In-situ constructed Cu/CuNC interfaces for low-overpotential reduction of CO2 to ethanol

被引:41
作者
Yang, Yan [1 ,6 ,7 ]
Fu, Jiaju [1 ]
Ouyang, Yixin [2 ]
Tang, Tang [1 ]
Zhang, Yun [3 ]
Zheng, Li-Rong [4 ]
Zhang, Qing-Hua [5 ]
Liu, Xiao-Zhi [5 ,7 ]
Wang, Jinlan [2 ]
Hu, Jin-Song [1 ,7 ]
机构
[1] Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci BNLMS, CAS Key Lab Mol Nanostruct & Nanotechnol, Beijing 100190, Peoples R China
[2] Southeast Univ, Sch Phys, Nanjing 211189, Peoples R China
[3] Shenzhen Univ, Inst Adv Study, Shenzhen 518060, Peoples R China
[4] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
[5] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
[6] Zhejiang Tiandi Environm Protect Technol Co Ltd, Res Inst, Hangzhou 310003, Peoples R China
[7] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
关键词
Cu; CuNC interface; low overpotential; CO2; reduction; ethanol; electrocatalysis; TOTAL-ENERGY CALCULATIONS; ELASTIC BAND METHOD; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; COPPER; ELECTROREDUCTION; INSIGHTS; IONS;
D O I
10.1093/nsr/nwac248
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Electrochemical CO2 reduction (ECR) to high-value multi-carbon (C2+) products is critical to sustainable energy conversion, yet the high energy barrier of C-C coupling causes catalysts to suffer high overpotential and low selectivity toward specific liquid C2+ products. Here, the electronically asymmetric Cu-Cu/Cu-N-C (Cu/CuNC) interface site is found, by theoretical calculations, to enhance the adsorption of *CO intermediates and decrease the reaction barrier of C-C coupling in ECR, enabling efficient C-C coupling at low overpotential. The catalyst consisting of high-density Cu/CuNC interface sites (noted as ER-Cu/CuNC) is then accordingly designed and constructed in situ on the high-loading Cu-N-C single atomic catalysts. Systematical experiments corroborate the theoretical prediction that the ER-Cu/CuNC boosts electrocatalytic CO2-to-ethanol conversion with a Faradaic efficiency toward C2+ of 60.3% (FEethanol of 55%) at a low overpotential of -0.35 V. These findings provide new insights and an attractive approach to creating electronically asymmetric dual sites for efficient conversion of CO2 to C2+ products. Cu-Cu/Cu-N-C multiatomic sites are discovered and achieved to synergistically promote the electrochemical reduction of CO2 into ethanol at low overpotentials by effectively lowering the energy barrier of C-C coupling.
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页数:9
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