Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals

被引:98
作者
Gao, Jing [1 ]
Bahmanpour, Alimohammad [2 ]
Krocher, Oliver [2 ,3 ]
Zakeeruddin, Shaik M. [1 ]
Ren, Dan [1 ,4 ]
Gratzel, Michael [1 ]
机构
[1] Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Lausanne, Switzerland
[2] Ecole Polytech Fed Lausanne, Grp Catalysis Biofuels, Lausanne, Switzerland
[3] Paul Scherrer Inst, Villigen, Switzerland
[4] Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian, Peoples R China
基金
瑞士国家科学基金会;
关键词
ENERGY-ELECTRON DIFFRACTION; ELECTROCATALYTIC CONVERSION; UNDERPOTENTIAL DEPOSITION; CO2; ELECTROREDUCTION; REDUCTION; CU; SELECTIVITY; CATALYSIS; INSIGHTS; ETHYLENE;
D O I
10.1038/s41557-023-01163-8
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The conversion of carbon dioxide to value-added products using renewable electricity would potentially help to address current climate concerns. The electrochemical reduction of carbon dioxide to propylene, a critical feedstock, requires multiple C-C coupling steps with the transfer of 18 electrons per propylene molecule, and hence is kinetically sluggish. Here we present the electrosynthesis of propylene from carbon dioxide on copper nanocrystals with a peak geometric current density of -5.5 mA cm(-2). The metallic copper nanocrystals formed from CuCl precursor present preponderant Cu(100) and Cu(111) facets, likely to favour the adsorption of key *C-1 and *C-2 intermediates. Strikingly, the production rate of propylene drops substantially when carbon monoxide is used as the reactant. From the electrochemical reduction of isotope-labelled carbon dioxide mixed with carbon monoxide, we infer that the key step for propylene formation is probably the coupling between adsorbed/molecular carbon dioxide or carboxyl with the *C-2 intermediates that are involved in the ethylene pathway.
引用
收藏
页码:705 / +
页数:19
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