焙烧温度和分散剂对Co_(0.8)Cu_(0.2)/CNC催化氨硼烷水解制氢性能的影响研究  

The effects of calcination temperature and dispersants on the catalytic performance of Co_(0.8)Cu_(0.2)/CNC for the hydrolysis of ammonia borane to hydrogen

作　　者：李蓉 左佑华 徐立成 花俊峰 冯佳佳 许立信[1] 叶明富[1,4,5,6] 万超 LI Rong;ZUO Youhua;XU Licheng;HUA Junfeng;FENG Jiajia;XU Lixin;YE Mingfu;WAN Chao(School of Chemistry and Chemical Engineering,Anhui University of Technology,Ma’anshan 243032,China;College of Polymer Science and Engineering,Qingdao University of Science and Technology,Qingdao 266042,China;Zhejiang Environment Technology Co.,Ltd,Hangzhou 310027,China;Engineering Research Center of Biofilm Water Purification and Utilization Technology of Ministry of Education,Anhui University of Technology,Ma’anshan 243032,China;Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,China;Key Laboratory of Green Energy and Environment Catalysis,Ningde Normal University,Ningde 352100,China;Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou University,Changzhou 213164,China;College of Chemical Engineering and Biological Engineering,Zhejiang University,Hangzhou 310058,China)

机构地区：[1]安徽工业大学化学与化工学院,安徽马鞍山243032 [2]青岛科技大学高分子科学与工程学院,山东青岛266042 [3]浙江省环境科技有限公司,浙江杭州310027 [4]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,安徽马鞍山243032 [5]南开大学先进能源材料化学教育部重点实验室,天津300071 [6]宁德师范学院绿色能源与环境催化福建高校重点实验室,福建宁德352100 [7]常州大学江苏省绿色催化材料与技术重点实验室,江苏常州213164 [8]浙江大学化学工程与生物工程学院,浙江杭州310058

出　　处：《燃料化学学报（中英文）》2024年第11期1736-1744,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金青年基金(22108238,U22A20408);安徽省自然科学基金青年基金(1908085QB68);中国博士后项目(2019M662060,PC2022046,2020T130580);江苏省绿色催化材料与技术重点实验室(BM2012110);绿色能源与环境催化福建省高校重点实验室开放课题(FJ-GEEC202204);2022、2023年国家级大学生创新创业训练计划项目(202210360037、S202310260212);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(BWPU2023KF06)资助。

摘　　要：氨硼烷(NH_(3)BH_(3),AB)被认为是一种便携式制氢的理想储氢材料。本工作在常温下搅拌反应物得到Co_(0.8)Cu_(0.2)-ZIF前驱体,并高温焙烧此前驱体制备了一种双金属碳立方体(Co_(0.8)Cu_(0.2)/CNC)催化剂。此外,采用多种表征方法对催化剂的微观结构以及组成成分进行了研究。通过单一变量法探究了催化剂的变化规律。结果表明,少量Cu的加入会对Co_(a8)Cu_(a2)/CNC催化剂的立方体形貌有一定的稳固作用。当分散剂为CTAB且焙烧温度为873 K时,其催化AB水解制氢的活化能(E_a)为50.79 kJ/mol,转化频率(TOF)值高达23.37 min^(-1)。此外,该催化剂经过25次循环后仍然可以催化AB完全水解制氢,表明该催化剂的稳定性能良好。Ammonia borane(NH3BH3,AB)is considered as an ideal hydrogen storage material for portable hydrogen production.In this paper,a bimetallic carbon cube(Co_(0.8)Cu_(0.2)/CNC)catalyst was prepared by high-temperature calcination of the Co_(0.8)Cu_(0.2)-ZIF precursor,which was obtained by stirring the reactants at room temperature.In addition,the microstructure and composition of the catalyst were investigated using various characterization methods.The change regularity of the catalyst was explored through the single-variable method.The results showed that the addition of a small amount of Cu had a stabilizing effect on the cubic morphology of the Co_(0.8)Cu_(0.2)/CNC catalyst.When the dispersant was CTAB and the calcination temperature was 873 K,the activation energy(Ea)for catalyzing the hydrolysis of AB to hydrogen was 50.79 kJ/mol with the transition frequency(TOF)value as high as 23.37 min^(-1).Moreover,the catalyst could still catalyze the complete hydrolysis of AB to hydrogen after 25 cycles,which indicated that the catalyst had good stability performance.

关 键 词：双金属碳立方体 氨硼烷 水解制氢 

分 类 号：O643.36[理学—物理化学]