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DNA for Assembly and Charge Transport Photocatalytic Reduction of CO2

DNA for Assembly and Charge Transport Photocatalytic Reduction of CO2 This report demonstrates the use of DNA to spatially organize photoactive nanocrystals into well‐defined Z‐scheme architectures to facilitate CO2 reduction to usable fuels upon solar irradiation through electron transfer. Coupling donor (Titanium Oxide, TiO2) and acceptor (Cadmium Sulfide, CdS) nanocrystals with DNA yield a 5.25‐fold improvement in CO2 reduction over simply mixing the photocatalysts in solution. In addition, it is demonstrated that electron transfer occurs over distances far greater than those achieved with polyethylene glycol spacer. Efficient Z‐scheme photocatalytic reduction of CO2 is observed for DNA lengths of 10–80 bases, which separate the donor and acceptor nanocrystals by 3–24 nm. More significantly, an interparticle distance of 9–10 nm yields the highest conversion of CO2, which is found for nanocrystals spaced using either linear 30mer double strand DNA (dsDNA) or a 40mer DNA composed of both linear and hairpin DNA. When the amount of 30mer DNA linking the photocatalysts is lowered, a corresponding decrease in CO2 reduction yields is seen, showcasing the role of DNA in mediating electron transfer. These results demonstrate the highly unique attributes of DNA as both a templating agent for precise nanoscale assembly and for enabling charge transport. This work uncovers new research directions for nanoelectronics, electrochemistry, and photocatalysis. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Sustainable Systems Wiley

DNA for Assembly and Charge Transport Photocatalytic Reduction of CO2

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References (86)

Publisher
Wiley
Copyright
© 2018 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim
eISSN
2366-7486
DOI
10.1002/adsu.201700156
Publisher site
See Article on Publisher Site

Abstract

This report demonstrates the use of DNA to spatially organize photoactive nanocrystals into well‐defined Z‐scheme architectures to facilitate CO2 reduction to usable fuels upon solar irradiation through electron transfer. Coupling donor (Titanium Oxide, TiO2) and acceptor (Cadmium Sulfide, CdS) nanocrystals with DNA yield a 5.25‐fold improvement in CO2 reduction over simply mixing the photocatalysts in solution. In addition, it is demonstrated that electron transfer occurs over distances far greater than those achieved with polyethylene glycol spacer. Efficient Z‐scheme photocatalytic reduction of CO2 is observed for DNA lengths of 10–80 bases, which separate the donor and acceptor nanocrystals by 3–24 nm. More significantly, an interparticle distance of 9–10 nm yields the highest conversion of CO2, which is found for nanocrystals spaced using either linear 30mer double strand DNA (dsDNA) or a 40mer DNA composed of both linear and hairpin DNA. When the amount of 30mer DNA linking the photocatalysts is lowered, a corresponding decrease in CO2 reduction yields is seen, showcasing the role of DNA in mediating electron transfer. These results demonstrate the highly unique attributes of DNA as both a templating agent for precise nanoscale assembly and for enabling charge transport. This work uncovers new research directions for nanoelectronics, electrochemistry, and photocatalysis.

Journal

Advanced Sustainable SystemsWiley

Published: Apr 1, 2018

Keywords: ; ; ; ;

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