Ruthenium(0) nanoparticles supported on nanotitania as highly active and reusable catalyst in hydrogen generation from the hydrolysis of ammonia borane

Ruthenium(0) nanoparticles supported on nanotitania as highly active and reusable catalyst in hydrogen generation from the hydrolysis of ammonia borane
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DOI:
10.1016/j.ijhydene.2014.04.091
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发表时间:
2014-06-15
影响因子:
7.2
通讯作者:
Ozkar, Saim
Ozkar, Saim
中科院分区:
工程技术2区
文献类型:
--
作者:
Akbayrak, Serdar;Tanyildizi, Seda;Ozkar, Saim

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在氨硼烷水解的过程中,通过还原浸渍在纳米二氧化钛上的钌(III)离子,原位生成负载在二氧化钛纳米球(Ru(0)/TiO 2)表面的钌(0)纳米颗粒。它们通过离心从反应溶液中分离,并通过先进的分析技术的组合进行表征。结果表明,在二氧化钛纳米球表面形成了高度分散的钌(0)纳米粒子,其粒径在1.5-3.3 nm之间。Ru(0)/TiO 2在25.0 +/-0.1 ℃下对氨硼烷水解制氢具有很高的催化活性,转化频率高达241 min(-1)。它们提供了前所未有的催化寿命,通过在25.0 +/- 0.1摄氏度下氨硼烷水解制氢的总转换数(TTO = 71,500)来测量。该报告还包括氨硼烷催化水解的动力学研究结果,取决于温度,以确定反应的活化能(E-a = 70 +/- 2 kJ/mol)和催化剂浓度,以建立反应的速率定律。版权所有(C)2014,氢能出版物有限责任公司。由爱思唯尔有限公司出版。保留所有权利。
Ruthenium(0) nanoparticles supported on the surface of titania nanospheres (Ru(0)/TiO2) were in situ generated from the reduction of ruthenium(III) ions impregnated on nanotitania during the hydrolysis of ammonia borane. They were isolated from the reaction solution by centrifugation and characterized by a combination of advanced analytical techniques. The results reveal that highly dispersed ruthenium(0) nanoparticles of size in the range 1.5-3.3 nm were formed on the surface of titania nanospheres. Ru(0)/TiO2 show high catalytic activity in hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value up to 241 min(-1) at 25.0 +/- 0.1 degrees C. They provide unprecedented catalytic lifetime measured by total turnover number (TTO = 71,500) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 +/- 0.1 degrees C. The report also includes the results of kinetic study on the catalytic hydrolysis of ammonia borane depending on the temperature to determine the activation energy of the reaction (E-a = 70 +/- 2 kJ/mol) and the catalyst concentration to establish the rate law of the reaction. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.