Coordination Chemistry Institute, State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210023, China.
Small. 2023 Mar;19(10):e2206070. doi: 10.1002/smll.202206070. Epub 2022 Dec 20.
Tandem catalysis is a promising way to break the limitation of linear scaling relationship for enhancing efficiency, and the desired tandem catalysts for electrochemical CO reduction reaction (CO RR) are urgent to be developed. Here, a tandem electrocatalyst created by combining Cu foil (CF) with a single-site Cu(II) metal-organic framework (MOF), named as Cu-MOF-CF, to realize improved electrochemical CO RR performance, is reported. The Cu-MOF-CF shows suppression of CH , great increase in C H selectivity (48.6%), and partial current density of C H at -1.11 V versus reversible hydrogen electrode. The outstanding performance of Cu-MOF-CF for CO RR results from the improved microenvironment of the Cu active sites that inhibits CH production, more CO intermediate produced by single-site Cu-MOF in situ for CF, and the enlarged active surface area by porous Cu-MOF. This work provides a strategy to combine MOFs with copper-based electrocatalysts to establish high-efficiency electrocatalytic CO RR.
串联催化是一种很有前途的方法,可以打破提高效率的线性比例关系的限制,对于电化学 CO 还原反应(CO RR),急需开发所需的串联催化剂。在此,报道了一种通过将铜箔(CF)与单原子 Cu(II) 金属有机骨架(MOF)相结合,构建串联电催化剂 Cu-MOF-CF,以实现电化学 CO RR 性能的改善。Cu-MOF-CF 表现出抑制 CH 的生成,大幅提高 C H 的选择性(48.6%),并在相对于可逆氢电极的-1.11 V 下获得 C H 的部分电流密度。Cu-MOF-CF 对 CO RR 的优异性能归因于 Cu 活性位的微环境得到改善,抑制了 CH 的生成,原位的单原子 Cu-MOF 产生更多的 CO 中间产物,多孔的 Cu-MOF 增加了活性表面积。这项工作为结合 MOFs 和铜基电催化剂以建立高效电催化 CO RR 提供了一种策略。