Interfacial oxygen vacancies yielding long-lived holes in hematite mesocrystal-based photoanodes

Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretica...

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Published inNature communications Vol. 10; no. 1; pp. 4832 - 12
Main Authors Zhang, Zhujun, Karimata, Izuru, Nagashima, Hiroki, Muto, Shunsuke, Ohara, Koji, Sugimoto, Kunihisa, Tachikawa, Takashi
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 23.10.2019
Nature Publishing Group
Nature Portfolio
Subjects
147/137
639/301/299/886
639/638/439/890
639/638/675
Carrier density
Charge efficiency
Depletion
Efficiency
Electrodes
Energy conversion
Energy conversion efficiency
Extreme values
Hematite
Humanities and Social Sciences
Light
multidisciplinary
Nanocrystals
Nanoparticles
Oxidation
Oxygen
Photoanodes
Radiation
Recombination
Science
Science (multidisciplinary)
Structural hierarchy
Thick films
Vacancies
Water splitting
Online AccessGet full text

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Abstract Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretical limit. Here we report thick hematite films (∼1500 nm) constructed by highly ordered and intimately attached hematite mesocrystals (MCs) for highly efficient PEC water oxidation. Due to the formation of abundant interfacial oxygen vacancies yielding a high carrier density of ∼10 20  cm −3 and the resulting extremely large proportion of depletion regions with short depletion widths (<10 nm) in hierarchical structures, charge separation and collection efficiencies could be markedly improved. Moreover, it was found that long-lived charges are generated via excitation by shorter wavelength light (below ∼500 nm), thus enabling long-range hole transfer through the MC network to drive high efficiency of light-to-energy conversion under back illumination. The performance of hematite (α-Fe 2 O 3 ) photoanodes is limited by fast charge recombination. Here, authors develop hematite mesocrystal-based photoanodes with abundant interfacial oxygen vacancies for highly efficient solar water splitting under back illumination.
AbstractList Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretical limit. Here we report thick hematite films (∼1500 nm) constructed by highly ordered and intimately attached hematite mesocrystals (MCs) for highly efficient PEC water oxidation. Due to the formation of abundant interfacial oxygen vacancies yielding a high carrier density of ∼10 20  cm −3 and the resulting extremely large proportion of depletion regions with short depletion widths (<10 nm) in hierarchical structures, charge separation and collection efficiencies could be markedly improved. Moreover, it was found that long-lived charges are generated via excitation by shorter wavelength light (below ∼500 nm), thus enabling long-range hole transfer through the MC network to drive high efficiency of light-to-energy conversion under back illumination. The performance of hematite (α-Fe 2 O 3 ) photoanodes is limited by fast charge recombination. Here, authors develop hematite mesocrystal-based photoanodes with abundant interfacial oxygen vacancies for highly efficient solar water splitting under back illumination.
Hematite (α-Fe O ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretical limit. Here we report thick hematite films (∼1500 nm) constructed by highly ordered and intimately attached hematite mesocrystals (MCs) for highly efficient PEC water oxidation. Due to the formation of abundant interfacial oxygen vacancies yielding a high carrier density of ∼10  cm and the resulting extremely large proportion of depletion regions with short depletion widths (<10 nm) in hierarchical structures, charge separation and collection efficiencies could be markedly improved. Moreover, it was found that long-lived charges are generated via excitation by shorter wavelength light (below ∼500 nm), thus enabling long-range hole transfer through the MC network to drive high efficiency of light-to-energy conversion under back illumination.
Hematite (α-Fe2O3) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretical limit. Here we report thick hematite films (∼1500 nm) constructed by highly ordered and intimately attached hematite mesocrystals (MCs) for highly efficient PEC water oxidation. Due to the formation of abundant interfacial oxygen vacancies yielding a high carrier density of ∼1020 cm−3 and the resulting extremely large proportion of depletion regions with short depletion widths (<10 nm) in hierarchical structures, charge separation and collection efficiencies could be markedly improved. Moreover, it was found that long-lived charges are generated via excitation by shorter wavelength light (below ∼500 nm), thus enabling long-range hole transfer through the MC network to drive high efficiency of light-to-energy conversion under back illumination.
