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, Zhen Zhou
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 PhenPtCl 2 nanosheets, revealing a N 2 -Pt-Cl 2 coordination structure through various characterization techniques. Remarkably, the electrocatalytic performance of these PhenPtCl 2 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 N 2 -Pt-Cl 2 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-Cl 2 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 H 2 evolution. This research illuminates the intricate dynamic coordination evolution and structural adaptability of PhenPtCl 2 nanosheets, firmly establishing them as a promising candidate for efficient and tunable electrocatalysts.