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Nat Commun. 2019 Apr 10;10(1):1657. doi: 10.1038/s41467-019-09596-x.

The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring.

Author information

1
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, 210023, Nanjing, China.
2
National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, China.
3
Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210, Shanghai, China.
4
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 110016, Shenyang, China.
5
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, 210023, Nanjing, China. wqchem@nju.edu.cn.
6
National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, 210093, Nanjing, China. wangpeng@nju.edu.cn.
7
Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, 210023, Nanjing, China. wangpeng@nju.edu.cn.
8
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, 210023, Nanjing, China. zhenghu@nju.edu.cn.

Abstract

Single-site catalysts feature high catalytic activity but their facile construction and durable utilization are highly challenging. Herein, we report a simple impregnation-adsorption method to construct platinum single-site catalysts by synergic micropore trapping and nitrogen anchoring on hierarchical nitrogen-doped carbon nanocages. The optimal catalyst exhibits a record-high electrocatalytic hydrogen evolution performance with low overpotential, high mass activity and long stability, much superior to the platinum-based catalysts to date. Theoretical simulations and experiments reveal that the micropores with edge-nitrogen-dopants favor the formation of isolated platinum atoms by the micropore trapping and nitrogen anchoring of [PtCl6]2-, followed by the spontaneous dechlorination. The platinum-nitrogen bonds are more stable than the platinum-carbon ones in the presence of adsorbed hydrogen atoms, leading to the superior hydrogen evolution stability of platinum single-atoms on nitrogen-doped carbon. This method has been successfully applied to construct the single-site catalysts of other precious metals such as palladium, gold and iridium.

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