دورية أكاديمية
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Facet-switching of rate-determining step on copper in CO 2 -to-ethylene electroreduction.

التفاصيل البيبلوغرافية
العنوان: Facet-switching of rate-determining step on copper in CO 2 -to-ethylene electroreduction.
المؤلفون: Zhang YC; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Zhang XL; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Wu ZZ; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Niu ZZ; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Chi LP; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Gao FY; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Yang PP; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Wang YH; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Yu PC; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Duanmu JW; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Sun SP; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China., Gao MR; Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
المصدر: Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2024 Jun 18; Vol. 121 (25), pp. e2400546121. Date of Electronic Publication: 2024 Jun 10.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: National Academy of Sciences Country of Publication: United States NLM ID: 7505876 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1091-6490 (Electronic) Linking ISSN: 00278424 NLM ISO Abbreviation: Proc Natl Acad Sci U S A Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Original Publication: Washington, DC : National Academy of Sciences
مستخلص: Reduction of carbon dioxide (CO 2 ) by renewable electricity to produce multicarbon chemicals, such as ethylene (C 2 H 4 ), continues to be a challenge because of insufficient Faradaic efficiency, low production rates, and complex mechanistic pathways. Here, we report that the rate-determining steps (RDS) on common copper (Cu) surfaces diverge in CO 2 electroreduction, leading to distinct catalytic performances. Through a combination of experimental and computational studies, we reveal that C─C bond-making is the RDS on Cu(100), whereas the protonation of *CO with adsorbed water becomes rate-limiting on Cu(111) with a higher energy barrier. On an oxide-derived Cu(100)-dominant Cu catalyst, we reach a high C 2 H 4 Faradaic efficiency of 72%, partial current density of 359 mA cm -2 , and long-term stability exceeding 100 h at 500 mA cm -2 , greatly outperforming its Cu(111)-rich counterpart. We further demonstrate constant C 2 H 4 selectivity of >60% over 70 h in a membrane electrode assembly electrolyzer with a full-cell energy efficiency of 23.4%.
Competing Interests: Competing interests statement:The authors declare no competing interest.
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معلومات مُعتمدة: 22225901 MOST | National Natural Science Foundation of China (NSFC); 21975237 MOST | National Natural Science Foundation of China (NSFC); 22175162 MOST | National Natural Science Foundation of China (NSFC); WK2340000101 MOE | Fundamental Research Funds for the Central Universities (Fundamental Research Fund for the Central Universities); YD2340002007 University of Science and Technology of China (USTC); YD9990002017 University of Science and Technology of China (USTC); 2018YFA0702001 National Basic Research Program of China; 2023M733371 China Postdoctoral Science Foundation (China Postdoctoral Foundation Project); 2022M723032 China Postdoctoral Science Foundation (China Postdoctoral Foundation Project); 2023T160617 China Postdoctoral Science Foundation (China Postdoctoral Foundation Project); 2308085QB37 Natural Science Foundation Youth Project of Anhui Province; BX20230340 China National Postdoctoral Program for Innovative Talents
فهرسة مساهمة: Keywords: CO2 electroreduction; ethylene; facet; rate-determining step; selectivity and long-term stability
تواريخ الأحداث: Date Created: 20240610 Latest Revision: 20240626
رمز التحديث: 20240626
مُعرف محوري في PubMed: PMC11194607
DOI: 10.1073/pnas.2400546121
PMID: 38857407
قاعدة البيانات: MEDLINE
الوصف
تدمد:1091-6490
DOI:10.1073/pnas.2400546121