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Thermally Stable N_2-Intercalated WO_3 Photoanodes for Water Oxidation

Mi, Qixi and Ping, Yuan and Li, Yan and Cao, Bingfei and Brunschwig, Bruce S. and Khalifah, Peter G. and Galli, Giulia A. and Gray, Harry B. and Lewis, Nathan S. (2012) Thermally Stable N_2-Intercalated WO_3 Photoanodes for Water Oxidation. Journal of the American Chemical Society, 134 (44). pp. 18318-18324. ISSN 0002-7863. http://resolver.caltech.edu/CaltechAUTHORS:20130212-095922217

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Abstract

We describe stable intercalation compounds of the composition xN_2•WO_3 (x = 0.034–0.039), formed by trapping N_2 in WO_3. The incorporation of N_2 significantly reduced the absorption threshold of WO_3; notably, 0.039N_2•WO_3 anodes exhibited photocurrent under illumination at wavelengths ≤640 nm with a faradaic efficiency for O_2 evolution in 1.0 M HClO_4(aq) of nearly unity. Spectroscopic and computational results indicated that deformation of the WO3 host lattice, as well as weak electronic interactions between trapped N_2 and the WO_3 matrix, contributed to the observed red shift in optical absorption. Noble-gas-intercalated WO_3 materials similar to xN_2•WO_3 are predicted to function as photoanodes that are responsive to visible light.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja3067622 DOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja3067622PublisherArticle
ORCID:
AuthorORCID
Brunschwig, Bruce S.0000-0002-6135-6727
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2012 American Chemical Society. Received: July 14, 2012. Published: September 28, 2012. We thank Prof. George R. Rossman for discussions and for assistance with the Raman microscope, and Prof. Francois Gygi for discussions of ab initio calculations. This work was supported by the National Science Foundation (NSF) Powering the Planet Center for Chemical Innovation (CCISolar), Grants CHE-0802907 and CHE-0947829. Q.M. was a CCI-Solar Postdoctoral Fellow. P.G.K. thanks the support of the U.S. Department of Energy under the Hydrogen Fuel Initiative. Research was in part carried out in the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology, and in part carried out at Brookhaven National Laboratory under No. DE-AC02-98CH10886 with the U.S. Department of Energy. Use of the Teragrid computational facilities is gratefully acknowledged.
Group:CCI Solar Fuels
Funders:
Funding AgencyGrant Number
NSFCHE-0802907
NSFCHE-0947829
NSF Postdoctoral FellowshipUNSPECIFIED
Department of Energy (DOE)DE-AC02-98CH10886
Record Number:CaltechAUTHORS:20130212-095922217
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20130212-095922217
Official Citation:Thermally Stable N2-Intercalated WO3 Photoanodes for Water Oxidation Qixi Mi, Yuan Ping, Yan Li, Bingfei Cao, Bruce S. Brunschwig, Peter G. Khalifah, Giulia A. Galli, Harry B. Gray, and Nathan S. Lewis Journal of the American Chemical Society 2012 134 (44), 18318-18324
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:36870
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:23 Feb 2013 00:05
Last Modified:02 Feb 2017 22:42

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