[{"publication_identifier":{"eissn":["1520-5002"],"issn":["0897-4756"]},"month":"01","tmp":{"name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","short":"CC BY (4.0)","image":"/images/cc_by.png"},"external_id":{"isi":["000914749700001"]},"oa":1,"project":[{"name":"Bottom-up Engineering for Thermoelectric Applications","grant_number":"M02889","_id":"9B8804FC-BA93-11EA-9121-9846C619BF3A"}],"quality_controlled":"1","isi":1,"doi":"10.1021/acs.chemmater.2c03542","language":[{"iso":"eng"}],"file_date_updated":"2023-08-14T12:57:25Z","license":"https://creativecommons.org/licenses/by/4.0/","acknowledgement":"The National Key Research and Development Program of China (2018YFA0702100), the Basic Science Center Project of the National Natural Science Foundation of China (51788104), the National Natural Science Foundation of China (51571007 and 51772012), the Beijing Natural Science Foundation (JQ18004), the 111 Project (B17002), the National Science Fund for Distinguished Young Scholars (51925101), and the FWF “Lise Meitner Fellowship” (grant agreement M2889-N). Open Access is funded by the Austrian Science Fund (FWF).","year":"2023","publisher":"American Chemical Society","department":[{"_id":"MaIb"}],"publication_status":"published","author":[{"first_name":"Siqi","last_name":"Wang","full_name":"Wang, Siqi"},{"orcid":"0000-0002-9515-4277","id":"9E331C2E-9F27-11E9-AE48-5033E6697425","last_name":"Chang","first_name":"Cheng","full_name":"Chang, Cheng"},{"full_name":"Bai, Shulin","last_name":"Bai","first_name":"Shulin"},{"last_name":"Qin","first_name":"Bingchao","full_name":"Qin, Bingchao"},{"first_name":"Yingcai","last_name":"Zhu","full_name":"Zhu, Yingcai"},{"first_name":"Shaoping","last_name":"Zhan","full_name":"Zhan, Shaoping"},{"full_name":"Zheng, Junqing","last_name":"Zheng","first_name":"Junqing"},{"full_name":"Tang, Shuwei","first_name":"Shuwei","last_name":"Tang"},{"full_name":"Zhao, Li Dong","first_name":"Li Dong","last_name":"Zhao"}],"volume":35,"date_updated":"2023-08-14T12:57:44Z","date_created":"2023-01-22T23:00:55Z","scopus_import":"1","article_processing_charge":"No","has_accepted_license":"1","day":"24","citation":{"ama":"Wang S, Chang C, Bai S, et al. Fine tuning of defects enables high carrier mobility and enhanced thermoelectric performance of n-type PbTe. Chemistry of Materials. 2023;35(2):755-763. doi:10.1021/acs.chemmater.2c03542","apa":"Wang, S., Chang, C., Bai, S., Qin, B., Zhu, Y., Zhan, S., … Zhao, L. D. (2023). Fine tuning of defects enables high carrier mobility and enhanced thermoelectric performance of n-type PbTe. Chemistry of Materials. American Chemical Society. https://doi.org/10.1021/acs.chemmater.2c03542","ieee":"S. Wang et al., “Fine tuning of defects enables high carrier mobility and enhanced thermoelectric performance of n-type PbTe,” Chemistry of Materials, vol. 35, no. 2. American Chemical Society, pp. 755–763, 2023.","ista":"Wang S, Chang C, Bai S, Qin B, Zhu Y, Zhan S, Zheng J, Tang S, Zhao LD. 2023. Fine tuning of defects enables high carrier mobility and enhanced thermoelectric performance of n-type PbTe. Chemistry of Materials. 35(2), 755–763.","short":"S. Wang, C. Chang, S. Bai, B. Qin, Y. Zhu, S. Zhan, J. Zheng, S. Tang, L.D. Zhao, Chemistry of Materials 35 (2023) 755–763.","mla":"Wang, Siqi, et al. “Fine Tuning of Defects Enables High Carrier Mobility and Enhanced Thermoelectric Performance of N-Type PbTe.” Chemistry of Materials, vol. 35, no. 2, American Chemical Society, 2023, pp. 755–63, doi:10.1021/acs.chemmater.2c03542.","chicago":"Wang, Siqi, Cheng Chang, Shulin Bai, Bingchao Qin, Yingcai Zhu, Shaoping Zhan, Junqing Zheng, Shuwei Tang, and Li Dong Zhao. “Fine Tuning of Defects Enables High Carrier Mobility and Enhanced Thermoelectric Performance of N-Type PbTe.” Chemistry of Materials. American Chemical Society, 2023. https://doi.org/10.1021/acs.chemmater.2c03542."