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High-loading single cobalt atoms on ultrathin MOF nanosheets for efficient photocatalytic CO_(2) reduction

查看全文 作　　者：Quan [1,2]Zuo;Rui [2]Cui;Lei [2]Wang;Yuling [2]Wang;Chunyang [2]Yu;Liang [2]Wu;Yiyong [2]Mai;Yongfeng [1]Zhou 高影响力作者 机构地区：[1]School of Packaging and Materials Engineering,Hunan University of Technology,Zhuzhou,412007,China;[2]School of Chemistry and Chemical Engineering,Frontiers Science Center for Transformative Molecules,State Key Laboratory of Metal Matrix Composites,Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing,Shanghai Jiao Tong University,Shanghai,200240,China高影响力机构 出　　处：《Science China Chemistry》索引2023年第66卷第2期,共8页高影响力期刊 基　　金：supported by the National Natural Science Foundation of China(52073173,21890730,21890733,and22231007);Hunan Provincial Natural Science Foundation of China(2022JJ40120);the Scientific Research Project of Education Department of Hunan Province(22B0602);the Program for Basic Research of Shanghai Science and Technology Commission(19JC1410400,and 19JC1410404);the Program of Shanghai Academic Research Leader(19XD1421700)。 摘　　要：Based on suitable scaffolds,constructing high-loading single-atom catalysts is a promising strategy to achieve highly efficient catalysis.Herein,using ultrathin metal-organic framework(MOF)nanosheets(2.4±0.5 nm)as the support,single-atom catalysts with high cobalt loading(6.0 wt%)were constructed(denoted as Co-MNSs)by a simple bottom-up synthetic strategy.The catalytic system of Co-MNSs exhibited an outstanding photocatalytic CO_(2)-to-CO evolution rate of 7,041μmol g^(-1)h^(-1)and a selectivity of 86%in aqueous media under visible-light irradiation,which has reached the top level of the reported MOF-based photocatalysts.The control experiments and theoretical calculation revealed that the Co-N_(4)moiety in the MOF nanosheets acted as the active site for the photocatalytic CO_(2)-to-CO conversion.The boosted photocatalytic performance could be ascribed to the high aspect-ratio of layered Co-MNSs providing abundant accessible active sites on their surfaces,which reduced the energy barrier,improved the charge separation efficiency,and also facilitated the adsorption of CO_(2)to form the reactive radicals of*COOH.Our study provides an appealing strategy for constructing high-loading single-atom catalysts and demonstrates the significance of 2D ultrathin MOF nanosheets as the support in boosting CO_(2)photoreduction efficiency. 关 键 词：two-dimensional material single-atom catalyst metal-organic framework photocatalysis CO_(2)reduction
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