Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation  

作　　者：Chengkai Xia Yuankai Li Minyeong Je Jaekyum Kim Sung Min Cho Chang Hyuck Choi Heechae Choi Tae-Hoon Kim Jung Kyu Kim 

机构地区：[1]School of Chemical Engineering,Sungkyunkwan University(SKKU),2066 Seobu-ro,Jangan-gu,Suwon 16419,Republic of Korea [2]Theoretical Materials and Chemistry Group,Institute of Inorganic Chemistry,University of Cologne,Greinstr.6,50939 Cologne,Germany [3]Department of Chemistry,Pohang University of Science and Technology(POSTECH),Pohang 37673,Republic of Korea [4]Department of Materials Science and Engineering,Engineering Research Center,Chonnam National University,Gwangju 61186,Republic of Korea

出　　处：《Nano-Micro Letters》2022年第12期387-400,共14页纳微快报（英文版）

基　　金：This study was supported by the financial support from the Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(20214000000500,training program of CCUS for the green growth);This work was supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government,Ministry of Science and ICT(MSIT)(2020M3D1A2102837).

摘　　要：A rational regulation of the solar water splitting reaction pathway by adjusting the surface composition and phase structure of catalysts is a substantial approach to ameliorate the sluggish reaction kinetics and improve the energy conversion efficiency.In this study,we demonstrate a nanocrystalline iron pyrophosphate(Fe_(4)(P_(2)O_(7))_(3),FePy)-regulated hybrid overlayer with amorphous iron phosphate(FePO_(4),FePi)on the surface of metal oxide nanostructure with boosted photoelectrochemical(PEC)water oxidation.By manipulating the facile electrochemical surface treatment followed by the phosphating process,nanocrystalline FePy is localized in the FePi amorphous overlayer to form a heterogeneous hybrid structure.The FePy-regulated hybrid overlayer(FePy@FePi)results in significantly enhanced PEC performance with long-term durability.Compared with the homogeneous FePi amorphous overlayer,FePy@FePi can improve the charge transfer efficiency more significantly,from 60% of FePi to 79%of [e-mail] density-functional theory calculations reveal that the coexistence of FePi and FePy phases on the surface of metal oxide results in much better oxygen evolution reaction kinetics,where the FePi was found to have a typical down-hill reaction for the conversion from OH*to O_(2),while FePy has a low free energy for the formation of OH*.

关 键 词：Water oxidation Photoelectrochemical cell Metal pyrophosphate Electrochemical surface treatment 

分 类 号：TQ426[化学工程]