化学
电合成
二氧化碳电化学还原
电化学
一氧化碳
无机化学
二氧化碳
铜
吸附
催化作用
有机化学
电极
物理化学
作者
Jing Gao,Ali M. Bahmanpour,Oliver Kröcher,Shaik M. Zakeeruddin,Dan Ren,Michaël Grätzel
出处
期刊:Nature Chemistry
[Springer Nature]
日期:2023-04-06
卷期号:15 (5): 705-713
被引量:49
标识
DOI:10.1038/s41557-023-01163-8
摘要
Abstract 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.
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