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

Zhiqi Zhang, Yugang Chen, Liqi Zhou, Chi Chen, Zhen Han, Bingsen Zhang, Qiang Wu (), Lijun Yang, Lingyu Du, Yongfeng Bu, Peng Wang (), Xizhang Wang, Hui Yang and Zheng Hu ()
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Zhiqi Zhang: Nanjing University
Yugang Chen: Nanjing University
Liqi Zhou: Nanjing University
Chi Chen: Chinese Academy of Sciences
Zhen Han: Nanjing University
Bingsen Zhang: Institute of Metal Research, Chinese Academy of Sciences
Qiang Wu: Nanjing University
Lijun Yang: Nanjing University
Lingyu Du: Nanjing University
Yongfeng Bu: Nanjing University
Peng Wang: Nanjing University
Xizhang Wang: Nanjing University
Hui Yang: Chinese Academy of Sciences
Zheng Hu: Nanjing University

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-09596-x

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