Rh/N-SBC纳米催化剂的制备及其催化氨硼烷水解产氢性能研究  

Preparation of Rh/N-SBC Nanocatalyst and Its Catalytic Performance for Hydrolytic Dehydrogenation of Ammonia Borane

作　　者：李贵 李蓉 刘勇 许立信[1] 叶明富[1,3,4,5] 万超 Li Gui;Li Rong;LiuYong;Xu Lixin;Ye Mingfu;Wan Chao(School of Chemistry and Chemical Engineering,Anhui University of Technology,Ma’anshan 243000,China;College of Chemical Engineering and Biological Engineering,Zhejiang University,Hangzhou 310027,China;Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University,Tianjin 300071,China;Anhui Key Laboratory of Photoelectric-Magnetic Functional Materials,Anhui Key Laboratory of Functional Coordination Compounds,Anqing Normal University,Anqing 246011,China;Jiangxi Province En-gineering Research Center of Ecological Chemical Industry,Jiujiang University,Jiujiang 332005,China)

机构地区：[1]安徽工业大学化学与化工学院,安徽马鞍山243000 [2]浙江大学化学工程与生物工程学院,浙江杭州310027 [3]南开大学先进能源材料化学教育部重点实验室,天津300071 [4]安庆师范大学安徽省光电磁性功能材料重点实验室,功能配合物安徽省重点实验室,安徽安庆246011 [5]九江学院江西省生态化工工程研究中心,江西九江332005

出　　处：《稀有金属》2024年第7期944-954,共11页Chinese Journal of Rare Metals

基　　金：国家自然科学基金青年项目(22108238)和联合项目(U22A20408);安徽省自然科学基金青年项目(1908085QB68);安徽省科技重大专项(201903a05020055);中国博士后面上项目(2019M662060)、派出项目(PC2022046)和特别资助站中项目(2020T130580);安徽省光电磁性功能材料重点实验室开放基金项目(ZD2021007);江西省生态化工工程研究中心开放基金项目(STKF2109);2022年国家级大学生创新创业训练计划项目(202210360037)资助。

摘　　要：氨硼烷(AB,NH_(3)BH_(3))作为储氢材料应用的关键是寻找催化性能优异的催化剂,从而进一步提高AB水解产氢的动力学和热力学性质。以氮掺杂蔗糖基碳材料(N-SBC)作为载体,负载活性组分Rh,低温还原制取Rh/N-SBC催化剂用于催化AB水解产氢。通过X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电镜(TEM)等一系列表征手段对催化剂进行表征,并探究其对催化AB水解产氢的性能的影响。结果表明,N-SBC的微观形貌呈现出片状结构,金属Rh被成功负载到N-SBC上。此外,金属Rh的负载量为0.4%时,催化剂催化活性最大。经过计算得出Rh/N-SBC催化AB水解产氢反应的转化频率(TOF)值最高可达4213.7 min^(-1),活化能为55.7 k J·mol^(-1)。循环5次后,催化活性依然保持良好,表明其拥有良好的稳定性。这种优异的催化性能可归因于碳材料中掺入N元素有效改变了载体的电子结构,显著改善催化剂催化AB的水解产氢性能。With the continuous consumption of fossil fuel and releasing of greenhouse gas carbon dioxide,increasing efforts have been made to develop new approach to meet the urgent need to recyclable and pollution-free energy.In the development of various new energy sources,hydrogen energy,producing water as the only byproduct,is green and sustainable with high energy density and it has been a globally accepted clean energy source,is an ideal energy carrier.As a liquid hydrogen storage material,ammonia borane has a hydrogen storage content of 19.6%,excellent stability at room temperature and low storage cost.In addition,the reaction by-product NH4BO2 after the hydrolysis and dehydrogenation of ammonia borane can be recovered by irreversible chemical reaction without pollution to the environment.Under mild conditions,the development of an efficient and highly selective catalyst is the key to realize the application of ammonia borane hydrolytic dehydrogenation.In this paper,nitrogen-doped sucrose-based carbon material was used as the support,the active component Rh was loaded,and Rh/N-SBC catalyst was prepared by low-temperature reduction,which was used to catalyze the hydrolysis and dehydrogenation of ammonia borane.Then,the microstructure was analyzed by a series of characterization methods.To study the microscopic morphology and structure of the catalyst,Rh/N-SBC catalysts were characterized by transmission electron microscopy(TEM).X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)were used to investigate the effects of different calcination temperatures on the phase composition and crystal structure,and analyze the chemical element valence state and bond type of Rh/N-SBC catalysts.In addition,the single-variable method was used in this experiment to explore its effect on the performance of catalyzing the hydrolysis and dehydrogenation of ammonia borane.By changing the quality of sucrose during the preparation of the support,a series of Rh/N-SBC catalysts with different N-doping amounts in the support were sy

关 键 词：铑催化剂 氨硼烷(AB NH3BH3) 水解产氢 氮掺杂碳材料 

分 类 号：O643.36[理学—物理化学]