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作 者:YANG Tianxuan WU Meixia WANG Junli CHEN Ning TANG Changqiang LI Jiang SHANG Jianpeng GUO Yong LI Zuopeng 杨天璇;武美霞;王俊丽;陈宁;唐昌强;李江;尚建鹏;郭永;李作鹏(山西大同大学化学与化工学院,山西省清洁能源材料联合实验室,山西大同037009)
出 处:《燃料化学学报(中英文)》2025年第4期555-564,共10页Journal of Fuel Chemistry and Technology
基 金:supported by the National Natural Science Foundation of China(21908135);Natural Science Foundation of Shanxi Datong University(2022K23);Graduate Research Innovation and Practice Innovation Projects of Shanxi Datong University(23CX31);Postgraduate Educational Reform and Research Program of Shanxi Datong University(23JG07)。
摘 要:Ammonia borane(AB)has received much attention as an environmentally friendly,non-toxic,room temperature stable hydrogen storage material with high hydrogen content of 19.6%.However,its hydrolysis for hydrogen production at room-temperature is kinetically slow and requires precious metal catalysts.In this work,it is found that the prepared Raney Ni W-r treated with high concentration of NaOH(6.25 mol/L)at 110℃exhibited excellent catalytic performance for AB hydrolysis at room temperature.The Raney Ni W-r can promote the AB complete hydrolysis within 60 s under basic condition at small sized trials,even higher than that of the 20%Pt/C catalyst.Its apparent activation energy at room temperature is only 26.6 kJ/mol and the turnover frequency(TOF)value is as high as 51.42 min-1.Owing to its high density and magnetic properties,the catalyst is very easy for magnetic separation.Furthermore,possible mechanism of the hydrolytic reaction of AB based on experimental results is proposed.As a well-established industrial catalyst,Raney Ni has been prepared on a large scale at low cost.This study provides a promising pathway for the large-scale preparation of low-cost and recyclable catalysts for AB hydrolysis.氨硼烷(AB)作为一种环境友好、无毒、室温稳定并高含氢量(质量储氢密度达19.6%)的储氢材料受到人们的广泛关注。然而,其室温水解制氢过程是动力学缓慢过程且需要贵金属催化剂。本工作中,通过对NiAl合金在110℃下进行高浓度NaOH(6.25 mol/L)处理,发现自制的雷尼镍(W-r)催化剂在室温下展现出优异的AB水解催化性能(碱性条件下小试反应可以实现60 s完全水解),甚至高于20%Pt/C催化剂。其在室温下的表观活化能仅为26.6 kJ/mol,且转换频率(TOF)值高达51.42 min^(-1)。此外,其高密度和磁性能使得催化剂很容易进行磁分离。最后,基于实验推断了雷尼镍催化AB水解可能的反应机理。作为一种工业催化剂,雷尼镍已经实现了低成本规模制备。本研究为发展低成本规模制备、可回收的AB水解催化剂提供了一条非常有前景的途径。
关 键 词:ammonia borane HYDROLYSIS Raney Ni hydrogen production
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