Sunlight-Driven Hydrogen Peroxide Production from Water and Molecular Oxygen by Metal-Free Photocatalysts
Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2O2) is a very important subject. Early reported processes, however, require hydrogen (H2) and palladium‐based catalysts. Herein we propose a photocatalytic process for H2O2 synthesis driven by metal‐free catalys...
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| Published in | Angewandte Chemie International Edition Vol. 53; no. 49; pp. 13454 - 13459 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Weinheim
WILEY-VCH Verlag
01.12.2014
WILEY‐VCH Verlag Wiley Subscription Services, Inc |
| Edition | International ed. in English |
| Subjects | |
| Online Access | Get full text |
| ISSN | 1433-7851 1521-3773 1521-3773 |
| DOI | 10.1002/anie.201407938 |
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| Abstract | Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2O2) is a very important subject. Early reported processes, however, require hydrogen (H2) and palladium‐based catalysts. Herein we propose a photocatalytic process for H2O2 synthesis driven by metal‐free catalysts with earth‐abundant water and molecular oxygen (O2) as resources under sunlight irradiation (λ>400 nm). We use graphitic carbon nitride (g‐C3N4) containing electron‐deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence‐band potential of the catalysts, while maintaining sufficient conduction‐band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2O2 by oxidation of water by the photoformed valence‐band holes and selective two‐electron reduction of O2 by the conduction band electrons.
Peroxide made by sunbathing: Sunlight irradiation (λ>400 nm) of graphitic carbon nitride (g‐C3N4) containing electron‐deficient aromatic diimide units successfully produces H2O2 from water and O2. This metal‐free H2O2 synthesis is driven by oxidation of water by the photoformed valence‐band holes and selective two‐electron reduction of O2 by the conduction‐band electrons. |
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| AbstractList | Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H sub(2)O sub(2)) is a very important subject. Early reported processes, however, require hydrogen (H sub(2)) and palladium-based catalysts. Herein we propose a photocatalytic process for H sub(2)O sub(2) synthesis driven by metal-free catalysts with earth-abundant water and molecular oxygen (O sub(2)) as resources under sunlight irradiation ( lambda >400nm). We use graphitic carbon nitride (g-C sub(3)N sub(4)) containing electron-deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence-band potential of the catalysts, while maintaining sufficient conduction-band potential for O sub(2) reduction. Visible light irradiation of the catalysts in pure water with O sub(2) successfully produces H sub(2)O sub(2) by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O sub(2) by the conduction band electrons. Peroxide made by sunbathing: Sunlight irradiation ( lambda >400nm) of graphitic carbon nitride (g-C sub(3)N sub(4)) containing electron-deficient aromatic diimide units successfully produces H sub(2)O sub(2) from water and O sub(2). This metal-free H sub(2)O sub(2) synthesis is driven by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O sub(2) by the conduction-band electrons. Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H 2 O 2 ) is a very important subject. Early reported processes, however, require hydrogen (H 2 ) and palladium‐based catalysts. Herein we propose a photocatalytic process for H 2 O 2 synthesis driven by metal‐free catalysts with earth‐abundant water and molecular oxygen (O 2 ) as resources under sunlight irradiation ( λ >400 nm). We use graphitic carbon nitride (g‐C 3 N 4 ) containing electron‐deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence‐band potential of the catalysts, while maintaining sufficient conduction‐band potential for O 2 reduction. Visible light irradiation of the catalysts in pure water with O 2 successfully produces H 2 O 2 by oxidation of water by the photoformed valence‐band holes and selective two‐electron reduction of O 2 by the conduction band electrons. Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2 O2 ) is a very important subject. Early reported processes, however, require hydrogen (H2 ) and palladium-based catalysts. Herein we propose a photocatalytic process for H2 O2 synthesis driven by metal-free catalysts with earth-abundant water and molecular oxygen (O2 ) as resources under sunlight irradiation (λ>400 nm). We use graphitic carbon nitride (g-C3 N4 ) containing electron-deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence-band potential of the catalysts, while maintaining sufficient conduction-band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2 O2 by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O2 by the conduction band electrons.Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2 O2 ) is a very important subject. Early reported processes, however, require hydrogen (H2 ) and palladium-based catalysts. Herein we propose a photocatalytic process for H2 O2 synthesis driven by metal-free catalysts with earth-abundant water and molecular oxygen (O2 ) as resources under sunlight irradiation (λ>400 nm). We use graphitic carbon nitride (g-C3 N4 ) containing electron-deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence-band potential of the catalysts, while maintaining sufficient conduction-band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2 O2 by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O2 by the conduction band electrons. Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2O2) is a very important subject. Early reported processes, however, require hydrogen (H2) and palladium-based catalysts. Herein we propose a photocatalytic process for H2O2 synthesis driven by metal-free catalysts with earth-abundant water and molecular oxygen (O2) as resources under sunlight irradiation (λ>400nm). We use graphitic carbon nitride (g-C3N4) containing electron-deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence-band potential of the catalysts, while maintaining sufficient conduction-band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2O2 by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O2 by the conduction band electrons. Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2 O2 ) is a very important subject. Early reported processes, however, require hydrogen (H2 ) and palladium-based catalysts. Herein we propose a photocatalytic process for H2 O2 synthesis driven by metal-free catalysts with earth-abundant water and molecular oxygen (O2 ) as resources under sunlight irradiation (λ>400 nm). We use graphitic carbon nitride (g-C3 N4 ) containing electron-deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence-band potential of the catalysts, while maintaining sufficient conduction-band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2 O2 by oxidation of water by the photoformed valence-band holes and selective two-electron reduction of O2 by the conduction band electrons. Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2O2) is a very important subject. Early reported processes, however, require hydrogen (H2) and palladium‐based catalysts. Herein we propose a photocatalytic process for H2O2 synthesis driven by metal‐free catalysts with earth‐abundant water and molecular oxygen (O2) as resources under sunlight irradiation (λ>400 nm). We use graphitic carbon nitride (g‐C3N4) containing electron‐deficient aromatic diimide units as catalysts. Incorporating the diimide units positively shifts the valence‐band potential of the catalysts, while maintaining sufficient conduction‐band potential for O2 reduction. Visible light irradiation of the catalysts in pure water with O2 successfully produces H2O2 by oxidation of water by the photoformed valence‐band holes and selective two‐electron reduction of O2 by the conduction band electrons. Peroxide made by sunbathing: Sunlight irradiation (λ>400 nm) of graphitic carbon nitride (g‐C3N4) containing electron‐deficient aromatic diimide units successfully produces H2O2 from water and O2. This metal‐free H2O2 synthesis is driven by oxidation of water by the photoformed valence‐band holes and selective two‐electron reduction of O2 by the conduction‐band electrons. |
| Author | Sakamoto, Hirokatsu Kanazawa, Shunsuke Tanaka, Shunsuke Shiraishi, Yasuhiro Ichikawa, Satoshi Hirai, Takayuki Kofuji, Yusuke |
| Author_xml | – sequence: 1 givenname: Yasuhiro surname: Shiraishi fullname: Shiraishi, Yasuhiro email: shiraish@cheng.es.osaka-u.ac.jp organization: Research Center for Solar Energy Chemistry, and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531 (Japan) – sequence: 2 givenname: Shunsuke surname: Kanazawa fullname: Kanazawa, Shunsuke organization: Research Center for Solar Energy Chemistry, and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531 (Japan) – sequence: 3 givenname: Yusuke surname: Kofuji fullname: Kofuji, Yusuke organization: Research Center for Solar Energy Chemistry, and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531 (Japan) – sequence: 4 givenname: Hirokatsu surname: Sakamoto fullname: Sakamoto, Hirokatsu organization: Research Center for Solar Energy Chemistry, and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531 (Japan) – sequence: 5 givenname: Satoshi surname: Ichikawa fullname: Ichikawa, Satoshi organization: Institute for NanoScience Design, Osaka University (Japan) – sequence: 6 givenname: Shunsuke surname: Tanaka fullname: Tanaka, Shunsuke organization: Department of Chemical, Energy and Environmental Engineering, Kansai University (Japan) – sequence: 7 givenname: Takayuki surname: Hirai fullname: Hirai, Takayuki organization: Research Center for Solar Energy Chemistry, and Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531 (Japan) |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/25293501$$D View this record in MEDLINE/PubMed |
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| CODEN | ACIEAY |
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| Keywords | photocatalysis oxygen water graphitic carbon nitride hydrogen peroxide |
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| Snippet | Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2O2) is a very important subject. Early reported processes, however,... Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H 2 O 2 ) is a very important subject. Early reported processes,... Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H2 O2 ) is a very important subject. Early reported processes, however,... Design of green, safe, and sustainable process for the synthesis of hydrogen peroxide (H sub(2)O sub(2)) is a very important subject. Early reported processes,... |
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| SubjectTerms | Carbon nitride Catalysis Catalysts Diimide graphitic carbon nitride Hydrogen peroxide Irradiation Oxidation Oxygen Palladium photocatalysis Reduction Sunlight Synthesis water |
| Title | Sunlight-Driven Hydrogen Peroxide Production from Water and Molecular Oxygen by Metal-Free Photocatalysts |
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