},"publication":"Chemistry of Materials","page":"755-763","article_type":"original","date_published":"2023-01-24T00:00:00Z","type":"journal_article","issue":"2","abstract":[{"lang":"eng","text":"High carrier mobility is critical to improving thermoelectric performance over a broad temperature range. However, traditional doping inevitably deteriorates carrier mobility. Herein, we develop a strategy for fine tuning of defects to improve carrier mobility. To begin, n-type PbTe is created by compensating for the intrinsic Pb vacancy in bare PbTe. Excess Pb2+ reduces vacancy scattering, resulting in a high carrier mobility of ∼3400 cm2 V–1 s–1. Then, excess Ag is introduced to compensate for the remaining intrinsic Pb vacancies. We find that excess Ag exhibits a dynamic doping process with increasing temperatures, increasing both the carrier concentration and carrier mobility throughout a wide temperature range; specifically, an ultrahigh carrier mobility ∼7300 cm2 V–1 s–1 is obtained for Pb1.01Te + 0.002Ag at 300 K. Moreover, the dynamic doping-induced high carrier concentration suppresses the bipolar thermal conductivity at high temperatures. The final step is using iodine to optimize the carrier concentration to ∼1019 cm–3. Ultimately, a maximum ZT value of ∼1.5 and a large average ZTave value of ∼1.0 at 300–773 K are obtained for Pb1.01Te0.998I0.002 + 0.002Ag. These findings demonstrate that fine tuning of defects with <0.5% impurities can remarkably enhance carrier mobility and improve thermoelectric performance."}],"user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","_id":"12331","intvolume":" 35","status":"public","ddc":["540"],"title":"Fine tuning of defects enables high carrier mobility and enhanced thermoelectric performance of n-type PbTe","file":[{"relation":"main_file","file_id":"14055","checksum":"b21dca2aa7a80c068bc256bdd1fea9df","success":1,"date_updated":"2023-08-14T12:57:25Z","date_created":"2023-08-14T12:57:25Z","access_level":"open_access","file_name":"2023_ChemistryMaterials_Wang.pdf","content_type":"application/pdf","file_size":2961043,"creator":"dernst"}],"oa_version":"Published Version"},{"publication_status":"published","publisher":"American Chemical Society","department":[{"_id":"MaIb"}],"acknowledgement":"The authors acknowledge support from the projects ENE2016-77798-C4-3-R and NANOGEN (PID2020-116093RB-C43) funded by MCIN/AEI/10.13039/501100011033/and by “ERDF A way of making Europe”, and by the “European Union”. K.X. and B.N. thank the China Scholarship Council (CSC) for scholarship support. The authors acknowledge funding from Generalitat de Catalunya 2017 SGR 327 and 2017 SGR 1246. ICN2 is supported by the Severo Ochoa program from the Spanish MCIN/AEI (Grant No.: CEX2021-001214-S). IREC and ICN2 are funded by the CERCA Programme/Generalitat de Catalunya. J.L. acknowledges support from the Natural Science Foundation of Sichuan province (2022NSFSC1229). Part of the present work was performed in the frameworks of Universitat de Barcelona Nanoscience Ph.D. program and Universitat Autònoma de Barcelona Materials Science Ph.D. program. Y.L. acknowledges funding from the National Natural Science Foundation of China (Grant No. 22209034) and the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province (Grants No. 2022LCX002). K.H.L. acknowledges the financial support of the National Natural Science Foundation of China (Grant No. 