电合成
碳酸二甲酯
催化作用
材料科学
氧化还原
无机化学
碳酸盐
化学工程
电化学
有机化学
冶金
电极
物理化学
化学
工程类
作者
Naohiro Fujinuma,Natalie Page,Anna G Boddy,Joshua Rivkind,L. Tomlinson,Erik P. Hoy,S. E. Lofland
标识
DOI:10.1002/adfm.202412402
摘要
Abstract This study reports ambient electrosynthesis of dimethyl carbonate with a palladium–gold catalyst. Material screening identifies a region of intermediate‐catalyst binding energy that facilitates interfacial electron and proton transfers for selective carbonylation, achieving a distinct maximum of 92% faradaic efficiency to dimethyl carbonate. Structural and electrochemical analyses suggest that the alloying of palladium and gold effectively modulates the CO* binding energy to the catalytic surface, in accord with subsequent computational studies. With an extended heterogeneous–homogeneous catalytic environment with a halide redox mediator, a remarkable partial current density of 52 mA cm −2 is observed for dimethyl carbonate for 100 h of continuous operation.
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