Zhang Chenghui, Zuo Wei, Ai Lunhong, Tu Sheng, Jiang Jing
College of Materials Science and Engineering, Chongqing Jiaotong University, Chongqing 400074, China.
College of Materials Science and Engineering, Chongqing Jiaotong University, Chongqing 400074, China.
J Colloid Interface Sci. 2024 Sep;669:794-803. doi: 10.1016/j.jcis.2024.05.020. Epub 2024 May 10.
The coordination between carrier and active metal is critical to the catalytic efficiency of ammonia borane (AB) hydrolysis reaction. In the present study, we report a new type of catalytic support based on molybdenum boride (MBene) MoAlB and demonstrate that the effective combination of MoAlB with Ru nanoparticles can realize the significantly enhanced performance for hydrogen generation. Owing to the efficient activation and dissociation of reactants, the optimal Ru/MoAlB catalyst achieves the large turnover frequency of 494 mol mol min, high hydrogen generation rate of 119817 mL min g and favorable apparent activation energy of 39.2 kJ mol for the catalytic hydrolysis of AB under alkaline-free condition. The isotopic test suggests the cleavage of OH bond in HO is the rate-determining step for hydrolysis reaction, while the fracture of B-H bond in AB is also well revealed by attenuated total reflectance (ATR)-Fourier transform infrared (FTIR) spectroscopy. Significantly, the flexible on-demand hydrogen generation is achieved by using chemical switches for on-off AB hydrolysis. This study provides a new support platform based on two-dimensional MBene to exploit efficient catalysts to boost AB dehydrogenation.
载体与活性金属之间的配位对于氨硼烷（AB）水解反应的催化效率至关重要。在本研究中，我们报道了一种基于硼化钼（MBene）MoAlB的新型催化载体，并证明MoAlB与钌纳米颗粒的有效结合能够实现显著增强的产氢性能。由于反应物的高效活化和解离，最佳的Ru/MoAlB催化剂在无碱条件下对AB催化水解实现了494 mol mol⁻¹ min⁻¹的大周转频率、119817 mL min⁻¹ g⁻¹的高产氢速率以及39.2 kJ mol⁻¹的良好表观活化能。同位素测试表明，H₂O中OH键的断裂是水解反应的速率决定步骤，而AB中B-H键的断裂也通过衰减全反射（ATR）-傅里叶变换红外（FTIR）光谱得到了很好的揭示。值得注意的是，通过使用化学开关来开启和关闭AB水解，实现了灵活的按需产氢。本研究提供了一个基于二维MBene的新载体平台，以开发高效催化剂来促进AB脱氢。