22208293).","year":"2023","pmid":1,"date_created":"2023-05-07T22:01:04Z","date_updated":"2023-10-04T11:29:22Z","volume":17,"author":[{"last_name":"Xing","first_name":"Congcong","full_name":"Xing, Congcong"},{"first_name":"Yu","last_name":"Zhang","full_name":"Zhang, Yu"},{"full_name":"Xiao, Ke","last_name":"Xiao","first_name":"Ke"},{"full_name":"Han, Xu","first_name":"Xu","last_name":"Han"},{"full_name":"Liu, Yu","orcid":"0000-0001-7313-6740","id":"2A70014E-F248-11E8-B48F-1D18A9856A87","last_name":"Liu","first_name":"Yu"},{"first_name":"Bingfei","last_name":"Nan","full_name":"Nan, Bingfei"},{"first_name":"Maria Garcia","last_name":"Ramon","id":"1ffff7cd-ed76-11ed-8d5f-be5e7c364eb9","full_name":"Ramon, Maria Garcia"},{"last_name":"Lim","first_name":"Khak Ho","full_name":"Lim, Khak Ho"},{"full_name":"Li, Junshan","first_name":"Junshan","last_name":"Li"},{"first_name":"Jordi","last_name":"Arbiol","full_name":"Arbiol, Jordi"},{"first_name":"Bed","last_name":"Poudel","full_name":"Poudel, Bed"},{"full_name":"Nozariasbmarz, Amin","first_name":"Amin","last_name":"Nozariasbmarz"},{"full_name":"Li, Wenjie","first_name":"Wenjie","last_name":"Li"},{"full_name":"Ibáñez, Maria","id":"43C61214-F248-11E8-B48F-1D18A9856A87","orcid":"0000-0001-5013-2843","first_name":"Maria","last_name":"Ibáñez"},{"full_name":"Cabot, Andreu","last_name":"Cabot","first_name":"Andreu"}],"quality_controlled":"1","isi":1,"external_id":{"isi":["000976063200001"],"pmid":["37071412"]},"language":[{"iso":"eng"}],"doi":"10.1021/acsnano.3c00495","month":"05","publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"status":"public","title":"Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites","intvolume":" 17","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","_id":"12915","oa_version":"None","type":"journal_article","abstract":[{"lang":"eng","text":"Cu2–xS and Cu2–xSe have recently been reported as promising thermoelectric (TE) materials for medium-temperature applications. In contrast, Cu2–xTe, another member of the copper chalcogenide family, typically exhibits low Seebeck coefficients that limit its potential to achieve a superior thermoelectric figure of merit, zT, particularly in the low-temperature range where this material could be effective. To address this, we investigated the TE performance of Cu1.5–xTe–Cu2Se nanocomposites by consolidating surface-engineered Cu1.5Te nanocrystals. This surface engineering strategy allows for precise adjustment of Cu/Te ratios and results in a reversible phase transition at around 600 K in Cu1.5–xTe–Cu2Se nanocomposites, as systematically confirmed by in situ high-temperature X-ray diffraction combined with differential scanning calorimetry analysis. The phase transition leads to a conversion from metallic-like to semiconducting-like TE properties. Additionally, a layer of Cu2Se generated around Cu1.5–xTe nanoparticles effectively inhibits Cu1.5–xTe grain growth, minimizing thermal conductivity and decreasing hole concentration. These properties indicate that copper telluride based compounds have a promising thermoelectric potential, translated into a high dimensionless zT of 1.3 at 560 K."}],"issue":"9","article_type":"original","page":"8442-8452","publication":"ACS Nano","citation":{"chicago":"Xing, Congcong, Yu Zhang, Ke Xiao, Xu Han, Yu Liu, Bingfei Nan, Maria Garcia Ramon, et al. “Thermoelectric Performance of Surface-Engineered Cu1.5–XTe–Cu2Se Nanocomposites.” ACS Nano. American Chemical Society, 2023. https://doi.org/10.1021/acsnano.3c00495.","short":"C. Xing, Y. Zhang, K. Xiao, X. Han, Y. Liu, B. Nan, M.G. Ramon, K.H. Lim, J. Li, J. Arbiol, B. Poudel, A. Nozariasbmarz, W. Li, M. Ibáñez, A. Cabot, ACS Nano 17 (2023) 8442–8452.","mla":"Xing, Congcong, et al. “Thermoelectric Performance of Surface-Engineered Cu1.5–XTe–Cu2Se Nanocomposites.” ACS Nano, vol. 17, no. 9, American Chemical Society, 2023, pp. 8442–52, doi:10.1021/acsnano.3c00495.","ieee":"C. Xing et al., “Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites,” ACS Nano, vol. 17, no. 9. American Chemical Society, pp. 8442–8452, 2023.","apa":"Xing, C., Zhang, Y., Xiao, K., Han, X., Liu, Y., Nan, B., … Cabot, A. (2023). Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. ACS Nano. American Chemical Society. https://doi.org/10.1021/acsnano.3c00495","ista":"Xing C, Zhang Y, Xiao K, Han X, Liu Y, Nan B, Ramon MG, Lim KH, Li J, Arbiol J, Poudel B, Nozariasbmarz A, Li W, Ibáñez M, Cabot A. 2023. Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. ACS Nano. 17(9), 8442–8452.","ama":"Xing C, Zhang Y, Xiao K, et al. Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. ACS Nano. 2023;17(9):8442-8452. doi:10.1021/acsnano.3c00495"},"date_published":"2023-05-09T00:00:00Z","scopus_import":"1","day":"09","article_processing_charge":"No"},{"article_number":"117369","year":"2023","acknowledgement":"This work was carried out within the framework of the project Combenergy, PID2019-105490RB-C32, financed by the Spanish MCIN/AEI/10.13039/501100011033. ICN2 is supported by the Severo Ochoa program from Spanish MCIN / AEI (Grant No.: CEX2021-001214-S). IREC and ICN2 are funded by the CERCA Programme from the Generalitat de Catalunya. Part of the present work has been performed in the frameworks of the Universitat de Barcelona Nanoscience PhD program. ICN2 acknowledges funding from Generalitat de Catalunya 2021SGR00457. This study was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and Generalitat de Catalunya. The authors thank the support from the project NANOGEN (PID2020-116093RB-C43), funded by MCIN/ AEI/10.13039/501100011033/ and by “ERDF A way of making Europe”, by the European Union. The project on which these results are based has received funding from the European Union's Horizon 2020 research and innovation programme under Marie Skłodowska-Curie grant agreement No. 801342 (Tecniospring INDUSTRY) and the Government of Catalonia's Agency for Business Competitiveness (ACCIÓ). J. Li is grateful for the project supported by the Natural Science Foundation of Sichuan (2022NSFSC1229). M.I. acknowledges funding by ISTA and the Werner Siemens Foundation.","department":[{"_id":"MaIb"}],"publisher":"Elsevier","publication_status":"published","author":[{"first_name":"Guillem","last_name":"Montaña-Mora","full_name":"Montaña-Mora, Guillem"},{"full_name":"Qi, Xueqiang","last_name":"Qi","first_name":"Xueqiang"},{"first_name":"Xiang","last_name":"Wang","full_name":"Wang, Xiang"},{"first_name":"Jesus","last_name":"Chacón-Borrero","full_name":"Chacón-Borrero, Jesus"},{"last_name":"Martinez-Alanis","first_name":"Paulina R.","full_name":"Martinez-Alanis, Paulina R."},{"first_name":"Xiaoting","last_name":"Yu","full_name":"Yu, Xiaoting"},{"full_name":"Li, Junshan","last_name":"Li","first_name":"Junshan"},{"full_name":"Xue, Qian","first_name":"Qian","last_name":"Xue"},{"first_name":"Jordi","last_name":"Arbiol","full_name":"Arbiol, Jordi"},{"full_name":"Ibáñez, Maria","orcid":"0000-0001-5013-2843","id":"43C61214-F248-11E8-B48F-1D18A9856A87","last_name":"Ibáñez","first_name":"Maria"},{"full_name":"Cabot, Andreu","last_name":"Cabot","first_name":"Andreu"}],"volume":936,"date_updated":"2023-10-04T11:52:33Z","date_created":"2023-04-16T22:01:06Z","publication_identifier":{"issn":["1572-6657"]},"month":"05","external_id":{"isi":["000967060900001"]},"project":[{"name":"HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of Semiconductors for Waste Heat Recovery","_id":"9B8F7476-BA93-11EA-9121-9846C619BF3A"}],"isi":1,"quality_controlled":"1","doi":"10.1016/j.jelechem.2023.117369","language":[{"iso":"eng"}],"type":"journal_article","abstract":[{"lang":"eng","text":"The