Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2023 May 22;62(22):e202301507. doi: 10.1002/anie.202301507. Epub 2023 Apr 25.
Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g-C N ) supported Cu nanoparticles (Cu-CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C N interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate -*CHO is advantage around the Cu/C N interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu-CN catalyst in the industrial application.
一氧化碳的电化学还原反应（CORR）提供了一种很有前途的方法，可以在温和的条件下直接从气态 CO 和水中制造乙酸。在此，我们发现具有适当尺寸的石墨相氮化碳（g-C3N）负载的铜纳米粒子（Cu-CN）具有高的乙酸法拉第效率 62.8%，在 CORR 中的部分电流密度为 188 mA·cm-2。原位实验和密度泛函理论计算研究表明，Cu/C3N 界面和金属 Cu 表面协同促进 CORR 生成乙酸。关键中间体 *CHO 的生成在 Cu/C3N 界面处具有优势，并且迁移的 *CHO 有利于在具有促进的 *CHO 覆盖率的金属 Cu 表面上生成乙酸。此外，在多孔固体电解质反应器中实现了乙酸水溶液的连续生产，这表明 Cu-CN 催化剂在工业应用中具有巨大的潜力。
