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Cu-O-Ce桥增强活性氢吸收和稳定Cu(I)物种,促进电催化CO2还原为乙烯
作者:小柯机器人 发布时间:2025/7/1 17:51:42

天津大学张志成团队近日实现了Cu-O-Ce桥增强活性氢吸收和稳定Cu(I)物种,促进电催化CO2还原为乙烯。2025年6月30日,《德国应用化学》杂志发表了这一成果。

合理设计水活化中心以促进活性氢(*H)的产生并稳定Cu(I)物种,对于电催化CO2还原反应(CO2RR)中铜基催化剂上多碳(C2+)产物的形成具有重要意义。在此,通过种子介导的生长方法,CeO2纳米颗粒和CuO纳米刺被选择性地沉积在Cu2O立方体的边缘。与Cu2O立方体相比,合成的CuxO-CeO2复合材料表现出增强的法拉第效率和C2H4的部分电流密度。 

原位光谱和理论计算证实,CuxO-CeO2复合材料中的Cu-O-Ce桥可以有效增强*H吸收并稳定Cu(I)物种,促进随后的C-C偶联并进一步质子化为C2H4的关键*COCHO中间体。这项工作为调节*H吸收和稳定Cu(I)物种以将CO2转化为C2+产物提供了新的见解。

附:英文原文

Title: Enhanced Active Hydrogen Absorption and Stabilized Cu(I) Species over Cu-O-Ce Bridges Boosting Electrocatalytic CO2 Reduction to Ethylene

Author: Zhenwei Zhao, Yu Zhang, Junjun Li, Bingqing Yao, Hui Zhang, Zhicheng Zhang

Issue&Volume: 2025-06-30

Abstract: Rational design of water activation center to promote active hydrogen (*H) generation and stabilize Cu(I) species are significant for the formation of multicarbon (C2+) products over Cu-based catalysts in electrocatalytic CO2 reduction reaction (CO2RR). Herein, CeO2 nanograins and CuO nanothorns were selectively deposited on the edges of Cu2O cubes through the seed-mediated growth method. The as-synthesized CuxO-CeO2 composites exhibit enhanced Faradaic efficiency and partial current density of C2H4 compared with Cu2O cubes. In situ spectroscopies and theoretical calculations confirm that the Cu-O-Ce bridges in CuxO-CeO2 composite can effectively enhance *H absorption and stabilize Cu(I) species, facilitating subsequent C-C coupling and further protonation into the key *COCHO intermediate of C2H4. This work provides new insights into modulating *H absorption and stabilizing Cu(I) species for boosting CO2 to C2+ products.

DOI: 10.1002/anie.202510383

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202510383

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx