Chengcheng Feng , Ruizhi Duan , Qin Zhou , Linqi Liu , Mingrun Li , Chunmei Ding , Can Li
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引用次数: 0
Abstract
Electrocatalytic CO2 reduction reaction (CO2RR) for producing valuable multi-carbon (C2+) chemicals is considered very promising, yet the rational design of catalysts and the regulation of reaction pathways remain difficult. Here, via introducing CeO2 on CuO catalyst, the Faradic efficiency of C2+ products, including C2H4 and ethanol, is obviously increased from 64% for CuO to as high as 87% for CeO2/CuO catalyst, along with a high partial current density of 0.52 A cm−2, and the C2H4 : C2H5OH ratio is obviously decreased. After introducing CeO2, CO2/CO adsorption is greatly enhanced as the electronic structure of Cu sites is regulated by CeO2, and H2O dissociation is promoted owing to the interfacial synergistic effect between Cu and CeO2. More importantly, the C–C coupling process changes from an endothermic process to a spontaneous *CO or *CHO dimerization process, which is critical for the enhanced selectivity of C2+ products. This work highlights that CeO2 promotes C–C coupling in CO2RR toward C2+ products on Cu-based catalysts by regulating adsorption properties.
电催化CO2还原反应(CO2RR)生产有价值的多碳化合物(C2+)被认为是很有前途的,但催化剂的合理设计和反应途径的调控仍然是一个难点。通过在CuO催化剂上引入CeO2, C2H4和乙醇等C2+产物的法拉奇效率由CuO催化剂的64%明显提高到CeO2/CuO催化剂的87%,分电流密度达到0.52 a cm−2,C2H4: C2H5OH比明显降低。引入CeO2后,由于Cu位点的电子结构受到CeO2的调控,CO2/CO的吸附能力大大增强,Cu和CeO2之间的界面协同作用促进了H2O的解离。更重要的是,C-C偶联过程由吸热过程转变为自发的*CO或*CHO二聚化过程,这是提高C2+产物选择性的关键。本研究强调,CeO2通过调节cu基催化剂对C2+产物的吸附特性,促进CO2RR中的C-C偶联。
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