Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-11-28 , DOI: 10.1016/j.jcat.2022.11.035 Jiaxin Li, Tong Shi, Fuli Tian, Shangpeng Liu, Qiyuan Fan, Yanxin Wu, Min Sun, Heng Zhang, Yanqiu Lei, Fenrong Liu, Shanghong Zeng
CO2 electroreduction is a prospective avenue to produce carbon-based fuels, yet atomic-level insights on the mechanistic origin of catalytic selectivity remains elusive. Taking the Ag and Cu2O@Ag electrocatalysts as examples, Fourier-transform infrared spectroscopy in conjunction with theoretical calculations reveal that the hollow-nanostructured Ag promotes CO production through a lower energy barrier of the rate-limiting *CO2 to *COOH, while the Cu2O-Ag boundaries in the honeycomb-like Cu2O@Ag reinforce CO2 physisorption and chemisorption on the catalyst surface. The interfaces of Cu2O@Ag facilitate CO hydrogenation and CC coupling, opening alternative reaction pathways toward CH4 and C2H4. More broadly, this study provides insights to develop effective electrocatalysts in CO2 electroreduction and beyond.
中文翻译:
阐明 CO2 电还原中的反应途径:Ag 和 Cu2O@Ag 催化剂的案例研究
CO 2电还原是生产碳基燃料的潜在途径,但对催化选择性的机制起源的原子级见解仍然难以捉摸。以 Ag 和 Cu 2 O@Ag 电催化剂为例,傅里叶变换红外光谱结合理论计算表明,空心纳米结构 Ag 通过较低的限速 *CO 2到 *COOH 的能垒促进 CO 的产生,而蜂窝状Cu 2 O@Ag中的Cu 2 O-Ag边界加强了CO 2在催化剂表面的物理吸附和化学吸附。Cu 2 O@Ag的界面促进 CO 加氢和 CC 偶联,打开对 CH 4和 C 2 H 4的替代反应途径。更广泛地说,这项研究为开发 CO 2电还原及其他领域的有效电催化剂提供了见解。