Catalytic methanolysis of ammonia borane represents a promising technology for in situ hydrogen production. However, the widespread application of this technology is constrained by the prohibitive cost associated with noble metal catalysts. Consequently, the development of cost-effective and robust is essential for commercial scaling of this technology. In this study, a series of NiO-CuO/Fe₃O₄ catalyst with three-phase interfaces for ammonia borane methanolysis were fabricated by supporting NiO-CuO with Fe₃O₄. It was demonstrated that the Fe₃O₄ support in the catalyst could not only modulate the electronic structure of catalyst but also and confer magnetic characteristics upon it. The catalyst bearing a Ni/Cu molar ratio of 2:2 achieved a turnover frequency (TOF) of 13.5 min^-1 in ammonia borane methanolysis, along with long-term stability. Furthermore, magnetic characterization confirmed the catalyst’s ferromagnetic properties with a coercivity of 51.8 Oe, facilitating the magnetic separation of the catalyst under an external magnetic field. Through various exhaustive characterizations, it was revealed that abundant interfacial positively charged Ni sites and negatively charged Cu sites in NiO-CuO/Fe₃O₄ catalyst could activate methanol and ammonia borane, respectively, thus promoting the hydrogen production efficiently. Considering the excellent activity and recyclability of NiO-CuO/Fe₃O₄, it is anticipated to gain widespread applications in the industrial production of hydrogen from ammonia borane methanolysis.

中文翻译：

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三相 NiO-CuO/Fe3O4 异质结构催化剂在氨硼烷甲烷分解中快速放氢的界面工程


氨硼烷的催化甲烷分解代表了一种很有前途的原位制氢技术。然而，这项技术的广泛应用受到与贵金属催化剂相关的高昂成本的限制。因此，开发具有成本效益和稳健性的产品对于该技术的商业规模化至关重要。在本研究中，通过用 Fe₃O₄ 支撑 NiO-CuO 制备了一系列具有三相界面的 NiO-CuO/Fe₃O₄ 催化剂，用于氨硼烷甲烷分解。结果表明，催化剂中的 Fe₃O₄ 载体不仅可以调节催化剂的电子结构，还可以赋予催化剂磁性。Ni/Cu 摩尔比为 2：2 的催化剂在氨硼烷甲烷分解中实现了 13.5min-1 的周转频率 （TOF），并具有长期稳定性。此外，磁性表征证实了催化剂的铁磁特性，矫顽力为 51.8Oe，有利于催化剂在外部磁场下的磁分离。通过各种详尽的表征，揭示了 NiO-CuO/Fe₃O₄ 催化剂中丰富的界面带正电荷的 Ni 位点和带负电荷的 Cu 位点可以分别活化甲醇和氨硼烷，从而有效地促进氢气的产生。考虑到 NiO-CuO/Fe₃O₄ 的优异活性和可回收性，有望在氨硼烷甲烷分解氢气的工业生产中获得广泛应用。