The conjugation of external species with two-dimensional (2D) materials has broad application prospects. In this study, we have explored the potential of noble metal/2D MOF heterostructures in hydrogen storage. Specifically, the MgH₂-Ni-MOF@Pd system has shown remarkable hydrogen desorption/sorption performances, starting to liberate hydrogen at 181 °C, which is 230 °C lower than that of pristine MgH₂. Under the catalytic effect of Ni-MOF@Pd, the dehydrogenation apparent activation energy of MgH₂ is noticeably decreased from (133.5 ± 17.5) to (34.58 ± 1.87) kJ·mol⁻¹, and the hydrogenation apparent activation energy is reduced from (70.41 ± 7.43) to (25.78 ± 4.64) kJ·mol⁻¹, which is lowered by 63.4%. The fully-dehydrogenated MgH₂-Ni-MOF@Pd composite rapidly uptakes hydrogen, with 2.62 wt% at 100 °C and 6.06 wt% at 150 °C within 300 s, respectively. The mechanism analysis of MgH₂ catalyzed by Ni-MOF@Pd has revealed that the transformation of Mg₂Ni and Mg₂NiH₄ could act as a “hydrogen pump”, providing numerous channels for fast diffusion and transport of hydrogen atoms. Moreover, in the dehydrogenation process, the element Pd reacts with MgH₂ to form the Mg-Pd alloy phase, which makes MgH₂ take precedence to decompose through the Mg-Pd alloy rather than self-decomposition, further reducing thermal stability and improving de/hydrogenation kinetics. The synergistic effect of Mg-Pd, Mg₂Ni, and the special ultra-thin 2D sheet structure of the additive is the main reason for the good hydrogen storage property of MgH₂-Ni-MOF@Pd. Our findings provide inspiration for designing efficient multi-functional additives with unique morphologies to optimize the hydrogen desorption/sorption behaviors of hydrogen storage materials.

外部物种与二维（2D）材料的共轭具有广阔的应用前景。在这项研究中，我们探索了贵金属/二维 MOF 异质结构在储氢方面的潜力。具体来说，MgH ₂ -Ni-MOF@Pd系统表现出显着的氢解吸/吸附性能，在181℃时开始释放氢气，比原始MgH ₂低230℃ 。在Ni-MOF@Pd的催化作用下，MgH ₂的脱氢表观活化能由(133.5±17.5)显着降低至(34.58±1.87) kJ·mol ^-1，加氢表观活化能由( 70.41±7.43）至（25.78±4.64）kJ·mol ^-1，降低了63.4%。完全脱氢的MgH ₂ -Ni-MOF@Pd复合材料快速吸收氢气，在300秒内分别在100°C和150°C下分别吸收2.62 wt%和6.06 wt%。_{Ni-MOF@Pd催化MgH 2}的机理分析表明，Mg ₂ Ni和Mg ₂ NiH ₄的转化可以充当“氢泵”，为氢原子的快速扩散和传输提供众多通道。而且，在脱氢过程中，元素Pd与MgH ₂反应形成Mg-Pd合金相，使得MgH ₂优先通过Mg-Pd合金分解而不是自分解，进一步降低了热稳定性，提高了脱氢性能。 /氢化动力学。_{Mg-Pd、Mg 2} Ni的协同作用以及添加剂特殊的超薄二维片状结构是MgH ₂ -Ni-MOF@Pd具有良好储氢性能的主要原因。我们的研究结果为设计具有独特形态的高效多功能添加剂提供了灵感，以优化储氢材料的氢解吸/吸附行为。