催化作用
铜
法拉第效率
化学
氧化还原
电极
电化学
无机化学
物理化学
有机化学
作者
Yu Zhang,Yicheng Li,Nana Gao,Ernest Pahuyo Delmo,Jiang Wu,A-Li Luo,Dongyang Wang,Ke Chen,Markus Antonietti,Tianxi Liu,Zhihong Tian
标识
DOI:10.1002/anie.202404676
摘要
Copper (Cu)-based catalysts have established their unique capability for yielding wide value-added products from CO2. Herein, we demonstrate that the pathways of the electrocatalytic CO2 reduction reaction (CO2RR) can be rationally altered toward C1 or C2+ products by simply optimizing the coordination of Cu with O-containing organic species (squarate (C4O4) and cyclohexanhexanone (C6O6)). It is revealed that the strength of Cu-O bonds can significantly affect the morphologies and electronic structures of derived Cu catalysts, resulting in the distinct behaviors during CO2RR. Specifically, the C6O6-Cu catalysts made up from organized nanodomains shows a dominant C1 pathway with a total Faradaic efficiency (FE) of 63.7% at -1.0 V (versus reversible hydrogen electrode, RHE). In comparison, the C4O4-Cu with an about perfect crystalline structure results in uniformly dispersed Cu-atoms, showing a notable FE of 65.8% for C2+ products with enhanced capability of C-C coupling. The latter system also shows stable operation over at least 10 h with a high current density of 205.1 mA cm-2 at -1.0 VRHE, i.e. is already at the boarder of practical relevance. This study sheds light on the rational design of Cu-based catalysts for directing the CO2RR reaction pathway.
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