Heteroatom coordination induces electric field polarization of single Pt sites to promote hydrogen evolution activity

Xianyun Peng; Haihong Bao; Jiaqiang Sun; Zhiyong Mao; Yuan Qiu; Zhaojun Mo; Longchao Zhuo; Shusheng Zhang; Jun Luo; Xijun Liu

doi:10.1039/D1NR00795E

Heteroatom coordination induces electric field polarization of single Pt sites to promote hydrogen evolution activity†

Xianyun Peng,‡^a Haihong Bao,‡^a Jiaqiang Sun,

^b Zhiyong Mao,

*^c Yuan Qiu,^a Zhaojun Mo,*^d Longchao Zhuo,^e Shusheng Zhang,

^f Jun Luo

^a and Xijun Liu

*^ag

Author affiliations

* Corresponding authors

^a Institute for New Energy Materials and Low-Carbon Technologies and Tianjin Key Lab for Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
E-mail: xjliu@tjut.edu.cn

^b State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China

^c School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
E-mail: mzhy1984@163.com

^d Ganjiang Innovation Academy, Chinese Academy of Sciences, Jiangxi 341000, China
E-mail: mozhaojun@gia.cas.cn

^e School of Materials Science and Engineering, Xi'an University of Technology, Xi'an 710048, China

^f College of Chemistry, Zhengzhou University, Zhengzhou 450000, China

^g Key Laboratory of Civil Aviation Thermal Hazards Prevention and Emergency Response, Civil Aviation University of China, Tianjin 300300, China

Abstract

Herein, we reported a kind of single Pt site (Pt-SA) stabilized on an MXene support (Pt-SA/MXene) via the formation of Pt–O and Pt–Ti bonds to effectively catalyze the hydrogen evolution reaction (HER). Due to the local electric field polarization derived from its unique asymmetric coordination, Pt-SA/MXene displays remarkably higher catalytic HER activity in an alkaline electrolyte. In detail, the Pt-SA/MXene electrocatalyst only needs a low overpotential of 33 mV to reach a current density of 10 mA cm⁻² and maintains the performance over 27 h. Besides, Pt-SA/MXene also has a competitive mass activity, 23.5 A mg_Pt⁻¹, at an overpotential of 100 mV, which is 29.4 times greater than that of the commercial Pt/C counterpart. Density functional theory (DFT) calculations revealed that the polarized electric field could efficiently tailor the electronic structure of Pt-SA/MXene and reduce the energy barrier of adsorption/desorption of the H* intermediate step, further improving its HER catalytic activity.

Nanoscale

Heteroatom coordination induces electric field polarization of single Pt sites to promote hydrogen evolution activity†

Abstract

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