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Vol. 14 (2022)

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

https://doi.org/10.1007/s40820-022-00955-w
Chengkai Xia
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑ro, Jangan‑gu, Suwon 16419, Republic of Korea
Yuankai Li
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑ro, Jangan‑gu, Suwon 16419, Republic of Korea
Minyeong Je
Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of Cologne, Greinstr. 6, 50939 Cologne, Germany
Jaekyum Kim
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑ro, Jangan‑gu, Suwon 16419, Republic of Korea
Sung Min Cho
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑ro, Jangan‑gu, Suwon 16419, Republic of Korea
Chang Hyuck Choi
Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
Heechae Choi
Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of Cologne, Greinstr. 6, 50939 Cologne, Germany
Tae‑Hoon Kim
Department of Materials Science and Engineering, Engineering Research Center, Chonnam National University, Gwangju 61186, Republic of Korea
Jung Kyu Kim
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑ro, Jangan‑gu, Suwon 16419, Republic of Korea

Corresponding Author: Jung Kyu Kim

legkim@skku.edu

Nano-Micro Letters, Vol. 14 (2022), Article Number: 209

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*.


Highlights:


1 Inducing a localized crystalline iron pyrophosphate in amorphous iron phosphate overlayer.
2 Enhanced photoelectrochemical water oxidation activity with long-term durability.
3 The heterogeneous hybrid structure overcoming the energy barrier in water oxidation.

Keywords

Water oxidation Photoelectrochemical cell Metal pyrophosphate Electrochemical surface treatment
Xia, Chengkai, Yuankai Li, Minyeong Je, Jaekyum Kim, Sung Min Cho, Chang Hyuck Choi, Heechae Choi, Tae‑Hoon Kim, and Jung Kyu Kim. 2022. “Nanocrystalline Iron Pyrophosphate-Regulated Amorphous Phosphate Overlayer for Enhancing Solar Water Oxidation”. Nano-Micro Letters 14 (October):209. https://doi.org/10.1007/s40820-022-00955-w.
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