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  Probing Photocatalytic Nitrogen Reduction to Ammonia with Water on the Rutile TiO2 (110) Surface by First-Principles Calculations

Xie, X.-Y., Xiao, P., Fang, W.-H., Cui, G., & Thiel, W. (2019). Probing Photocatalytic Nitrogen Reduction to Ammonia with Water on the Rutile TiO2 (110) Surface by First-Principles Calculations. ACS Catalysis, 9(10), 9178-9187. doi:10.1021/acscatal.9b01551.

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 Creators:
Xie, Xiao-Ying1, Author
Xiao, Pin1, Author
Fang, Wei-Hai1, Author
Cui, Ganglong1, Author
Thiel, Walter2, Author              
Affiliations:
1Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, People’s Republic of China, ou_persistent22              
2Research Department Thiel, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445590              

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Free keywords: photocatalysis; nitrogen fixation; TiO2; DFT; oxygen vacancy; hydroxyl group
 Abstract: Photocatalytic ammonia production from air and water under ambient conditions is ideally suited for artificial nitrogen fixation. It has been the subject of several recent experimental studies with titanium dioxide and titania-based semiconductors as catalysts. The TiO2-mediated photocatalytic NH3 production from H2O and N2 is a very complex process that is not yet well understood mechanistically, which hampers further advances. In the present work, we address the detailed mechanism of N2 reduction to NH3 driven by the photolysis of water adsorbed on the rutile TiO2 (110) surface containing oxygen vacancies, by means of reliable density functional calculations (HSE06+D3//PBE+U+D3). We show that each major step of the reaction is driven by H2O photolysis and can proceed under ambient conditions. The initial N2 adsorption, the activation of the inert N≡N bond, and the N–N cleavage are all efficiently promoted by TiO2 surface hydroxylation and photogenerated electrons, as well as their synergistic effects, while proton-coupled electron transfers play a decisive role in the N2 reduction to NH3. These mechanistic insights can probably guide further experimental studies of TiO2 photocatalytic nitrogen fixation and NH3 photosynthesis.

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Language(s): eng - English
 Dates: 2019-04-162019-08-292019-10-04
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.9b01551
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 9 (10) Sequence Number: - Start / End Page: 9178 - 9187 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435