Abstract Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the significant charge recombination, however, the photoelectrochemical (PEC) conversion efficiency of hematite is still far below the theoretical limit. Here we report thick hematite films (∼1500 nm) constructed by highly ordered and intimately attached hematite mesocrystals (MCs) for highly efficient PEC water oxidation. Due to the formation of abundant interfacial oxygen vacancies yielding a high carrier density of ∼10 20  cm −3 and the resulting extremely large proportion of depletion regions with short depletion widths (<10 nm) in hierarchical structures, charge separation and collection efficiencies could be markedly improved. Moreover, it was found that long-lived charges are generated via excitation by shorter wavelength light (below ∼500 nm), thus enabling long-range hole transfer through the MC network to drive high efficiency of light-to-energy conversion under back illumination.
The performance of hematite (α-Fe2O3) photoanodes is limited by fast charge recombination. Here, authors develop hematite mesocrystal-based photoanodes with abundant interfacial oxygen vacancies for highly efficient solar water splitting under back illumination.
ArticleNumber 4832
Author Muto, Shunsuke
Zhang, Zhujun
Tachikawa, Takashi
Sugimoto, Kunihisa
Ohara, Koji
Karimata, Izuru
Nagashima, Hiroki
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  surname: Zhang
  fullname: Zhang, Zhujun
  organization: Department of Chemistry, Graduate School of Science, Kobe University
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  givenname: Izuru
  surname: Karimata
  fullname: Karimata, Izuru
  organization: Department of Chemistry, Graduate School of Science, Kobe University
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  givenname: Hiroki
  orcidid: 0000-0003-1162-6669
  surname: Nagashima
  fullname: Nagashima, Hiroki
  organization: Molecular Photoscience Research Center, Kobe University
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  givenname: Shunsuke
  orcidid: 0000-0001-6275-0649
  surname: Muto
  fullname: Muto, Shunsuke
  organization: Electron Nanoscopy Section, Advanced Measurement Technology Center, Institute of Materials and Systems for Sustainability, Nagoya University, Furo-cho
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  givenname: Koji
  orcidid: 0000-0002-3134-512X
  surname: Ohara
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  organization: Diffraction and Scattering Division, Center for Synchrotron Radiation, Japan Synchrotron Radiation Research Institute
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  givenname: Kunihisa
  orcidid: 0000-0002-0103-8153
  surname: Sugimoto
  fullname: Sugimoto, Kunihisa
  organization: Department of Chemistry, Graduate School of Science, Kobe University, Diffraction and Scattering Division, Center for Synchrotron Radiation, Japan Synchrotron Radiation Research Institute, Institute for Integrated Cell-Material Sciences (iCeMS), Kyoto University, Yoshida-Ushinomiya-cho
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  givenname: Takashi
  orcidid: 0000-0001-6465-5792
  surname: Tachikawa
  fullname: Tachikawa, Takashi
  email: tachikawa@port.kobe-u.ac.jp
  organization: Department of Chemistry, Graduate School of Science, Kobe University, Molecular Photoscience Research Center, Kobe University
BackLink https://www.ncbi.nlm.nih.gov/pubmed/31645549$$D View this record in MEDLINE/PubMed
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SSID ssj0000391844
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Snippet Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the...
Hematite (α-Fe O ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the...
Abstract Hematite (α-Fe 2 O 3 ) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in...
Hematite (α-Fe2O3) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to the difficulty in suppressing the...
The performance of hematite (α-Fe2O3) photoanodes is limited by fast charge recombination. Here, authors develop hematite mesocrystal-based photoanodes with...
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pubmedcentral
proquest
crossref
pubmed
springer
SourceType Open Website
Open Access Repository
Aggregation Database
Index Database
Publisher
StartPage 4832
SubjectTerms 147/137
639/301/299/886
639/638/439/890
639/638/675
Carrier density
Charge efficiency
Depletion
Efficiency
Electrodes
Energy conversion
Energy conversion efficiency
Extreme values
Hematite
Humanities and Social Sciences
Light
multidisciplinary
Nanocrystals
Nanoparticles
Oxidation
Oxygen
Photoanodes
Radiation
Recombination
Science
Science (multidisciplinary)
Structural hierarchy
Thick films
Vacancies
Water splitting
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Title Interfacial oxygen vacancies yielding long-lived holes in hematite mesocrystal-based photoanodes
URI https://link.springer.com/article/10.1038/s41467-019-12581-z
https://www.ncbi.nlm.nih.gov/pubmed/31645549
https://www.proquest.com/docview/2309511174
https://search.proquest.com/docview/2308525259
https://pubmed.ncbi.nlm.nih.gov/PMC6811569
https://doaj.org/article/e8a4528b538d4f50a7a63061090f397b
Volume 10
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