Hydrolytic dehydrogenation of NH3BH3 catalyzed by ruthenium nanoparticles supported on magnesium–aluminum layered double-hydroxides |
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Authors: | Xueying Qiu Jiaxi Liu Pengru Huang Shujun Qiu Chaoming Weng Hailiang Chu Yongjin Zou Cuili Xiang Fen Xu Lixian Sun |
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Institution: | Guangxi Key Laboratory of Information Materials, Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials, School of Materials Science and Engineering, Guilin University of Electronic Technology, Guilin 541004 P. R. China, Fax: +86-773-2290129, +86-773-2216607 |
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Abstract: | Ammonia borane (AB, NH3BH3) with extremely high hydrogen content (19.6 wt%) is considered to be one of the most promising chemical hydrides for storing hydrogen. According to the starting materials of AB and H2O, a hydrogen capacity of 7.8 wt% is achieved for the AB hydrolytic dehydrogenation system with the presence of a highly efficient catalyst. In this work, ruthenium nanoparticles supported on magnesium–aluminum layered double hydroxides (Ru/MgAl-LDHs) were successfully synthesized via a simple method, i.e., chemical reduction. The effect of Mg/Al molar ratios in MgAl-LDHs on the catalytic performance for AB hydrolytic dehydrogenation was systematically investigated. Catalyzed by the as-synthesized Ru/Mg1Al1-LDHs catalyst, it took about 130 s at room temperature to complete the hydrolysis reaction of AB, which achieved a rate of hydrogen production of about 740 ml s−1 g−1. Furthermore, a relatively high activity (TOF = 137.1 molH2 molRu−1 min−1), low activation energy (Ea = 30.8 kJ mol−1) and fairly good recyclability of the Ru/Mg1Al1-LDHs catalyst in ten cycles were achieved toward AB hydrolysis for hydrogen generation. More importantly, the mechanism of AB hydrolysis catalyzed by Ru/MgAl-LDHs was simulated via density functional theory. The facile preparation and high catalytic performance of Ru/MgAl-LDHs make it an efficient catalyst for hydrolytic dehydrogenation of AB.Ru/MgAl-LDHs catalyst was successfully prepared, which exhibited higher catalytic activity and lower activation energy toward the hydrolysis of ammonia borane for hydrogen production. |
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