deployment of direct formate fuel cells (DFFCs) relies on the development of active and stable catalysts for the formate oxidation reaction (FOR). Palladium, providing effective full oxidation of formate to CO2, has been widely used as FOR catalyst, but it suffers from low stability, moderate activity, and high cost. Herein, we detail a colloidal synthesis route for the incorporation of P on Pd2Sn nanoparticles. These nanoparticles are dispersed on carbon black and the obtained composite is used as electrocatalytic material for the FOR. The Pd2Sn0.8P-based electrodes present outstanding catalytic activities with record mass current densities up to 10.0 A mgPd-1, well above those of Pd1.6Sn/C reference electrode. These high current densities are further enhanced by increasing the temperature from 25 °C to 40 °C. The Pd2Sn0.8P electrode also allows for slowing down the rapid current decay that generally happens during operation and can be rapidly re-activated through potential cycling. The excellent catalytic performance obtained is rationalized using density functional theory (DFT) calculations."}],"user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","_id":"12829","intvolume":" 936","status":"public","title":"Phosphorous incorporation into palladium tin nanoparticles for the electrocatalytic formate oxidation reaction","oa_version":"None","scopus_import":"1","article_processing_charge":"No","day":"01","citation":{"chicago":"Montaña-Mora, Guillem, Xueqiang Qi, Xiang Wang, Jesus Chacón-Borrero, Paulina R. Martinez-Alanis, Xiaoting Yu, Junshan Li, et al. “Phosphorous Incorporation into Palladium Tin Nanoparticles for the Electrocatalytic Formate Oxidation Reaction.” Journal of Electroanalytical Chemistry. Elsevier, 2023. https://doi.org/10.1016/j.jelechem.2023.117369.","short":"G. Montaña-Mora, X. Qi, X. Wang, J. Chacón-Borrero, P.R. Martinez-Alanis, X. Yu, J. Li, Q. Xue, J. Arbiol, M. Ibáñez, A. Cabot, Journal of Electroanalytical Chemistry 936 (2023).","mla":"Montaña-Mora, Guillem, et al. “Phosphorous Incorporation into Palladium Tin Nanoparticles for the Electrocatalytic Formate Oxidation Reaction.” Journal of Electroanalytical Chemistry, vol. 936, 117369, Elsevier, 2023, doi:10.1016/j.jelechem.2023.117369.","apa":"Montaña-Mora, G., Qi, X., Wang, X., Chacón-Borrero, J., Martinez-Alanis, P. R., Yu, X., … Cabot, A. (2023). Phosphorous incorporation into palladium tin nanoparticles for the electrocatalytic formate oxidation reaction. Journal of Electroanalytical Chemistry. Elsevier. https://doi.org/10.1016/j.jelechem.2023.117369","ieee":"G. Montaña-Mora et al., “Phosphorous incorporation into palladium tin nanoparticles for the electrocatalytic formate oxidation reaction,” Journal of Electroanalytical Chemistry, vol. 936. Elsevier, 2023.","ista":"Montaña-Mora G, Qi X, Wang X, Chacón-Borrero J, Martinez-Alanis PR, Yu X, Li J, Xue Q, Arbiol J, Ibáñez M, Cabot A. 2023. Phosphorous incorporation into palladium tin nanoparticles for the electrocatalytic formate oxidation reaction. Journal of Electroanalytical Chemistry. 936, 117369.","ama":"Montaña-Mora G, Qi X, Wang X, et al. Phosphorous incorporation into palladium tin nanoparticles for the electrocatalytic formate oxidation reaction. Journal of Electroanalytical Chemistry. 