Dynamic coordination engineering of 2D PhenPtCl2 nanosheets for superior hydrogen evolution

Gonglei Shao (), Changfei Jing, Zhinan Ma, Yuanyuan Li, Weiqi Dang, Dong Guo, Manman Wu, Song Liu, Xu Zhang, Kun He, Yifei Yuan, Jun Luo, Sheng Dai (), Jie Xu () and Zhen Zhou ()
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Gonglei Shao: Zhengzhou University
Changfei Jing: Wenzhou University
Zhinan Ma: North University of China
Yuanyuan Li: Henan University of Technology
Weiqi Dang: Nanjing University
Dong Guo: Zhengzhou University
Manman Wu: Zhengzhou University
Song Liu: Hunan University
Xu Zhang: Zhengzhou University
Kun He: Wenzhou University
Yifei Yuan: Wenzhou University
Jun Luo: University of Electronic Science and Technology of China
Sheng Dai: East China University of Science and Technology
Jie Xu: Wenzhou University
Zhen Zhou: Zhengzhou University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Exploring the dynamic structural evolution of electrocatalysts during reactions represents a fundamental objective in the realm of electrocatalytic mechanism research. In pursuit of this objective, we synthesized PhenPtCl2 nanosheets, revealing a N2-Pt-Cl2 coordination structure through various characterization techniques. Remarkably, the electrocatalytic performance of these PhenPtCl2 nanosheets for hydrogen evolution reaction (HER) surpasses that of the commercial Pt/C catalyst across the entire pH range. Furthermore, our discovery of the dynamic coordination changes occurring in the N2-Pt-Cl2 active sites during the electrocatalytic process, as clarified through in situ Raman and X-ray photoelectron spectroscopy, is particularly noteworthy. These changes transition from Phen-Pt-Cl2 to Phen-Pt-Cl and ultimately to Phen-Pt. The Phen-Pt intermediate plays a pivotal role in the electrocatalytic HER, dynamically coordinating with Cl- ions in the electrolyte. Additionally, the unsaturated, two-coordinated Pt within Phen-Pt provides additional space and electrons to enhance both H+ adsorption and H2 evolution. This research illuminates the intricate dynamic coordination evolution and structural adaptability of PhenPtCl2 nanosheets, firmly establishing them as a promising candidate for efficient and tunable electrocatalysts.

Date: 2024
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DOI: 10.1038/s41467-024-44717-1

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