Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation
Abstract 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 nano...
| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
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SpringerOpen
2022-10-01
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| Series: | Nano-Micro Letters |
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| Online Access: | https://doi.org/10.1007/s40820-022-00955-w |
| _version_ | 1811223497579429888 |
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| author | Chengkai Xia Yuankai Li Minyeong Je Jaekyum Kim Sung Min Cho Chang Hyuck Choi Heechae Choi Tae-Hoon Kim Jung Kyu Kim |
| author_facet | Chengkai Xia Yuankai Li Minyeong Je Jaekyum Kim Sung Min Cho Chang Hyuck Choi Heechae Choi Tae-Hoon Kim Jung Kyu Kim |
| author_sort | Chengkai Xia |
| collection | DOAJ |
| description | Abstract 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 (Fe4(P2O7)3, FePy)-regulated hybrid overlayer with amorphous iron phosphate (FePO4, 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 FePy@FePi. Our 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 O2, while FePy has a low free energy for the formation of OH*. Graphical abstract |
| first_indexed | 2024-04-12T08:33:45Z |
| format | Article |
| id | doaj.art-3894b8ad43c34587b5237c36c36f3041 |
| institution | Directory Open Access Journal |
| issn | 2311-6706 2150-5551 |
| language | English |
| last_indexed | 2024-04-12T08:33:45Z |
| publishDate | 2022-10-01 |
| publisher | SpringerOpen |
| record_format | Article |
| series | Nano-Micro Letters |
| spelling | doaj.art-3894b8ad43c34587b5237c36c36f30412022-12-22T03:40:03ZengSpringerOpenNano-Micro Letters2311-67062150-55512022-10-0114111410.1007/s40820-022-00955-wNanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water OxidationChengkai Xia0Yuankai Li1Minyeong Je2Jaekyum Kim3Sung Min Cho4Chang Hyuck Choi5Heechae Choi6Tae-Hoon Kim7Jung Kyu Kim8School of Chemical Engineering, Sungkyunkwan University (SKKU)School of Chemical Engineering, Sungkyunkwan University (SKKU)Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of CologneSchool of Chemical Engineering, Sungkyunkwan University (SKKU)School of Chemical Engineering, Sungkyunkwan University (SKKU)Department of Chemistry, Pohang University of Science and Technology (POSTECH)Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of CologneDepartment of Materials Science and Engineering, Engineering Research Center, Chonnam National UniversitySchool of Chemical Engineering, Sungkyunkwan University (SKKU)Abstract 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 (Fe4(P2O7)3, FePy)-regulated hybrid overlayer with amorphous iron phosphate (FePO4, 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 FePy@FePi. Our 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 O2, while FePy has a low free energy for the formation of OH*. Graphical abstracthttps://doi.org/10.1007/s40820-022-00955-wWater oxidationPhotoelectrochemical cellMetal pyrophosphateElectrochemical surface treatment |
| spellingShingle | Chengkai Xia Yuankai Li Minyeong Je Jaekyum Kim Sung Min Cho Chang Hyuck Choi Heechae Choi Tae-Hoon Kim Jung Kyu Kim Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation Nano-Micro Letters Water oxidation Photoelectrochemical cell Metal pyrophosphate Electrochemical surface treatment |
| title | Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation |
| title_full | Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation |
| title_fullStr | Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation |
| title_full_unstemmed | Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation |
| title_short | Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation |
| title_sort | nanocrystalline iron pyrophosphate regulated amorphous phosphate overlayer for enhancing solar water oxidation |
| topic | Water oxidation Photoelectrochemical cell Metal pyrophosphate Electrochemical surface treatment |
| url | https://doi.org/10.1007/s40820-022-00955-w |
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