Co0.6Ni0.4/NC催化剂的制备及其催化氨硼烷水解制氢性能研究

PREPARATION OF Co0.6Ni0.4/NC CATALYST AND ITS CATALYTIC PERFORMANCE FOR HYDROGEN PRODUCTION FROM AMMONIA BORANE HYDROLYSIS

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中文摘要：为了提高氨硼烷(AB)在温和条件下的水解制氢性能,开发了兼具高活性和高稳定性的催化剂.首先在常温常压下直接搅拌反应物溶液得到沸石咪唑酯骨架材料CoNi-ZIF[金属有机骨架(MOFs)材料的一种],然后高温焙烧CoNi-ZIF前体制得以氮掺杂多孔炭(NC)为载体的CoxNi1-x/NC(x为Co原子的摩尔分数,0＜x＜1)催化剂.采用扫描电子显微镜、透射电镜、X射线光电子能谱等一系列手段对CoxNi1-x/NC催化剂的结构形貌进行表征,并通过改变Co/Ni金属配比、催化剂用量、AB浓度、反应温度等条件探究催化剂对AB水解制氢反应的催化性能.结果表明:Co/Ni摩尔比为6∶4时得到的催化剂Co06Ni0.4/NC拥有较大的比表面积;Co0.6Ni0.4/NC的催化活性最优,在温度298 K下其催化AB完全水解的时间最短;Co0.6Ni0.4/NC催化AB制氢的反应转化频率为1 832.79 h-1,活化能为64.81 kJ/mol;经10次循环使用,其催化AB完全水解制氢的速率几乎没有变化,循环使用稳定性良好.

外文摘要：In order to improve the performance of ammonia borane(AB)hydrolysis for hydrogen production under mild conditions,a catalyst with both high activity and high stability was developed.Firstly,the zeolitic imidazolate frameworks material CoNi-ZIF(a type of metal-organic frameworks material)was prepared by directly stirring the reaction solution at normal temperature and pressure,and then the CoNi-ZIF precursor was calcined at high temperature to prepare CoxNi1-x/NC catalyst(where x represents the molar fraction of Co atoms,0＜x＜1)supported on nitrogen-doped porous carbon(NC).The structure and morphology of CoxNi1-x/NC catalyst were characterized by scanning spectroscopy microscopy,transmission electron microscopy,and X-ray photoelectron spectroscopy,and the catalytic performance of the catalyst for hydrogen production from hydrolysis of AB was investigated by changing the metal ratio of Co/Ni,the amount of catalyst,the concentration of AB,reaction temperature and other conditions.The results showed that Co0.6Ni0.4/NC with a Co/Ni molar ratio of 6∶4 had a larger specific surface area and the best catalytic activity,and the time of AB complete hydrolysis was the shortest at 298 K.The TOF value of Co0.6Ni0.4/NC catalyzing AB hydrolysis for hydrogen production was 1 832.79 h-1,and the activation energy(Ea)of the reaction was 64.81 kJ/mol.After 10 cycles of use,the rate of hydrogen production by catalyzing the complete hydrolysis of AB had almost no change,and the catalytic activity was still good.

外文关键词：

hydrogen storage materialammonia borane hydrolysismetal-organic frameworks derived materialCo/Ni alloy

作者：

朱若璇、刘睿莹、谢婧、陈香香、王志远、曹振

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作者单位：

安徽工业大学化学与化工学院,安徽马鞍山 243032

安徽工业大学生物膜法水质净化及利用技术教育部工程研究中心

关键词：

储氢材料氨硼烷水解金属有机骨架衍生材料 CoNi合金

基金：

安徽省自然科学基金青年基金项目生物膜法水质净化及利用技术教育部工程研究中心开放基金资助项目国家级大学生创新创业训练计划项目安徽省大学生创新创业训练计划项目安徽省大学生创新创业训练计划项目安徽省大学生创新创业训练计划项目

项目编号：

1908085QB68BWPU2023KF06202210360037S202110360217S202310360212S202310360222

出版年：

2024

石油炼制与化工

中国石油化工股份有限公司石油化工科学研究院

石油炼制与化工

CSTPCD北大核心

影响因子：0.825

ISSN：1005-2399

年,卷(期)：2024.55(7)