功能化石墨烯担载型AuPd纳米催化剂增强甲酸制氢反应  

Hydrogen Generation from Formic Acid Boosted by Functionalized Graphene Supported AuPd Nanocatalysts

作　　者：王虹力 王男 王丽莹 宋二红 赵占奎 WANG Hongli;WANG Nan;WANG Liying;SONG Erhong;ZHAO Zhankui(Key Laboratory of Advanced Structural Materials,Ministry of Education,School of Materials Science and Engineering,Changchun University of Technology,Changchun 130012,China;State Key Laboratory of High Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China)

机构地区：[1]长春工业大学材料科学与工程学院,先进结构材料教育部重点实验室,长春130012 [2]中国科学院上海硅酸盐研究所,高性能陶瓷和超微结构国家重点实验室,上海200050

出　　处：《无机材料学报》2022年第5期547-553,共7页Journal of Inorganic Materials

基　　金：国家自然科学基金(51601018,51671035);上海市自然科学基金面上项目(21ZR1472900);吉林省教育厅“十三五”科学技术项目(JJKH20200660KJ)。

摘　　要：甲酸(FA)因具有储氢量高、易加注等优点而成为极具应用前景的新型储氢材料,寻求高效率催化剂对于解决甲酸制氢反应动力学缓慢的问题尤为重要。本工作以聚乙烯亚胺修饰石墨烯(PEI-rGO)作为催化剂衬底,通过湿化学法制备PEI-rGO担载型AuPd纳米复合材料(Au_(0.3)Pd_(0.7)/PEI-rGO)。Au_(0.3)Pd_(0.7)/PEI-rGO催化剂在催化FA制氢的反应中表现出极其优异的活性,在无添加剂辅助下的转化频率(TOF)为2357.5mol_(H_(2))·molcatalyst^(–1)·h^(–1),高于大多数相同反应条件下的异相催化剂。这归因于PEI-rGO衬底与AuPd纳米颗粒之间的强相互作用对金属活性组分的尺寸、分散度和电子结构的调控。此外,循环测试结果表明该催化剂的稳定性良好。Formic acid(FA) is considered as a new type of hydrogen storage material with great application prospect due to its high hydrogen content and easy recharging as a liquid. Seeking high efficiency catalysts to solve the problem of slow reaction kinetics of hydrogen evolution from FA is vital. In this work, polyethyleneimine modified graphene(PEI-rGO) was used as the catalyst substrate, and PEI-rGO supported AuPd nanocomposite material(Au_(0.3)Pd_(0.7)/PEI-rGO) was prepared by wet chemical method. The Au_(0.3)Pd_(0.7)/PEI-rGO catalyst exhibits remarkable activity for the hydrogen generation from FA, affording an unprecedented turnover frequency(TOF) of 2357.5mol_(H_(2))·molcatalyst^(-1)·h^(-1) without any additives, which is superior to most heterogeneous catalysts under similar reaction conditions. Its excellent catalytic performance is attributed to the strong interaction between PEI-rGO substrate and AuPd nanoparticles, which regulates the size, dispersion and electronic structure of metal active components. Furthermore, the recycle test result shows that the catalyst has good stability.

关 键 词：功能化石墨烯 纳米金属催化剂 甲酸 制氢反应 

分 类 号：TQ174[化学工程—陶瓷工业]