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Interfacial Proton Transfer for Hydrogen Evolution at the Sub-Nanometric Platinum/Electrolyte Interface

文献类型：期刊论文

作者Zhang, Hao3,4; Cao, Lina5; Wang, Yanlei6; Gan, Zhongdong6; Sun, Fanfei7; Xiao, Meiling8; Yang, Yuqi2,3; Mei, Bingbao2,3; Wu, Dongshuang1; Lu, Junling5
刊名ACS APPLIED MATERIALS & INTERFACES
出版日期2021-10-06
卷号13期号:39页码:47252-47261
关键词electrode-electrolyte interface hydrogen evolution interfacial water proton transfer operando XAS
ISSN号1944-8244
DOI10.1021/acsami.1c14615
英文摘要Understanding the dynamic process of interfacial charge transfer prior to chemisorption is crucial to the development of electrocatalysis. Recently, interfacial water has been highlighted in transferring protons through the electrode/electrolyte interface; however, the identification of the related structural configurations and their influences on the catalytic mechanism is largely complicated by the amorphous and mutable structure of the electrical double layer (EDL). To this end, sub-nanometric Pt electrocatalysts, potentially offering intriguing activity and featuring fully exposed atoms, are studied to uncover the elusive electrode/electrolyte interface via operando X-ray absorption spectroscopy during the hydrogen evolution reaction (HER). Our results show that the metallic Pt clusters derived from the reduction of sub-nanometric Pt clusters (SNM-Pt) exhibit excellent HER activity, with an only 18 mV overpotential at 10 mA/cm(2) and one-magnitude-higher mass activity than commercial Pt/C. More importantly, a unique Pt-interfacial water configuration with a Pt (from Pt clusters)-O (from water) radial distance of approximately 2.5 angstrom is experimentally identified as the structural foundation for the interfacial proton transfer. Toward high overpotentials, the interfacial water that structurally evolves from "O-close" to "O-far" accelerates the proton transfer and is responsible for the improved reaction rate by increasing the hydrogen coverage.
WOS关键词GENERALIZED GRADIENT APPROXIMATION ; RAY-ABSORPTION SPECTROSCOPY ; ELECTRICAL DOUBLE-LAYER ; ENERGY ; CATALYSTS ; WATER ; NANOSHEETS ; WAVELET ; SITES ; ATOMS
资助项目Joint Fund of the National Natural Science Foundation of China[U1732267]
WOS研究方向Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:000706187100103
出版者AMER CHEMICAL SOC
资助机构Joint Fund of the National Natural Science Foundation of China
源URL[http://ir.ipe.ac.cn/handle/122111/50567]  
专题中国科学院过程工程研究所
通讯作者Wu, Dongshuang; He, Hongyan; Jiang, Zheng
作者单位1.Kyoto Univ, Grad Sch Sci, Div Chem, Kyoto 6068502, Japan
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China
4.Soochow Univ, Inst Funct Nano & Soft Mat Lab FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China
5.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
6.Chinese Acad Sci, Beijing Key Lab Ion Liquid Clean Proc, CAS Key Lab Green Proc & Engn, Inst Proc Engn, Beijing 100190, Peoples R China
7.Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Natl Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
8.Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Peoples R China
推荐引用方式
GB/T 7714		 Zhang, Hao,Cao, Lina,Wang, Yanlei,et al. Interfacial Proton Transfer for Hydrogen Evolution at the Sub-Nanometric Platinum/Electrolyte Interface[J]. ACS APPLIED MATERIALS & INTERFACES,2021,13(39):47252-47261.
APA Zhang, Hao.,Cao, Lina.,Wang, Yanlei.,Gan, Zhongdong.,Sun, Fanfei.,...&Jiang, Zheng.(2021).Interfacial Proton Transfer for Hydrogen Evolution at the Sub-Nanometric Platinum/Electrolyte Interface.ACS APPLIED MATERIALS & INTERFACES,13(39),47252-47261.
MLA Zhang, Hao,et al."Interfacial Proton Transfer for Hydrogen Evolution at the Sub-Nanometric Platinum/Electrolyte Interface".ACS APPLIED MATERIALS & INTERFACES 13.39(2021):47252-47261.

入库方式： OAI收割

来源：过程工程研究所

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