Jiang Han, Ding Zhao, Li Yuting, Lin Guo, Li Shaoyuan, Du Wenjia, Chen Yu'an, Shaw Leon L, Pan Fusheng
College of Materials Science and Engineering, National Engineering Research Center for Magnesium Alloys, National Innovation Centre for Industry-Education Integration of Energy Storage Technology, Chongqing University Chongqing China
Chongqing Institute of New Energy Storage Materials and Equipment Chongqing China.
Chem Sci. 2025 Apr 1;16(18):7610-7636. doi: 10.1039/d5sc01169h. eCollection 2025 May 7.
Interface engineering fundamentally revolutionizes magnesium-based hydrogen storage systems by orchestrating atomic-scale interactions and mass transport pathways through precisely engineered structural architectures and chemical environments. This review presents a paradigm-shifting framework that transcends conventional surface modification approaches, establishing interface engineering as a cornerstone strategy for next-generation hydrogen storage materials. Through sophisticated control of interface architecture - from one-dimensional confined channels that facilitate directional hydrogen diffusion, to two-dimensional platforms that maximize catalytic interactions, to three-dimensional networks that optimize spatial organization - we unlock unprecedented control over hydrogen storage dynamics. The strategic modulation of interface chemistry creates synergistic effects between structural features and catalytic functionalities. Metal-metal interfaces orchestrate electron transfer processes and facilitate hydrogen dissociation, while engineered support interfaces maintain structural integrity and enhance cycle life. This multi-level interface control enables simultaneous optimization of thermodynamic destabilization and kinetic enhancement. Advanced characterization and theoretical modeling reveal that the controlled evolution of interface structure during hydrogen cycling plays a pivotal role in determining long-term performance stability. Our comprehensive analysis establishes fundamental correlations between interface architecture and hydrogen storage mechanisms, providing critical insights for rational material design. The review concludes by identifying key challenges and opportunities in translating these interface engineering principles into practical energy storage technologies, offering a roadmap for future development of high-performance magnesium-based hydrogen storage systems.
界面工程通过精心设计的结构架构和化学环境来调控原子尺度的相互作用和质量传输路径，从根本上革新了镁基储氢系统。本综述提出了一个范式转变框架，超越了传统的表面改性方法，将界面工程确立为下一代储氢材料的基石策略。通过对界面架构的精确控制——从促进氢定向扩散的一维受限通道，到最大化催化相互作用的二维平台，再到优化空间组织的三维网络——我们实现了对储氢动力学前所未有的控制。界面化学的策略性调控在结构特征和催化功能之间产生了协同效应。金属-金属界面协调电子转移过程并促进氢解离，而设计的载体界面保持结构完整性并延长循环寿命。这种多层次的界面控制能够同时优化热力学失稳和动力学增强。先进的表征和理论建模表明，氢循环过程中界面结构的可控演化在决定长期性能稳定性方面起着关键作用。我们的综合分析建立了界面架构与储氢机制之间的基本关联，为合理的材料设计提供了关键见解。综述最后指出了将这些界面工程原理转化为实际储能技术的关键挑战和机遇，为高性能镁基储氢系统的未来发展提供了路线图。
