Selective CO 2 Electromethanation on Surface-Modified Cu Catalyst by Local Microenvironment Modulation

作者：Yaoxuan Shi, Kun Sun, Jingjing Shan, Huiyi Li, Jianmin Gao, Zhaoyu Chen, Chengyue Sun, Yong Shuai, Zhijiang Wang · 发表于：ACS Catalysis · 年份：2022 · DOI：10.1021/acscatal.2c01544 · 被引用次数：76 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Ammonia Synthesis and Nitrogen Reduction

Renewable methane synthesized via CO 2 electroreduction has the potential to serve as a carbon-neutral medium benefiting from its high energy density. However, challenges remain in achieving high selectivity for electromethanation with low energy input. Here, we found that the adhered ligands on the copper surface can modulate the local microenvironment to realize high rates for methane electrogeneration. The designed glutathione-modified copper electrode exhibited an impressive CO 2 to CH 4 Faradaic efficiency of 61.7% with a partial current density of 153.7 mA cm –2, which was 35-fold higher than that of pristine copper. Operando Raman spectroscopy experiments suggest that the carboxyl and amino groups of glutathione ligands play a crucial role in regulating intermediate configurations and local proton availability. More broadly, these findings offer routes to alter surface reactivity and create a platform for designing highly selective CO 2 electroreduction catalysts.