Selective and Stable CO2 Electroreduction to CH4 via Electronic Metal-Support Interaction upon Decomposition/Redeposition of MOF

被引:28
|
作者
Liu, Guanyu [1 ,2 ,3 ]
Trinh, Quang Thang [4 ,5 ]
Wang, Haojing [2 ]
Wu, Shuyang [2 ,3 ]
Arce-Ramos, Juan Manuel [4 ]
Sullivan, Michael B.
Kraft, Markus [3 ,6 ]
Ager, Joel W. W. [7 ,8 ]
Zhang, Jia [4 ]
Xu, Rong [2 ,3 ]
机构
[1] Tongji Univ, Sch Mat Sci & Engn, Shanghai 201804, Peoples R China
[2] Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore
[3] Cambridge Ctr Adv Res & Educ Singapore CARES, CREATE Tower,1 Create Way, Singapore 138602, Singapore
[4] ASTAR, Inst High Performance Comp IHPC, 1 Fusionopolis Way 16-16 Connexis, Singapore 138632, Singapore
[5] Griffith Univ, Queensland Micro & Nanotechnol Ctr, Nathan Campus,170 Kessels Rd, Brisbane, Qld 4111, Australia
[6] Univ Cambridge, Dept Chem Engn & Biotechnol, West Cambridge Site,Philippa Fawcett Dr, Cambridge CB3 0AS, England
[7] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
[8] Berkeley Educ Alliance Res Singapore BEARS, 1 Create Way, Singapore 138602, Singapore
基金
新加坡国家研究基金会;
关键词
CO2; reduction; copper-based catalysts; density functional theory calculations; metal-support interaction; metal-organic frameworks (MOFs); INITIO MOLECULAR-DYNAMICS; DENSITY-FUNCTIONAL THEORY; X-RAY SPECTROSCOPY; ELECTROCHEMICAL REDUCTION; CARBONACEOUS MATERIALS; COMBINING EXPERIMENTS; REACTION-MECHANISMS; ENERGY CALCULATIONS; ORGANIC FRAMEWORK; CU CLUSTERS;
D O I
10.1002/smll.202301379
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The CO2 electroreduction to fuels is a feasible approach to provide renewable energy sources. Therefore, it is necessary to conduct experimental and theoretical investigations on various catalyst design strategies, such as electronic metal-support interaction, to improve the catalytic selectivity. Here a solvent-free synthesis method is reported to prepare a copper (Cu)-based metal-organic framework (MOF) as the precursor. Upon electrochemical CO2 reduction in aqueous electrolyte, it undergoes in situ decomposition/redeposition processes to form abundant interfaces between Cu nanoparticles and amorphous carbon supports. This Cu/C catalyst favors the selective and stable production of CH4 with a Faradaic efficiency of approximate to 55% at -1.4 V versus reversible hydrogen electrode (RHE) for 12.5 h. The density functional theory calculation reveals the crucial role of interfacial sites between Cu and amorphous carbon support in stabilizing the key intermediates for CO2 reduction to CH4. The adsorption of COOH* and CHO* at the Cu/C interface is up to 0.86 eV stronger than that on Cu(111), thus promoting the formation of CH4. Therefore, it is envisioned that the strategy of regulating electronic metal-support interaction can improve the selectivity and stability of catalyst toward a specific product upon electrochemical CO2 reduction.
引用
收藏
页数:11
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