铈
法拉第效率
催化作用
密度泛函理论
选择性
化学工程
可再生能源
材料科学
化学
无机化学
电化学
物理化学
计算化学
电极
有机化学
工程类
电气工程
作者
Xupeng Yan,Chunjun Chen,Yahui Wu,Shoujie Liu,Yizhen Chen,Rongjuan Feng,Jing Zhang,Buxing Han
出处
期刊:Chemical Science
[The Royal Society of Chemistry]
日期:2021-01-01
卷期号:12 (19): 6638-6645
被引量:99
摘要
Electrocatalytic reduction of CO2 into multicarbon (C2+) products powered by renewable electricity offers one promising method for CO2 utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C2+ products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO2/CuO) and showed an outstanding catalytic performance for C2+ products. The faradaic efficiency of the C2+ products could reach 75.2% with a current density of 1.21 A cm-2. In situ experiments and density functional theory (DFT) calculations demonstrated that the interface between CeO2 and Cu and the subsurface Cu2O coexisted in CeO2/CuO during CO2RR and two competing pathways for C-C coupling were promoted separately, of which hydrogenation of *CO to *CHO is energetically favoured. In addition, the introduction of CeO2 also enhanced water activation, which could accelerate the formation rate of *CHO. Thus, the selectivity and activity for C2+ products over CeO2/CuO can be improved simultaneously.
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