Though ammonia borane (AB) is considered as one of the potential hydrogen storage materials, the effective and economical utilization of AB hydrolysis for efficient hydrogen release encounters hindrances primarily due to the unavailability of an appropriate catalyst. Herein, we present a solvothermal route for synthesizing a series of MOFs and demonstrate superior hydrogen (H₂) production via AB hydrolysis using the optimized Cu-MOF-74 catalyst with an activation energy of 32.1 kJmol^–1 and a turnover frequency (TOF) of 26 min^–1. The influence of ions, AB, and catalyst concentration variation on the rate of AB hydrolysis reaction was investigated. The kinetic isotopic experiment unveils the pivotal step in ammonia borane hydrolysis as the breaking of the O–H bond. Isotope-labeling mass spectrometry techniques were employed to determine the origin of hydrogen and elucidate the underlying reaction mechanism. Interestingly, significant uptake of ammonia by Cu-MOF-74 during hydrolysis of AB can be promising in safeguarding fuel cells. Based on our findings, Cu-MOF-74 catalyst emerges as a dual performer enabling simultaneous hydrogen generation from AB and ammonia capture.

中文翻译：

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利用金属有机框架通过 O-H 键活化通过氨硼烷水解催化产氢


尽管氨硼烷（AB）被认为是潜在的储氢材料之一，但有效且经济地利用AB水解来高效释放氢遇到了障碍，这主要是由于缺乏合适的催化剂。在此，我们提出了一种合成一系列 MOF 的溶剂热路线，并展示了使用优化的 Cu-MOF-74 催化剂通过 AB 水解产生优异的氢气 (H ₂ )，其活化能为 32.1 kJmol ^–1 和 26 分钟的周转频率 (TOF) ^–1 。研究了离子、AB 和催化剂浓度变化对AB 水解反应速率的影响。动力学同位素实验揭示了氨硼烷水解的关键步骤是 O-H 键的断裂。采用同位素标记质谱技术来确定氢的来源并阐明潜在的反应机制。有趣的是，AB 水解过程中 Cu-MOF-74 大量吸收氨可能有利于保护燃料电池。根据我们的研究结果，Cu-MOF-74 催化剂具有双重性能，能够同时从 AB 产生氢气和捕获氨。