2023;936. doi:10.1016/j.jelechem.2023.117369"},"publication":"Journal of Electroanalytical Chemistry","article_type":"original","date_published":"2023-05-01T00:00:00Z"},{"abstract":[{"lang":"eng","text":"A light-triggered fabrication method extends the functionality of printable nanomaterials"}],"issue":"6665","type":"journal_article","oa_version":"None","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","_id":"14404","status":"public","title":"Widening the use of 3D printing","intvolume":" 381","day":"29","article_processing_charge":"No","scopus_import":"1","date_published":"2023-09-29T00:00:00Z","publication":"Science","citation":{"chicago":"Balazs, Daniel, and Maria Ibáñez. “Widening the Use of 3D Printing.” Science. AAAS, 2023. https://doi.org/10.1126/science.adk3070.","mla":"Balazs, Daniel, and Maria Ibáñez. “Widening the Use of 3D Printing.” Science, vol. 381, no. 6665, AAAS, 2023, pp. 1413–14, doi:10.1126/science.adk3070.","short":"D. Balazs, M. Ibáñez, Science 381 (2023) 1413–1414.","ista":"Balazs D, Ibáñez M. 2023. Widening the use of 3D printing. Science. 381(6665), 1413–1414.","ieee":"D. Balazs and M. Ibáñez, “Widening the use of 3D printing,” Science, vol. 381, no. 6665. AAAS, pp. 1413–1414, 2023.","apa":"Balazs, D., & Ibáñez, M. (2023). Widening the use of 3D printing. Science. AAAS. https://doi.org/10.1126/science.adk3070","ama":"Balazs D, Ibáñez M. Widening the use of 3D printing. Science. 2023;381(6665):1413-1414. doi:10.1126/science.adk3070"},"article_type":"letter_note","page":"1413-1414","author":[{"id":"302BADF6-85FC-11EA-9E3B-B9493DDC885E","orcid":"0000-0001-7597-043X","first_name":"Daniel","last_name":"Balazs","full_name":"Balazs, Daniel"},{"full_name":"Ibáñez, Maria","last_name":"Ibáñez","first_name":"Maria","orcid":"0000-0001-5013-2843","id":"43C61214-F248-11E8-B48F-1D18A9856A87"}],"date_created":"2023-10-08T22:01:16Z","date_updated":"2023-10-09T07:32:58Z","volume":381,"acknowledgement":"The authors thank the Werner-Siemens-Stiftung and the Institute of Science and Technology Austria for financial support.","year":"2023","pmid":1,"publication_status":"published","publisher":"AAAS","department":[{"_id":"MaIb"},{"_id":"LifeSc"}],"month":"09","publication_identifier":{"eissn":["1095-9203"]},"doi":"10.1126/science.adk3070","language":[{"iso":"eng"}],"external_id":{"pmid":["37769110"]},"quality_controlled":"1","project":[{"name":"HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of Semiconductors for Waste Heat Recovery","_id":"9B8F7476-BA93-11EA-9121-9846C619BF3A"}]},{"day":"30","article_processing_charge":"Yes (via OA deal)","has_accepted_license":"1","keyword":["Colloid and Surface Chemistry","Biochemistry","General Chemistry","Catalysis"],"date_published":"2023-06-30T00:00:00Z","article_type":"original","page":"14894-14902","publication":"Journal of the American Chemical Society","citation":{"apa":"Bunting, R., Wodaczek, F., Torabi, T., & Cheng, B. (2023). Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane. Journal of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/jacs.3c04030","ieee":"R. Bunting, F. Wodaczek, T. Torabi, and B. Cheng, “Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane,” Journal of the American Chemical Society, vol. 145, no. 27. American Chemical Society, pp. 14894–14902, 2023.","ista":"Bunting R, Wodaczek F, Torabi T, Cheng B. 2023. Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane. Journal of the American Chemical Society. 145(27), 14894–14902.","ama":"Bunting R, Wodaczek F, Torabi T, Cheng B. Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane. Journal of the American Chemical Society. 2023;145(27):14894-14902. doi:10.1021/jacs.3c04030","chicago":"Bunting, Rhys, Felix Wodaczek, Tina Torabi, and Bingqing Cheng. “Reactivity of Single-Atom Alloy Nanoparticles: Modeling the Dehydrogenation of Propane.” Journal of the American Chemical Society. American Chemical Society, 2023. https://doi.org/10.1021/jacs.3c04030.","short":"R. Bunting, F. Wodaczek, T. Torabi, B. Cheng, Journal of the American Chemical Society 145 (2023) 14894–14902.","mla":"Bunting, Rhys, et al. “Reactivity of Single-Atom Alloy Nanoparticles: Modeling the Dehydrogenation of Propane.” Journal of the American Chemical Society, vol. 145, no. 27, American Chemical Society, 2023, pp. 14894–902, doi:10.1021/jacs.3c04030."