Ma Bing, Chen Gui, Fave Claire, Chen Lingjing, Kuriki Ryo, Maeda Kazuhiko, Ishitani Osamu, Lau Tai-Chu, Bonin Julien, Robert Marc
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.
J Am Chem Soc. 2020 Apr 1;142(13):6188-6195. doi: 10.1021/jacs.9b13930. Epub 2020 Mar 18.
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-CN) 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 CO catalytic light-driven reduction.
要在仅使用储量丰富的元素的情况下，实现具有高选择性控制和耐久性的可见光驱动二氧化碳还原，需要新的策略。通过酰胺键将钴-四吡啶分子络合物共价接枝到半导体介孔石墨氮化碳（mpg-CN）上，制备了混合催化材料。该分子材料通过各种光谱技术进行了表征，包括XPS、红外光谱和阻抗谱。在使用太阳模拟器的情况下，它被证明是乙腈中CO生成的选择性催化剂，选择性高达98%，而且非常稳定，因为在照射4天（约500个催化循环）后未观察到降解。这种选择性分子催化剂与简单且稳定的半导体材料的独特组合，为CO的光驱动催化还原开辟了新途径。
