电催化剂
乙二醇
乙烯
氯化物
阳极
法拉第效率
化学
无机化学
电化学
偶联反应
电合成
化学工程
材料科学
催化作用
电极
物理化学
有机化学
工程类
作者
Linke Cai,Yao Liu,Ying Gao,Bo‐Hang Zhao,Jiacheng Guan,Lei Zhu,Bin Zhang,Yi Huang
标识
DOI:10.1002/anie.202417092
摘要
The chloride‐mediated ethylene oxidation reaction (EOR) of ethylene chlorohydrin (ECH) via electrocatalysis is practically attractive because of its sustainability and mild reaction conditions. However, the chlorine oxidation reaction (COR), which is essential for the above process, is commonly catalyzed by dimensionally stable anodes (DSAs) with high contents of precious Ru and/or Ir. The development of highly efficient COR electrocatalysts composed of nonprecious metals or decreased amounts of precious metals is highly desirable. Herein, we report a modified Co3O4 with a single‐atom Ir substitution (Ir1/Co3O4) as a highly efficient COR electrocatalyst for chloride‐mediated EOR to ECH in neutral seawater. Ir1/Co3O4 achieves a Faradaic efficiency (FE) of up to 94.8% for ECH generation and remarkable stability. Combining experimental results and density functional theory (DFT) calculations, the unique atomically asymmetrical Ir‐O‐Co configuration with a strong electron coupling effect in Ir1/Co3O4 can accelerate electron transfer to increase the reaction kinetics and maintain the structural stability of Co3O4 during COR. Moreover, a coupling reaction system integrating the anodic chloride‐mediated and cathodic H2O2‐mediated EOR show a total FE of ~170% for paired electrosynthesis of ECH and ethylene glycol (EG) using ethylene as the raw material. The technoeconomic analysis highlights the promising application prospects of this system.
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