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负载于镁铝层状双氢氧化物上的钌纳米颗粒催化的NHBH水解脱氢反应

Hydrolytic dehydrogenation of NHBH catalyzed by ruthenium nanoparticles supported on magnesium-aluminum layered double-hydroxides.

作者信息

Qiu Xueying, Liu Jiaxi, Huang Pengru, Qiu Shujun, Weng Chaoming, Chu Hailiang, Zou Yongjin, Xiang Cuili, Xu Fen, Sun Lixian

机构信息

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

出版信息

RSC Adv. 2020 Mar 9;10(17):9996-10005. doi: 10.1039/d0ra01720e. eCollection 2020 Mar 6.

Abstract

Ammonia borane (AB, NHBH) 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 HO, 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 a simple method, , 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/MgAl-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 g. Furthermore, a relatively high activity (TOF = 137.1 mol mol min), low activation energy ( = 30.8 kJ mol) and fairly good recyclability of the Ru/MgAl-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 density functional theory. The facile preparation and high catalytic performance of Ru/MgAl-LDHs make it an efficient catalyst for hydrolytic dehydrogenation of AB.

摘要

氨硼烷(AB,NH₃BH₃)具有极高的氢含量(19.6 wt%),被认为是最有前景的储氢化学氢化物之一。根据AB和H₂O的起始原料,在高效催化剂存在下,AB水解脱氢体系的储氢容量可达7.8 wt%。在本工作中,通过一种简单的方法——化学还原法,成功合成了负载在镁铝层状双氢氧化物(Ru/MgAl-LDHs)上的钌纳米颗粒。系统研究了MgAl-LDHs中Mg/Al摩尔比对AB水解脱氢催化性能的影响。在室温下,以合成的Ru/MgAl-LDHs催化剂催化,AB的水解反应约130 s完成,产氢速率约为740 ml s⁻¹ g⁻¹。此外,Ru/MgAl-LDHs催化剂对AB水解制氢具有较高的活性(TOF = 137.1 mol mol⁻¹ min⁻¹)、较低的活化能(Ea = 30.8 kJ mol⁻¹)以及在十个循环中相当好的可循环性。更重要的是,利用密度泛函理论模拟了Ru/MgAl-LDHs催化AB水解的机理。Ru/MgAl-LDHs的简便制备方法和高催化性能使其成为AB水解脱氢的高效催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/975f/9052328/2755d3a4ead2/d0ra01720e-f1.jpg

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