journal article·2022-09-27Open access

Efficient Water Dissociation on Confined Ultrafine Pt via Pyridinic N-Enhanced Heavy d−π Interaction

Yuan Dong, Jiang-Bo Chen, Jie Ying, Yu-Xuan Xiao, Ge Tian, Mark D. Symes, Xiao-Yu Yang

Chemistry of Materials· Volume 34· Issue 18
Publisher page

Abstract

Sluggish water dissociation on Pt electrocatalysts results in poor performance for the alkaline hydrogen evolution reaction (HER) and thus greatly limits their practical application in industrial water electrolysis. Herein, ultrafine Pt nanoparticles have been confined into N-doped carbon by an in situ galvanic replacement reaction, and the pyridinic N-enhanced heavy d−π interaction is found to significantly enhance the water dissociation catalytic activity of Pt. The electron-deficient Pt generated by this enhanced heavy d−π effect exhibits an ultralow overpotential for hydrogen evolution of 10 mV at a current density of 10 mA cm–2 and an ultrahigh mass current density of 7.74 mA μgPt–1 at an overpotential of 70 mV (7.9-fold higher than that of commercial Pt/C). Theoretical calculations reveal that the pyridinic N-enhanced heavy d−π effect can largely reduce the water dissociation energy barrier on Pt, thus greatly enhancing Pt’s performance for the alkaline HER.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Ammonia Synthesis and Nitrogen Reduction · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering & NRC (Nanostructure Research Centre) & Shenzhen Research Institute & Joint Laboratory for Marine Advanced Materials in Pilot National Laboratory for Marine Science and Technology (Qingdao), Wuhan University of Technology, Wuhan 430070, China

School of Chemical Engineering and Technology, Sun Yat-sen University, Zhuhai 519082, China

WestCHEM, School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, U.K.

Funding

Royal Society · Science, Technology and Innovation Commission of Shenzhen Municipality · National Natural Science Foundation of China · Higher Education Discipline Innovation Project · Guangzhou Science and Technology Project · Guangdong Province International Scientific and Technological Cooperation Projects · Guangdong Basic and Applied Basic Research Foundation · Sino-German Centre's COVID-19 Related Bilateral Collaborative project · FRFCU · Program for Changjiang Scholars and Innovative Research Team in University

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