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A computational study of the competing reaction mechanisms of the photo-catalytic reduction of CO2 on anatase(101)
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Ip, Chung Man and Troisi, Alessandro (2016) A computational study of the competing reaction mechanisms of the photo-catalytic reduction of CO2 on anatase(101). Physical Chemistry Chemical Physics, 18 (36). pp. 25010-25021. doi:10.1039/C6CP02642G ISSN 1463-9076.
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WRAP_0483109-ch-141116-photo_co2.pdf - Accepted Version - Requires a PDF viewer. Download (1419Kb) |
Official URL: http://dx.doi.org/10.1039/C6CP02642G
Abstract
We perform a computational study of three different reaction mechanisms for the photo-catalytic reduction of CO2 on the TiO2 anatase(101) surface known as (i) the carbene, (ii) the formaldehyde and (iii) the glyoxal pathways. We define a set of approximations that allows testing a number of mechanistic hypotheses and design experiments to validate them. We find that the energetically most favourable reaction mechanism among those proposed in the literature is the formaldehyde path, and the rate-limiting step is likely to be the formation of CH3 radicals from dissociation of CH3OH. We show that an intermediate that supports this mechanism is OCH2OH. We also find that formaldehyde would be an energetically favorable intermediate forming from CO and HCO, intermediates that are proposed in the early stage of the carbene and glyoxal pathways respectively. Some possible variants of mechanisms and methods to ease the formation of CH3 radicals are also discussed.
Item Type: | Journal Article | ||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TJ Mechanical engineering and machinery |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||
Library of Congress Subject Headings (LCSH): | Photocatalysis, Solar energy, Carbon dioxide, Methane | ||||||||||
Journal or Publication Title: | Physical Chemistry Chemical Physics | ||||||||||
Publisher: | Royal Society of Chemistry | ||||||||||
ISSN: | 1463-9076 | ||||||||||
Official Date: | 28 September 2016 | ||||||||||
Dates: |
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Volume: | 18 | ||||||||||
Number: | 36 | ||||||||||
Page Range: | pp. 25010-25021 | ||||||||||
DOI: | 10.1039/C6CP02642G | ||||||||||
Status: | Peer Reviewed | ||||||||||
Publication Status: | Published | ||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||
Date of first compliant deposit: | 16 November 2016 | ||||||||||
Date of first compliant Open Access: | 12 August 2017 | ||||||||||
Funder: | Engineering and Physical Sciences Research Council (EPSRC), European Research Council (ERC) |
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