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Hole extraction by design in photocatalytic architectures interfacing CdSe quantum dots with topochemically stabilized tin vanadium oxide
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Andrews, Justin L., Cho, Junsang, Wangoh, Linda, Suwandaratne, Nuwanthi, Sheng, Aaron, Chauhan, Saurabh, Nieto, Kelly, Mohr, Alec, Kadassery, Karthika J., Popeil, Melissa R., Thakur, Pardeep K., Sfeir, Matthew, Lacy, David C., Lee, Tien-Lin, Zhang, Peihong, Watson, David F., Piper, Louis F. J. and Banerjee, Sarbajit (2018) Hole extraction by design in photocatalytic architectures interfacing CdSe quantum dots with topochemically stabilized tin vanadium oxide. Journal of the American Chemical Society, 140 (49). pp. 17163-17174. doi:10.1021/jacs.8b09924 ISSN 0002-7863.
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Official URL: http://dx.doi.org/10.1021/jacs.8b09924
Abstract
Tackling the complex challenge of harvesting solar energy to generate energy-dense fuels such as hydrogen requires the design of photocatalytic nanoarchitectures interfacing components that synergistically mediate a closely interlinked sequence of light-harvesting, charge separation, charge/mass transport, and catalytic processes. The design of such architectures requires careful consideration of both thermodynamic offsets and interfacial charge-transfer kinetics to ensure long-lived charge carriers that can be delivered at low overpotentials to the appropriate catalytic sites while mitigating parasitic reactions such as photocorrosion. Here we detail the theory-guided design and synthesis of nanowire/quantum dot heterostructures with interfacial electronic structure specifically tailored to promote light-induced charge separation and photocatalytic proton reduction. Topochemical synthesis yields a metastable β-Sn0.23V2O5 compound exhibiting Sn 5s-derived midgap states ideally positioned to extract photogenerated holes from interfaced CdSe quantum dots. The existence of these midgap states near the upper edge of the valence band (VB) has been confirmed, and β-Sn0.23V2O5/CdSe heterostructures have been shown to exhibit a 0 eV midgap state-VB offset, which underpins ultrafast subpicosecond hole transfer. The β-Sn0.23V2O5/CdSe heterostructures are further shown to be viable photocatalytic architectures capable of efficacious hydrogen evolution. The results of this study underscore the criticality of precisely tailoring the electronic structure of semiconductor components to effect rapid charge separation necessary for photocatalysis.
Item Type: | Journal Article | ||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) | ||||||
Journal or Publication Title: | Journal of the American Chemical Society | ||||||
Publisher: | ACS Publications | ||||||
ISSN: | 0002-7863 | ||||||
Official Date: | 1 November 2018 | ||||||
Dates: |
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Volume: | 140 | ||||||
Number: | 49 | ||||||
Page Range: | pp. 17163-17174 | ||||||
DOI: | 10.1021/jacs.8b09924 | ||||||
Status: | Peer Reviewed | ||||||
Publication Status: | Published | ||||||
Access rights to Published version: | Restricted or Subscription Access |
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