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Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction

The photocatalytic reduction of N to NH is typically hampered by poor binding of N to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such... Full description

Journal Title: Nature Materials Sep 2013, Vol.12(9), pp.836-41
Main Author: Zhu, Di
Other Authors: Zhang, Linghong , Ruther, Rose , Hamers, Robert
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: ISSN: 14761122 ; DOI: 10.1038/nmat3696
Link: http://search.proquest.com/docview/1441322635/?pq-origsite=primo
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title: Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction
format: Article
creator:
  • Zhu, Di
  • Zhang, Linghong
  • Ruther, Rose
  • Hamers, Robert
subjects:
  • Ammonia–Chemistry
  • Diamond–Chemistry
  • Electrons–Chemistry
  • Nitrogen–Chemistry
  • Oxidation-Reduction–Chemistry
  • Photochemical Processes–Chemistry
  • Water–Chemistry
  • Photocatalysis
  • Catalysts
  • Materials Science
  • Diamonds
  • Water
  • Ammonia
  • Diamond
  • Nitrogen
ispartof: Nature Materials, Sep 2013, Vol.12(9), pp.836-41
description: The photocatalytic reduction of N to NH is typically hampered by poor binding of N to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N to NH at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface. [PUBLICATION ]
language: eng
source:
identifier: ISSN: 14761122 ; DOI: 10.1038/nmat3696
fulltext: fulltext
issn:
  • 14761122
  • 1476-1122
url: Link


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titlePhoto-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction
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ispartofNature Materials, Sep 2013, Vol.12(9), pp.836-41
identifierISSN: 14761122 ; DOI: 10.1038/nmat3696
subjectAmmonia–Chemistry ; Diamond–Chemistry ; Electrons–Chemistry ; Nitrogen–Chemistry ; Oxidation-Reduction–Chemistry ; Photochemical Processes–Chemistry ; Water–Chemistry ; Photocatalysis ; Catalysts ; Materials Science ; Diamonds ; Water ; Ammonia ; Diamond ; Nitrogen
descriptionThe photocatalytic reduction of N to NH is typically hampered by poor binding of N to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N to NH at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface. [PUBLICATION ]
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descriptionThe photocatalytic reduction of N to NH is typically hampered by poor binding of N to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N to NH at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface. [PUBLICATION ]
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titlePhoto-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction
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abstractThe photocatalytic reduction of N to NH is typically hampered by poor binding of N to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N to NH at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface. [PUBLICATION ABSTRACT]
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