Yi Jun-Dong, Si Duan-Hui, Xie Ruikuan, Yin Qi, Zhang Meng-Di, Wu Qiao, Chai Guo-Liang, Huang Yuan-Biao, Cao Rong
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China.
University of Chinese Academy of Science, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2021 Jul 26;60(31):17108-17114. doi: 10.1002/anie.202104564. Epub 2021 Jun 24.
The electrocatalytic conversion of CO into value-added chemicals is a promising approach to realize a carbon-energy balance. However, low current density still limits the application of the CO electroreduction reaction (CO RR). Metal-organic frameworks (MOFs) are one class of promising alternatives for the CO RR due to their periodically arranged isolated metal active sites. However, the poor conductivity of traditional MOFs usually results in a low current density in CO RR. We have prepared conductive two-dimensional (2D) phthalocyanine-based MOF (NiPc-NiO ) nanosheets linked by nickel-catecholate, which can be employed as highly efficient electrocatalysts for the CO RR to CO. The obtained NiPc-NiO has a good conductivity and exhibited a very high selectivity of 98.4 % toward CO production and a large CO partial current density of 34.5 mA cm , outperforming the reported MOF catalysts. This work highlights the potential of conductive crystalline frameworks in electrocatalysis.
将CO电催化转化为高附加值化学品是实现碳-能源平衡的一种很有前景的方法。然而，低电流密度仍然限制了CO电还原反应（CO RR）的应用。金属有机框架（MOF）由于其周期性排列的孤立金属活性位点，是CO RR一类很有前景的替代物。然而，传统MOF的导电性差通常导致CO RR中的电流密度较低。我们制备了由镍-儿茶酚连接的导电二维（2D）酞菁基MOF（NiPc-NiO）纳米片，其可作为将CO RR电催化为CO的高效电催化剂。所获得的NiPc-NiO具有良好的导电性，对CO生成表现出98.4%的极高选择性和34.5 mA cm的大CO分电流密度，优于已报道的MOF催化剂。这项工作突出了导电晶体框架在电催化中的潜力。