},"abstract":[{"lang":"eng","text":"Physical catalysts often have multiple sites where reactions can take place. One prominent example is single-atom alloys, where the reactive dopant atoms can preferentially locate in the bulk or at different sites on the surface of the nanoparticle. However, ab initio modeling of catalysts usually only considers one site of the catalyst, neglecting the effects of multiple sites. Here, nanoparticles of copper doped with single-atom rhodium or palladium are modeled for the dehydrogenation of propane. Single-atom alloy nanoparticles are simulated at 400–600 K, using machine learning potentials trained on density functional theory calculations, and then the occupation of different single-atom active sites is identified using a similarity kernel. Further, the turnover frequency for all possible sites is calculated for propane dehydrogenation to propene through microkinetic modeling using density functional theory calculations. The total turnover frequencies of the whole nanoparticle are then described from both the population and the individual turnover frequency of each site. Under operating conditions, rhodium as a dopant is found to almost exclusively occupy (111) surface sites while palladium as a dopant occupies a greater variety of facets. Undercoordinated dopant surface sites are found to tend to be more reactive for propane dehydrogenation compared to the (111) surface. It is found that considering the dynamics of the single-atom alloy nanoparticle has a profound effect on the calculated catalytic activity of single-atom alloys by several orders of magnitude."}],"issue":"27","type":"journal_article","oa_version":"Published Version","file":[{"relation":"main_file","file_id":"13219","checksum":"e07d5323f9c0e5cbd1ad6453f29440ab","success":1,"date_updated":"2023-07-12T10:22:04Z","date_created":"2023-07-12T10:22:04Z","access_level":"open_access","file_name":"2023_JACS_Bunting.pdf","file_size":3155843,"content_type":"application/pdf","creator":"cchlebak"}],"title":"Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane","status":"public","ddc":["540"],"intvolume":" 145","user_id":"8b945eb4-e2f2-11eb-945a-df72226e66a9","_id":"13216","month":"06","publication_identifier":{"eissn":["1520-5126"],"issn":["0002-7863"]},"language":[{"iso":"eng"}],"doi":"10.1021/jacs.3c04030","quality_controlled":"1","isi":1,"tmp":{"name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","short":"CC BY (4.0)","image":"/images/cc_by.png"},"oa":1,"external_id":{"isi":["001020623900001"],"pmid":["37390457"]},"file_date_updated":"2023-07-12T10:22:04Z","date_created":"2023-07-12T09:16:40Z","date_updated":"2023-10-11T08:45:10Z","volume":145,"author":[{"last_name":"Bunting","first_name":"Rhys","orcid":"0000-0001-6928-074X","id":"91deeae8-1207-11ec-b130-c194ad5b50c6","full_name":"Bunting, Rhys"},{"id":"8b4b6a9f-32b0-11ee-9fa8-bbe85e26258e","orcid":"0009-0000-1457-795X","first_name":"Felix","last_name":"Wodaczek","full_name":"Wodaczek, Felix"},{"full_name":"Torabi, Tina","last_name":"Torabi","first_name":"Tina"},{"orcid":"0000-0002-3584-9632","id":"cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9","last_name":"Cheng","first_name":"Bingqing","full_name":"Cheng, Bingqing"}],"publication_status":"published","department":[{"_id":"MaIb"},{"_id":"BiCh"}],"publisher":"American Chemical Society","year":"2023","acknowledgement":"B.C. acknowledges resources provided by the Cambridge Tier2 system operated by the University of Cambridge Research\r\nComputing Service funded by EPSRC Tier-2 capital grant EP/\r\nP020259/1.","pmid":1}]