石墨烯负载分子铁酞菁催化剂的形貌结构调控与氧还原催化应用  

Molecular iron phthalocyanine catalysts on morphology-engineered graphene towards the oxygen reduction reaction

作　　者：高曼 刘静静 叶龚兰 赵忠坤 柳建斌 何观朝 龚智超 黄康 孙洪涛 费慧龙 Man Gao;Jingjing Liu;Gonglan Ye;Zhongkun Zhao;Jianbin Liu;Guanchao He;Zhichao Gong;Kang Huang;Hongtao Sun;Huilong Fei(Advanced Catalytic Engineering Research Center of the Ministry of Education,State Key Laboratory for Chemo/Biosensing and Chemometrics,and College of Chemistry and Chemical Engineering,Hunan University,Changsha 410082,China;The Harold&Inge Marcus Department of Industrial&Manufacturing Engineering,Materials Research Institute(MRI),The Pennsylvania State University,University Park 16802,Pennsylvania,USA)

机构地区：[1]Advanced Catalytic Engineering Research Center of the Ministry of Education,State Key Laboratory for Chemo/Biosensing and Chemometrics,and College of Chemistry and Chemical Engineering,Hunan University,Changsha 410082,China [2]The Harold&Inge Marcus Department of Industrial&Manufacturing Engineering,Materials Research Institute(MRI),The Pennsylvania State University,University Park 16802,Pennsylvania,USA

出　　处：《Science China Materials》2023年第10期3865-3874,共10页中国科学（材料科学（英文版）

基　　金：financial support from the National Natural Science Foundation of China(92163116),the support from the National Natural Science Foundation of China(22209043);the Major Program of the Natural Science Foundation of Hunan Province(2021JC0006)。

摘　　要：分散在纳米碳基底上的分子催化剂由于具有明确的活性位点和结构可调的特点,成为了一类独特的单原子催化剂,有望代替贵金属催化剂用于电催化氧还原反应.本文中,我们开发了一种高活性氧还原催化剂,该催化剂由均匀且密集分散在泡芙状石墨烯载体上的铁酞菁(FePc/PG)构成.泡芙状石墨烯载体由于具有独特的皱褶和球状形貌,具有较大的比表面积和多尺度的孔结构,有利于FePc的高密度负载、活性位点的暴露和催化过程中传质效率的提高.当用旋转圆盘电极评估性能时,FePc/PG表现出优异的半波电位,达0.909 V(相对于可逆氢电极).此外,当用作气体扩散电极时,FePc/PG在高电流密度下表现出优异的高倍率和高功率性能.这项工作为设计纳米碳材料的形貌以及高性能异相分子催化剂提供了有效的策略,有望在多种能源转换和存储技术中得到应用.Molecular catalysts dispersed on nanocarbon substrates represent a unique class of single atom catalysts(SACs)for their well-defined active sites and tailorable structures,and are promising substitutes to precious metals for catalyzing the technologically important oxygen reduction reaction(ORR).Herein,we develop a highly active ORR catalyst consisting of iron phthalocyanine uniformly and densely dispersed on puff-like graphene(FePc/PG).With the unique crumpled and spheroid morphology,the graphene carrier possesses a large surface area and multiscale porosity,benefiting the high-density loading of FePc,exposure of the active sites and mass transfer efficiency during catalysis.When evaluated by a rotating disk electrode,FePc/PG presents a high half-wave potential of 0.909 V vs.the reversible hydrogen electrode.Furthermore,when employed as the gas diffusion electrode,FePc/PG exhibits outstanding high-rate and highpower capabilities at practically high current densities.This work provides efficient strategies to engineer the morphology of the nanocarbon substrates to design high-performance heterogeneous molecular catalysts toward applications in diverse energy conversion and storage technologies.

关 键 词：GRAPHENE single atom catalyst iron phthalocyanine morphology engineering oxygen reduction reaction 

分 类 号：TQ426[化学工程]