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Enhanced Bulk Transport in Copper Vanadate Photoanodes Identified by Combinatorial Alloying

Newhouse, Paul F. and Guevarra, Dan and Zhou, Lan and Wang, Yu and Umehara, Mitsutaro and Boyd, David A. and Gregoire, John M. and Haber, Joel A. (2020) Enhanced Bulk Transport in Copper Vanadate Photoanodes Identified by Combinatorial Alloying. Matter, 3 (5). pp. 1601-1613. ISSN 2590-2385. doi:10.1016/j.matt.2020.08.032.

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The impact of alloying on the performance of β-Cu₂V₂O₇ photoanodes was investigated using inkjet printing of composition libraries containing 1,809 Cu₂V₂O₇-based photoanodes. Six elements (Zr, Ca, Hf, Gd, La, and Lu) were alloyed and pairwise co-alloyed at concentrations up to 7 at % into Cu-rich, stoichiometric, and Cu-deficient host Cu₂V₂O₇. A 1.7-fold increase in oxygen evolution photocurrent in pH 9.2 electrolyte was obtained by alloying Ca into β-Cu₂V₂O₇. Experiments employing a hole scavenger to better characterize bulk charge separation and transport revealed a 2.2-fold increase in photoactivity via alloying with Hf, Zr, and La, which increased to 2.7-fold upon co-alloying these elements with Ca. Concurrent with increased photoactivity is substantially decreased photon absorption between 1.5 and 2 eV, a range reported to coincide with high exciton absorption in β-Cu₂V₂O₇, motivating further exploration of whether these co-alloy compositions may destabilize the excitonic state that appears to have limited performance to date.

Item Type:Article
Related URLs:
URLURL TypeDescription
Newhouse, Paul F.0000-0003-2032-3010
Guevarra, Dan0000-0002-9592-3195
Zhou, Lan0000-0002-7052-266X
Wang, Yu0000-0003-3589-9274
Umehara, Mitsutaro0000-0001-8665-0028
Gregoire, John M.0000-0002-2863-5265
Haber, Joel A.0000-0001-7847-5506
Additional Information:© 2020 Elsevier Inc. Received 3 July 2020, Revised 8 August 2020, Accepted 27 August 2020, Available online 1 October 2020. This study is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy (award no. DE-SC0004993). Author Contributions: P.F.N. synthesized and collected optical and PEC data on the libraries and contributed to manuscript preparation. D.G. performed data analysis and visualization of the library data. L.Z. collected and analyzed XRD data. Y.W. collected library PEC data. M.U. analyzed Raman data. D.A.B. collected and analyzed Raman data. J.M.G. designed the library printing strategy and supported the design of analysis algorithms and visualization schemes. J.A.H. facilitated aggregation of results and their interpretation in the context of the literature. J.M.G. and J.A.H. supervised and contributed to manuscript preparation. The authors declare no competing interests.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Issue or Number:5
Record Number:CaltechAUTHORS:20201002-103843089
Persistent URL:
Official Citation:Paul F. Newhouse, Dan Guevarra, Lan Zhou, Yu Wang, Mitsutaro Umehara, David A. Boyd, John M. Gregoire, Joel A. Haber, Enhanced Bulk Transport in Copper Vanadate Photoanodes Identified by Combinatorial Alloying, Matter, Volume 3, Issue 5, 2020, Pages 1601-1613, ISSN 2590-2385, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105755
Deposited By: Tony Diaz
Deposited On:02 Oct 2020 21:00
Last Modified:16 Nov 2021 18:46

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