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

Nano-Micro Letters 2022年第12期14卷 387-400页

作者： Chengkai Xia Yuankai Li Minyeong Je jaekyum kim Sung Min Cho Chang Hyuck Choi Heechae Choi Tae-Hoon kim Jung Kyu kim School of Chemical Engineering Sungkyunkwan University(SKKU)2066 Seobu-roJangan-guSuwon 16419Republic of Korea Theoretical Materials and Chemistry Group Institute of Inorganic ChemistryUniversity of CologneGreinstr.650939 CologneGermany Department of Chemistry Pohang University of Science and Technology(POSTECH)Pohang 37673Republic of Korea Department of Materials Science and Engineering Engineering Research CenterChonnam National UniversityGwangju 61186Republic of Korea

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 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 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

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A conformal titanyl phosphate amorphous overlayer for enhancing photoelectrochemical hydrogen peroxide production

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Journal of Energy Chemistry 2023年第11期86卷 399-408,I0009页

作者： jaekyum kim Young Eun kim Minyeong Je Won Tae Hong Chang-Lyoul Lee Tae-Hoon kim Sung Min Cho Chang Hyuck Choi Heechae Choi Woo-Seok Choe Jung Kyu kim School of Chemical Engineering Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea SKKU Advanced Institute of Nano Technology(SAINT) Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Theoretical Materials&Chemistry Group Institute of Inorganic ChemistryUniversity of CologneGreinstr.650939CologneGermany Advanced Photonics Research Institute(APRI) Gwangju Institute of Science and Technology(GIST)Gwangju 61005Republic of Korea Department of Materials Science and Engineering Chonnam National UniversityGwangju 61186Republic of Korea Department of Chemistry Pohang University of Science and Technology(POSTECH)Pohang 37673Republic of Korea Institute for Convergence Research and Education in Advanced Technology(I-CREATE) Yonsei UniversitySeoul 03722Republic of Korea Department of Chemistry Xi’an Jiaotong-Liverpool UniversitySuzhou 215123JiangsuChina

Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.

关键词： Solar H_(2)O_(2) production In-situ surface reforming Titanyl phosphate Amorphous overlayer Reaction pathway control

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A sulfur self-doped multifunctional biochar catalyst for overall water splitting and a supercapacitor from Camellia japonica flowers

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Carbon Energy 2022年第4期4卷 491-505页

作者： Chengkai Xia Subramani Surendran Seulgi Ji Dohun kim Yujin Chae jaekyum kim Minyeong Je Mi-Kyung Han Woo-Seok Choe Chang Hyuck Choi Heechae Choi Jung Kyu kim Uk Sim School of Chemistry Engineering Sungkyunkwan UniversitySuwonRepublic of Korea Hydrogen Energy Technology Laboratory Korea Institute of Energy Technology(KENTECH)NajuRepublic of Korea Department of Materials Science&Engineering Chonnam National UniversityGwangjuRepublic of Korea Theoretical Materials&Chemistry Group University of CologneCologneGermany Research Institute NEEL SciencesInc.NajuSouth Korea Department of Chemistry Pohang University of Science and Technology(POSTECH)Gyeongsangbuk-doRepublic of Korea

A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content in the camellia flower facilitates in situ self-doping of sulfur,which highly activates the camellia-driven biochar(SA-Came)as a multifunctional catalyst with the enhanced electron-transfer ability and long-term durability.For water splitting,an SA-Came-based electrode is highly stable and shows reaction activities in both hydrogen and oxygen evolution reactions,with overpotentials of 154 and 362 mV at 10 mA cm^(−2),respectively.For supercapacitors,SA-Came achieves a specific capacitance of 125.42 F g^(−1)at 2 A g^(−1)and high cyclic stability in a three-electrode system in a 1 M KOH electrolyte.It demonstrated a high energy density of 34.54 Wh kg^(−1)at a power density of 1600 W kg^(−1)as a symmetric hybrid supercapacitor device with a wide working potential range of 0-1.6 V.

关键词： activated carbon biomass supercapacitor sustainable chemistry water splitting

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