Efficient Visible-Light-Driven CO2 Reduction by a Cobalt Molecular Catalyst Covalently Linked to Mesoporous Carbon Nitride
Efficient Visible-Light-Driven CO2 Reduction by a Cobalt Molecular Catalyst Covalently Linked to Mesoporous Carbon Nitride
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DOI：
10.1021/jacs.9b13930
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发表时间：
2020-04-01
影响因子：
15
通讯作者：
Robert, Marc
中科院分区：
文献类型：
--
作者：
Ma, Bing;Chen, Gui;Robert, Marc
实现具有高选择性控制和耐久性的可见光驱动的二氧化碳减少，同时仅使用地球丰富的元素，需要新的策略。通过酰胺键将Co-quaterpyridine分子复合物共价接枝到介孔石墨碳氮化物（mpg-C3 N4）上，制备了杂化催化材料。通过XPS、IR和阻抗谱等多种光谱技术对分子材料进行了表征。使用太阳能模拟器，证明它是用于在乙腈中产生CO的选择性催化剂，具有98%的高选择性，同时由于在照射4天后没有观察到降解而非常耐用（约100%）。500个催化循环）。这种选择性分子催化剂与简单而坚固的可降解材料的独特组合为CO2催化光驱动还原开辟了新的途径。
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.