文献类型：期刊文献

英文题名：Cascade Dual Sites Modulate Local CO Coverage and Hydrogen-Binding Strength to Boost CO2 Electroreduction to Ethylene

作者：Li, Junjun[1,2];Chen, Yu[3];Yao, Bingqing[4];Yang, Wenjuan[5];Cui, Xiaoya[6];Liu, Huiling[7];Dai, Sheng[8,9];Xi, Shibo[10];Sun, Zhiyi[11];Chen, Wenxing[11];Qin, Yuchen[12];Wang, Jinlan[3];He, Qian[4];Ling, Chongyi[3];Wang, Dingsheng[13];Zhang, Zhicheng[1,2]

机构：[1]Tianjin Univ, Sch Sci, Dept Chem, Tianjin 300072, Peoples R China;[2]Tianjin Univ, Tianjin Key Lab Mol Optoelect Sci, Tianjin 300072, Peoples R China;[3]Southeast Univ, Sch Phys, Key Lab Quantum Mat & Devices, Minist Educ, Nanjing 211189, Peoples R China;[4]Natl Univ Singapore, Coll Design & Engn, Dept Mat Sci & Engn, Singapore 117575, Singapore;[5]Shenzhen Technol Univ, Julong Coll, Shenzhen 518118, Peoples R China;[6]Tsinghua Univ, Beijing Adv Innovat Ctr Struct Biol, Minist Educ, Key Lab Prot Sci,Sch Life Sci, Beijing 100084, Peoples R China;[7]Tianjin Univ Technol, Inst New Energy Mat & Low Carbon Technol, Sch Mat Sci & Engn, Tianjin Key Lab Adv Funct Porous Mat, Tianjin 300384, Peoples R China;[8]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[9]East China Univ Sci & Technol, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China;[10]ASTAR, Inst Sustainabil Chem Energy & Environm ISCE2, Singapore 627833, Singapore;[11]Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Construct Tailorable Adv Funct Mat, Beijing 100081, Peoples R China;[12]Henan Agr Univ, Coll Sci, Zhengzhou 450000, Peoples R China;[13]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

年份：2024

卷号：146

期号：8

起止页码：5693

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20240815582917);WOS:【SCI-EXPANDED(收录号:WOS:001167238200001)】；

基金：This work was supported by the National Natural Science Foundation of China (22071172, 22375142, and 22325101), 2022 Subsidized Project of Tianjin University Graduate Arts and Science Excellence Innovation Award Program (B2-2022-002), the Basic Research Program of Jiangsu Province (BK20220800), and the Fundamental Research Funds for the Central Universities (3207022307A2). The authors thank the computational resources from the Big Data Center of Southeast University. Q.H. acknowledges the support of the National Research Foundation (NRF), Singapore, under its NRF Fellowship (NRF-NRFF11-2019-0002) and the Singapore Low-Carbon Energy Research Funding Initiative (award number LCERFI01-0017). The authors thank the BL14W1 in the Shanghai Synchrotron Radiation Facility (SSRF) for the help with characterizations.

语种：英文

外文关键词：Binding sites - Copper - Electrolytic reduction - Ethylene - Hydrogen - Reaction intermediates - Silver - Surface reactions

摘要：Rationally modulating the binding strength of reaction intermediates on surface sites of copper-based catalysts could facilitate C-C coupling to generate multicarbon products in an electrochemical CO2 reduction reaction. Herein, theoretical calculations reveal that cascade Ag-Cu dual sites could synergistically increase local CO coverage and lower the kinetic barrier for CO protonation, leading to enhanced asymmetric C-C coupling to generate C2H4. As a proof of concept, the Cu3N-Ag nanocubes (NCs) with Ag located in partial Cu sites and a Cu3N unit center are successfully synthesized. The Faraday efficiency and partial current density of C2H4 over Cu3N-Ag NCs are 7.8 and 9.0 times those of Cu3N NCs, respectively. In situ spectroscopies combined with theoretical calculations confirm that Ag sites produce CO and Cu sites promote asymmetric C-C coupling to *COCHO, significantly enhancing the generation of C2H4. Our work provides new insights into the cascade catalysis strategy at the atomic scale for boosting CO2 to multicarbon products.