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Context <p>Metal-based complex hydrogen storage materials demonstrate high hydrogen storage density and reversibility, attracting significant attention. This study focuses on analyzing the reaction mechanism of As-doped (LiNH<sub>2</sub>)<sub>2</sub> clusters with LiH and NaH. The results indicate that As doping decreases the stability of (LiNH<sub>2</sub>)<sub>2</sub>, causing minimal changes in the lowest unoccupied molecular orbital while significantly shifting the electron cloud distribution of the highest occupied molecular orbital towards As, concentrating electron deficiency around As. The dehydrogenation process favors the –AsH<sub>2</sub> group, while the –NH<sub>2</sub> group facilitates hydrogen storage. A new hydrogen storage and release mechanism involving hydrogen transfer between –NH<sub>2</sub> and –AsH<sub>2</sub> is proposed, which lowers the energy barrier for hydrogen release and improves the reversibility of hydrogen storage.</p> Methods <p>Density functional theory (DFT) was employed to analyze the reaction mechanism. Key stationary points along the reaction path underwent geometric optimization, and their correctness was verified through frequency analysis.</p>

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Exploring the reaction mechanism of As-doped (LiNH2)2 clusters with LiH/NaH: insights into a new hydrogen transfer mechanism

  • 期刊论文

  • 发表日期：

    2026年1月27日

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  • Xiao Dong,
  • Rong Yuan,
  • Shishuai Liu,
  • Aochen Du,
  • Genzhuang Li

摘要

Context

Metal-based complex hydrogen storage materials demonstrate high hydrogen storage density and reversibility, attracting significant attention. This study focuses on analyzing the reaction mechanism of As-doped (LiNH2)2 clusters with LiH and NaH. The results indicate that As doping decreases the stability of (LiNH2)2, causing minimal changes in the lowest unoccupied molecular orbital while significantly shifting the electron cloud distribution of the highest occupied molecular orbital towards As, concentrating electron deficiency around As. The dehydrogenation process favors the –AsH2 group, while the –NH2 group facilitates hydrogen storage. A new hydrogen storage and release mechanism involving hydrogen transfer between –NH2 and –AsH2 is proposed, which lowers the energy barrier for hydrogen release and improves the reversibility of hydrogen storage.

Methods

Density functional theory (DFT) was employed to analyze the reaction mechanism. Key stationary points along the reaction path underwent geometric optimization, and their correctness was verified through frequency analysis.