Wei Yue-Wei, Yang Guang, Xu Xi-Xi, Liu Yan-Yan, Li Bao-Jun, Wang Yong-Zhao, Zhao Yong-Xiang
School of Chemistry and Chemical Engineering, Shanxi University Taiyuan 030006 China
Engineering Research Center of Ministry of Education for Fine Chemicals, Shanxi University Taiyuan 030006 China.
RSC Adv. 2023 Mar 8;13(11):7673-7681. doi: 10.1039/d3ra00358b. eCollection 2023 Mar 1.
Ammonia borane (AB) is a potential hydrogen storage material with high-efficiency hydrolytic dehydrogenation under a suitable catalyst. Noble metal catalysts have drawn a lot of attention. In this study, a carbon-coated zeolite was obtained by calcination at high temperatures using glucose as a carbon source. Pt nanoparticles were fixed on a core-shell composite support by a simple chemical reduction method. A series of catalysts were prepared with different synthesis parameters. The results show that PSC-2 has excellent catalytic performance for hydrolytic dehydrogenation of AB in alkaline solution at room temperature, and the turnover frequency (TOF) is 593 min. The excellent catalytic performance is attributed to the carbon layer on the zeolite surface which inhibits the aggregation or deformation of metals in the catalytic reaction. The metal-support interaction activates the water and accelerates the rate-limiting step of hydrolysis. The activation energy ( = 44 kJ mol) was calculated based on the reaction temperature. In addition, the kinetics of AB hydrolysis was studied, and the effects of catalyst concentration, AB concentration and NaOH concentration on AB hydrolysis rate were further investigated. The high-efficiency catalyst prepared in this work provides a new strategy for the development of chemical hydrogen production in the field of catalysis.
氨硼烷（AB）是一种潜在的储氢材料，在合适的催化剂作用下可进行高效水解脱氢反应。贵金属催化剂备受关注。在本研究中，以葡萄糖为碳源，通过高温煅烧获得了碳包覆沸石。采用简单的化学还原法将铂纳米颗粒固定在核壳复合载体上。通过不同的合成参数制备了一系列催化剂。结果表明，PSC - 2在室温下对碱性溶液中AB的水解脱氢反应具有优异的催化性能，周转频率（TOF）为593 min⁻¹。优异的催化性能归因于沸石表面的碳层，它在催化反应中抑制了金属的聚集或变形。金属 - 载体相互作用使水活化并加速了水解的限速步骤。基于反应温度计算出活化能（Ea = 44 kJ mol⁻¹）。此外，研究了AB水解的动力学，并进一步考察了催化剂浓度、AB浓度和NaOH浓度对AB水解速率的影响。本工作制备的高效催化剂为催化领域化学制氢的发展提供了新策略。
