Jie Wang, Min Wang, Yang Wang, Zixuan Wei, Xin He, Haojie Zang, Xixiong Jin, Lingxia Zhang
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引用次数: 0
Abstract
For CO2 electroreduction, efficient catalysts with superior selectivity toward multi-carbon (C2+) products (such as C2H4, C2H5OH, etc.) are intensely desired. Amorphous Cu-based catalysts show appealing performance on the crucial C–C coupling, but their synthesis procedures are complicated and their actual mechanisms are still unclear. In this work, surface amorphization has been implemented on Cu2(OH)2CO3 catalysts by a very simple microwave-induction method, improving the Faradaic efficiency for C2+ products (\({\rm FE}_{{\rm C}_{2+}}\)) up to 86% (increased by ∼26% than that on Cu2(OH)2CO3) at a partial current density of 258 mA cm−2, and a high \({\rm FE}_{{\rm C}_{2+}}\) of 75% at 500 mA cm−2 in a flow cell. Moreover, the catalyst exhibits good stability. In situ investigations disclose that the amorphous surface optimizes the adsorption state (binding mode and coverage) of key intermediate *CO and stabilizes Cu+ pieces, facilitating the dimerization of *CO into *OCCO and hydrogenation to *OC2H5, ultimately achieving high yields of C2+ products. This work highlights a simple microwave approach for surface amorphization and the roles of amorphous features in CO2 reduction to C2+ products, which could be valuable references for designing high-performance catalysts for CO2 electroreduction.
对于CO2电还原,迫切需要对多碳(C2+)产物(如C2H4, C2H5OH等)具有优越选择性的高效催化剂。非晶铜基催化剂在关键的碳-碳偶联反应上表现出令人满意的性能,但其合成过程复杂,实际机理尚不清楚。在这项工作中,通过一种非常简单的微波感应方法在Cu2(OH)2CO3催化剂上实现了表面非晶化,将C2+产物的法拉第效率(\({\rm FE}_{{\rm C}_{2+}}\))提高到86% (increased by ∼26% than that on Cu2(OH)2CO3) at a partial current density of 258 mA cm−2, and a high \({\rm FE}_{{\rm C}_{2+}}\) of 75% at 500 mA cm−2 in a flow cell. Moreover, the catalyst exhibits good stability. In situ investigations disclose that the amorphous surface optimizes the adsorption state (binding mode and coverage) of key intermediate *CO and stabilizes Cu+ pieces, facilitating the dimerization of *CO into *OCCO and hydrogenation to *OC2H5, ultimately achieving high yields of C2+ products. This work highlights a simple microwave approach for surface amorphization and the roles of amorphous features in CO2 reduction to C2+ products, which could be valuable references for designing high-performance catalysts for CO2 electroreduction.
期刊介绍:
Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field.
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