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Unlocking Dynamic Solvation Chemistry and Hydrogen Evolution Mechanism in Aqueous Zinc Batteries.
Yu, Xiaoyu; Chen, Ming; Li, Zhengang; Tan, Xi; Zhang, Haitang; Wang, Junhao; Tang, Yonglin; Xu, Juping; Yin, Wen; Yang, Yang; Chao, Dongliang; Wang, Fei; Zou, Yeguo; Feng, Guang; Qiao, Yu; Zhou, Haoshen; Sun, Shi-Gang.
Afiliação
  • Yu X; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Chen M; State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST), Wuhan 430074, China.
  • Li Z; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Tan X; State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST), Wuhan 430074, China.
  • Zhang H; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Wang J; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Tang Y; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Xu J; Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China.
  • Yin W; Spallation Neutron Source Science Center, Dongguan 523803, China.
  • Yang Y; Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China.
  • Chao D; Spallation Neutron Source Science Center, Dongguan 523803, China.
  • Wang F; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Zou Y; Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, School of Chemistry and Materials, Fudan University, Shanghai 200433, China.
  • Feng G; Department of Chemistry, Department of Materials Science, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China.
  • Qiao Y; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
  • Zhou H; Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen 361005, PR China.
  • Sun SG; State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST), Wuhan 430074, China.
J Am Chem Soc ; 146(25): 17103-17113, 2024 Jun 26.
Article em En | MEDLINE | ID: mdl-38869216
ABSTRACT
Understanding the interfacial hydrogen evolution reaction (HER) is crucial to regulate the electrochemical behavior in aqueous zinc batteries. However, the mechanism of HER related to solvation chemistry remains elusive, especially the time-dependent dynamic evolution of the hydrogen bond (H-bond) under an electric field. Herein, we combine in situ spectroscopy with molecular dynamics simulation to unravel the dynamic evolution of the interfacial solvation structure. We find two critical change processes involving Zn-electroplating/stripping, including the initial electric double layer establishment to form an H2O-rich interface (abrupt change) and the subsequent dynamic evolution of an H-bond (gradual change). Moreover, the number of H-bonds increases, and their strength weakens in comparison with the bulk electrolyte under bias potential during Zn2+ desolvation, forming a diluted interface, resulting in massive hydrogen production. On the contrary, a concentrated interface (H-bond number decreases and strength enhances) is formed and produces a small amount of hydrogen during Zn2+ solvation. The insights on the above results contribute to deciphering the H-bond evolution with competition/corrosion HER during Zn-electroplating/stripping and clarifying the essence of electrochemical window widened and HER suppression by high concentration. This work presents a new strategy for aqueous electrolyte regulation by benchmarking the abrupt change of the interfacial state under an electric field as a zinc performance-enhancement criterion.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Am Chem Soc Ano de publicação: 2024 Tipo de documento: Article País de afiliação: China

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Am Chem Soc Ano de publicação: 2024 Tipo de documento: Article País de afiliação: China