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Interfacial charge transfer mechanism of oxygen reduction reaction in alkali media: Effects of molecular charge states and triphenylamine substituent on cobalt porphyrin electrocatalysts

文献类型：期刊论文

作者Xu, Qingxiang1; Zhao, Long1; Yuan, Rui1; Chen, Yan1; Xue, Zhaoli1; Zhang, Jianming1; Qiu, Xinping2; Qu, Jingkui3
刊名COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
出版日期2021-11-20
卷号629页码:9
关键词Cobalt porphyrin Oxygen reduction reaction Triphenylamine Alkaline electrolyte Partial charge
ISSN号0927-7757
DOI10.1016/j.colsurfa.2021.127435
英文摘要Substituents can affect the partial charge distribution on porphyrin, and in tandem with the ion states in electrolyte, the charge transfer mechanism can be altered at catalytic interface. Three cobalt porphyrins with methyl phenyl, 2,1,3-benzothiadiazole (BTD) and BTD-triphenylamine (TPA) substituents at the 5,15-positions, nominated as CoPor, BTD-CoPor and TPA-BTD-CoPor, respectively, have been examined in oxygen reduction reactions (ORR) under alkaline condition. Reduced reduction potentials and enhanced response current densities were observed on the two substituent porphyrin-coated catalysts as compared to CoPor/C. Importantly, TPABTD-CoPor/C obtained slightly larger ORR current with less hydroperoxide anion generation yields than BTDCoPor/C. We proposed that the electronic structure along with the induced partial charge effect caused the difference in ORR potential, while the electron-withdrawing property of BTD contributed to the increased response current. Though TPA unit still benefits the ORR performance, the more exposed cation orbitals on TPA that merit the acidic ORR activity was suggested to be ineffective in alkali condition. These findings demonstrate the importance of the induced intramolecular partial charges in affecting the catalytic process in alkali medium and point out the limitation in utilizing the structural merit of TPA in accelerating the interfacial charge transfer.
WOS关键词CARBON NANOTUBES ; DIOXYGEN REDUCTION ; CATALYST ; COMPLEXES ; ELECTROREDUCTION ; PERFORMANCE ; HYDROGEN ; O-2
资助项目National Natural Science Foundation of China[22075110] ; National Natural Science Foundation of China[51872128] ; Postdoctoral Foundation of Jiangsu Province[2021K068A] ; Centre for High Performance Computing in Jiangsu University
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000703312200002
出版者ELSEVIER
资助机构National Natural Science Foundation of China ; Postdoctoral Foundation of Jiangsu Province ; Centre for High Performance Computing in Jiangsu University
源URL[http://ir.ipe.ac.cn/handle/122111/50432]  
专题中国科学院过程工程研究所
通讯作者Zhao, Long; Zhang, Jianming; Qiu, Xinping
作者单位1.Jiangsu Univ, Sch Chem & Chem Engn, Zhenjiang 212013, Jiangsu, Peoples R China
2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
3.Chinese Acad Sci, Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714		 Xu, Qingxiang,Zhao, Long,Yuan, Rui,et al. Interfacial charge transfer mechanism of oxygen reduction reaction in alkali media: Effects of molecular charge states and triphenylamine substituent on cobalt porphyrin electrocatalysts[J]. COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS,2021,629:9.
APA Xu, Qingxiang.,Zhao, Long.,Yuan, Rui.,Chen, Yan.,Xue, Zhaoli.,...&Qu, Jingkui.(2021).Interfacial charge transfer mechanism of oxygen reduction reaction in alkali media: Effects of molecular charge states and triphenylamine substituent on cobalt porphyrin electrocatalysts.COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS,629,9.
MLA Xu, Qingxiang,et al."Interfacial charge transfer mechanism of oxygen reduction reaction in alkali media: Effects of molecular charge states and triphenylamine substituent on cobalt porphyrin electrocatalysts".COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS 629(2021):9.

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来源：过程工程研究所

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