Publication 901

J. Am. Chem. Soc., 142 (13), 6188-6195, 2020 DOI:10.1021/jacs.9b13930b
Efficient Visible-Light Driven CO2 Reduction by a Cobalt Molecular Catalyst Covalently Linked to Mesoporous Carbon Nitride

Laboratoire d’Electrochimie Moléculaire, CNRS, Université de Paris, 15 Rue Jean-Antoine de Baïf, F-75013 Paris, France
School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, Guangdong, P. R. China
Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-1 Okayama, Meguro-ku, Tokyo 152-8550, Japan
Department of Chemistry, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong, P. R. China

Abstract
Achieving visible-light-driven carbon dioxide reduction with high selectivity control and durability while using only earth abundant elements requires new strategies. Hybrid catalytic material was prepared upon covalent grafting a Co–quaterpyridine molecular complex to semiconductive mesoporous graphitic carbon nitride (mpg-C3N4) through an amide linkage. The molecular material was characterized by various spectroscopic techniques, including XPS, IR, and impedance spectroscopy. It proved to be a selective catalyst for CO production in acetonitrile using a solar simulator with a high 98% selectivity, while being remarkably robust since no degradation was observed after 4 days of irradiation (ca. 500 catalytic cycles). This unique combination of a selective molecular catalyst with a simple and robust semiconductive material opens new pathways for CO2 catalytic light-driven reduction..