kaskel S, Prehal C, Freunberger SA. Current status and future perspectives of Lithium metal batteries, IST Austria, 63p. mla: Varzi, Alberto, et al. Current Status and Future Perspectives of Lithium Metal Batteries. IST Austria, doi:10.15479/AT:ISTA:8067. short: A. Varzi, K. Thanner, R. Scipioni, D. Di Lecce, J. Hassoun, S. Dörfler, H. Altheus, S. Kaskel, C. Prehal, S.A. Freunberger, Current Status and Future Perspectives of Lithium Metal Batteries, IST Austria, n.d. date_created: 2020-06-30T07:37:39Z date_published: 2020-07-01T00:00:00Z date_updated: 2023-08-22T09:20:36Z day: '01' ddc: - '540' department: - _id: StFr doi: 10.15479/AT:ISTA:8067 file: - access_level: open_access checksum: d183ca1465a1cbb4f8db27875cd156f7 content_type: application/pdf creator: dernst date_created: 2020-07-02T07:36:04Z date_updated: 2020-07-14T12:48:08Z file_id: '8076' file_name: 20200612_JPS_review_Li_metal_submitted.pdf file_size: 2612498 relation: main_file file_date_updated: 2020-07-14T12:48:08Z has_accepted_license: '1' keyword: - Battery - Lithium metal - Lithium-sulphur - Lithium-air - All-solid-state language: - iso: eng month: '07' oa: 1 oa_version: Published Version page: '63' publication_identifier: issn: - 2664-1690 publication_status: submitted publisher: IST Austria related_material: record: - id: '8361' relation: later_version status: public status: public title: Current status and future perspectives of Lithium metal batteries type: technical_report user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9 year: '2020' ...