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Title: DNA for Assembly and Charge Transport Photocatalytic Reduction of CO 2

Abstract

Abstract This report demonstrates the use of DNA to spatially organize photoactive nanocrystals into well‐defined Z‐scheme architectures to facilitate CO 2 reduction to usable fuels upon solar irradiation through electron transfer. Coupling donor (Titanium Oxide, TiO 2 ) and acceptor (Cadmium Sulfide, CdS) nanocrystals with DNA yield a 5.25‐fold improvement in CO 2 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 CO 2 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 CO 2 , 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 CO 2 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.more » This work uncovers new research directions for nanoelectronics, electrochemistry, and photocatalysis.« less

Authors:
 [1];  [1];  [1];  [2]
+ Show Author Affiliations
  1. Department of Chemical and Biological Engineering University of Colorado Boulder CO 80309‐0596 USA
  2. Department of Chemical and Biological Engineering University of Colorado Boulder CO 80309‐0596 USA, Materials Science and Engineering Program University of Colorado Boulder CO 80309‐0596 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1423701
Grant/Contract Number:  
DE‐SC0006398
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Advanced Sustainable Systems
Additional Journal Information:
Journal Name: Advanced Sustainable Systems Journal Volume: 2 Journal Issue: 4; Journal ID: ISSN 2366-7486
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Ma, Ke, Yehezkeli, Omer, He, Liangcan, and Cha, Jennifer N. DNA for Assembly and Charge Transport Photocatalytic Reduction of CO 2. Germany: N. p., 2018. Web. doi:10.1002/adsu.201700156.
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Ma, Ke, Yehezkeli, Omer, He, Liangcan, & Cha, Jennifer N. DNA for Assembly and Charge Transport Photocatalytic Reduction of CO 2. Germany. https://doi.org/10.1002/adsu.201700156
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Ma, Ke, Yehezkeli, Omer, He, Liangcan, and Cha, Jennifer N. Mon . "DNA for Assembly and Charge Transport Photocatalytic Reduction of CO 2". Germany. https://doi.org/10.1002/adsu.201700156.
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@article{osti_1423701,
title = {DNA for Assembly and Charge Transport Photocatalytic Reduction of CO 2},
author = {Ma, Ke and Yehezkeli, Omer and He, Liangcan and Cha, Jennifer N.},
abstractNote = {Abstract This report demonstrates the use of DNA to spatially organize photoactive nanocrystals into well‐defined Z‐scheme architectures to facilitate CO 2 reduction to usable fuels upon solar irradiation through electron transfer. Coupling donor (Titanium Oxide, TiO 2 ) and acceptor (Cadmium Sulfide, CdS) nanocrystals with DNA yield a 5.25‐fold improvement in CO 2 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 CO 2 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 CO 2 , 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 CO 2 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.},
doi = {10.1002/adsu.201700156},
journal = {Advanced Sustainable Systems},
number = 4,
volume = 2,
place = {Germany},
year = {Mon Mar 05 00:00:00 EST 2018},
month = {Mon Mar 05 00:00:00 EST 2018}
}
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https://doi.org/10.1002/adsu.201700156
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