Molecular Catalyst with Near 100% Selectivity for CO 2 Reduction in Acidic Electrolytes

作者：Zhan Jiang, Zisheng Zhang, Huan Li, Yirong Tang, Yubo Yuan, Jie Zao, Hongzhi Zheng, Yongye Liang · 发表于：Advanced Energy Materials · 年份：2022 · DOI：10.1002/aenm.202203603 · 被引用次数：136 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Covalent Organic Framework Applications

Abstract The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) in an acidic medium is conducive to the efficient utilization of CO 2 by preventing the formation of carbonate/bicarbonate. However, acidic media are more favorable for the hydrogen evolution reaction (HER), resulting in unsatisfactory CO 2 RR selectivities. It is demonstrated that the molecularly dispersed electrocatalyst of β‐tetra methoxy‐substituted nickel phthalocyanine on carbon nanotubes (NiPc‐OMe MDE) can efficiently catalyze CO 2 RR in acidic media (pH 2 to 0.47) with Faradaic efficiencies of CO >98% over a wide range of current densities from −50 to −400 mA cm −2 . It is found that the superior selectivity performance can be attributed to the presence of potassium ions, the high preference of CO 2 RR over HER on the active site, and few side reaction sites. The study illuminates the potential of molecular electrocatalysts for selective and rapid reduction of CO 2 in acid media.