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Cascade Surface Immobilization Strategy to Access High-density and Closely-distanced Atomic Pt Sites for Enhancing Alkaline Hydrogen Evolution Reaction

Abstract

Increasing the active site density of single-atomic catalysts (SACs) is expected to generate the closely neighboring atomic sites with the potential synergetic interaction. However, the synthesis of SACs with high active site density still remains a great challenge due to the easy aggregation of high density metal atoms during the synthesis. In the present work, we develop a stepwise anchoring strategy for the large-scale preparation of carbon-supported high-density Pt SACs (denoted as PtSA@BP). The Pt loading of PtSA@BP is as high as 2.5 wt%, leading to the observation of abundant closely distanced single Pt sites. The produced PtSA@BP catalyst exhibits ultrahigh catalytic activity for alkaline hydrogen evolution reaction with a low overpotential of 26 mV at 10 mA cm–2 in 1.0 M KOH under ultralow Pt loadings of 0.0009 mgPt cm-2 on the electrode, much superior to commercial Pt/C (20 wt%). Mechanistic studies suggest the main contribution of the coordination of closely distanced three-coordinated PtC2N1 moieties to the excellent catalytic activities towards the conversion of water to H2, due to their close-to-zero metal-hydrogen binding value and intense adsorption capability to H2O molecule as well as low water-dissociation energy barrier. More importantly, this strategy has been verified to be feasible for preparing other noble-metal based SACs, for example, Rh and Pd. The present result provides an enabling and versatile platform for facile accessing SACs with technological importance in various areas.

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Article information


Accepted
10 Feb 2020
First published
10 Feb 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

Cascade Surface Immobilization Strategy to Access High-density and Closely-distanced Atomic Pt Sites for Enhancing Alkaline Hydrogen Evolution Reaction

J. Jiang, W. Liu, J. Ji, X. Yan, W. Liu, Y. Huang, K. Wang, P. Jin and X. Yao, J. Mater. Chem. A, 2020, Accepted Manuscript , DOI: 10.1039/D0TA00495B

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