氮掺杂空心碳纳米球嵌入氮掺杂石墨烯负载钯纳米粒子作为甲酸氧化的高效电催化剂  

N-doped hollow carbon nanospheres embedded in N-doped graphene loaded with palladium nanoparticles as an efficient electrocatalyst for formic acid oxidation

作　　者：房越 杨富开 曲微丽 邓超[1] 王振波[3,4] FANG Yue;YANG Fu-kai;QU Wei-li;DENG Chao;WANG Zhen-bo(College of Chemistry and Chemical Engineering,Harbin Normal University,Harbin 150025,China;Key Laboratory of Photochemical Biomaterials and Energy Storage Materials,Harbin Normal University,Harbin 150025,China;MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage,School of Chemistry and Chemical Engineering,State Key Lab of Urban Water Resource and Environment,Harbin Institute of Technology,Harbin 150001,China;Shenzhen Key Laboratory of Special Functional Materials,Shenzhen Engineering Laboratory for Advance Technology of Ceramics,Guangdong Research Center for Interfacial Engineering of Functional Materials,College of Materials Science and Engineering,Shenzhen University,Shenzhen 518060,China)

机构地区：[1]哈尔滨师范大学化学化工学院,黑龙江哈尔滨150025 [2]哈尔滨师范大学黑龙江省光化学生物材料与储能材料重点实验室,黑龙江哈尔滨150025 [3]哈尔滨工业大学化学化工学院新能源转化与存储关键材料技术工信部重点实验室,国家哈尔滨工业大学重点实验室城市水资源与环境实验室,黑龙江哈尔滨150001 [4]深圳大学材料科学与工程学院深圳市特种功能材料重点实验室,深圳市陶瓷先进技术工程实验室,广东省功能材料界面工程研究中心,广东深圳518060

出　　处：《新型炭材料（中英文）》2024年第2期321-333,共13页New Carbon Materials

基　　金：国家自然科学基金(21503059);哈尔滨师范大学研究生创新基金(HSDSSCX2019-37).

摘　　要：低成本、高活性、耐久性好的高效电催化剂对直接甲酸燃料电池的应用起着至关重要的作用。本文采用简单经济的方法,研究了以三维层状多孔结构嵌入氮掺杂石墨烯(NG)的氮掺杂空心碳纳米球(NHCN)负载Pd纳米粒子作为直接甲酸燃料电池催化剂。由于具有独特的氮原子掺杂三维互联层状多孔结构,Pd纳米颗粒尺寸较小的Pd/NHCN@NG催化剂具有较大的催化活性表面积、优越的电催化活性、较高的稳态电流密度和较强的抗CO中毒能力,明显超过传统的Pd/C、Pd/NG和Pd/NHCN催化剂对甲酸电氧化的催化性能。通过优化HCN/GO比,当HCN/GO质量比为1∶1时,Pd/NHCN@NG催化剂对甲酸的催化氧化性能最佳,其活性是Pd/C的4.21倍。本工作开发了一种优越的碳基电催化剂载体材料,为燃料电池的发展带来了广阔的应用前景。Efficient electrocatalysts with a low cost,high activity and good durability play a crucial role in the use of direct formic acid fuel cells.Pd nanoparticles supported on N-doped hollow carbon nanospheres(NHCNs)embedded in an assembly of N-doped graphene(NG)with a three-dimensional(3D)porous structure by a simple and economical method were investigated as direct formic acid fuel cell catalysts.Because of the unique porous configuration of interconnected layers doped with nitrogen atoms,the Pd/NHCN@NG catalyst with Pd nanoparticles has a large catalytic active surface area,superior electrocatalytic activity,a high steady-state current density,and a strong resistance to CO poisoning,far surpassing those of conventional Pd/C,Pd/NG,and Pd/NHCN catalysts for formic acid electrooxidation.When the HCN/GO mass ratio was 1∶1,the Pd/NHCN@NG catalyst had an outstanding performance in the catalytic oxidation of formic acid,with an activity 4.21 times that of Pd/C.This work indicates a way to produce superior carbon-based support materials for electrocatalysts,which will be beneficial for the development of fuel cells.

关 键 词：甲酸电氧化 氮掺杂中空碳纳米球 氮掺杂石墨烯 载体材料 三维互连层状多孔结构 

分 类 号：TB33[一般工业技术—材料科学与工程]