化学
氧合物
电化学
金属
碳纤维
联轴节(管道)
金属有机骨架
乙烯
乙醇
无机化学
催化作用
电极
物理化学
有机化学
吸附
复合材料
工程类
材料科学
复合数
机械工程
作者
Zhen‐Hua Zhao,Jia‐Run Huang,Pei‐Qin Liao,Xiao‐Ming Chen
摘要
The electroreduction of CO2 into value-added liquid fuels holds great promise for addressing global environmental and energy challenges. However, achieving highly selective yielding of multi-carbon oxygenates through the electrochemical CO2 reduction reaction (eCO2RR) is a formidable task, primarily due to the sluggish asymmetric C-C coupling reaction. In this study, a novel metal-organic framework (CuSn-HAB) with unprecedented heterometallic Sn···Cu dual sites (namely, a pair of SnN2O2 and CuN4 sites bridged by μ-N atoms) was designed to overcome this limitation. CuSn-HAB demonstrated an impressive Faradic efficiency (FE) of 56(2)% for eCO2RR to alcohols, achieving a current density of 68 mA cm-2 at a low potential of -0.57 V (vs RHE). Notably, no significant degradation was observed over a continuous 35 h operation at the specified current density. Mechanistic investigations revealed that, in comparison to the copper site, the SnN2O2 site exhibits a higher affinity for oxygen atoms. This enhanced affinity plays a pivotal role in facilitating the generation of the key intermediate *OCH2. Consequently, compared to homometallic Cu···Cu dual sites (generally yielding ethylene product), the heterometallic dual sites were proved to be more thermodynamically favorable for the asymmetric C-C coupling between *CO and *OCH2, leading to the formation of the key intermediate *CO-*OCH2, which is favorable for yielding ethanol product.
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