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Published October 7, 2016 | Supplemental Material
Journal Article Open

The role of the CeO_2/BiVO_4 interface in optimized Fe-Ce oxide coatings for solar fuels photoanodes

Abstract

Solar fuel generators entail a high degree of materials integration, and efficient photoelectrocatalysis of the constituent reactions hinges upon the establishment of highly functional interfaces. The recent application of high throughput experimentation to interface discovery for solar fuels photoanodes has revealed several surprising and promising mixed-metal oxide coatings for BiVO_4. Using sputter deposition of composition and thickness gradients on a uniform BiVO_4 film, we systematically explore photoanodic performance as a function of the composition and loading of Fe–Ce oxide coatings. This combinatorial materials integration study not only enhances the performance of this new class of materials but also identifies CeO_2 as a critical ingredient that merits detailed study. A heteroepitaxial CeO_2(001)/BiVO_4(010) interface is identified in which Bi and V remain fully coordinated to O such that no surface states are formed. Ab initio calculations of the integrated materials and inspection of the electronic structure reveals mechanisms by which CeO_2 facilitates charge transport while mitigating deleterious recombination. The results support the observations that addition of Ce to BiVO_4 coatings greatly enhances photoelectrocatalytic activity, providing an important strategy for developing a scalable solar fuels technology.

Additional Information

© 2016 The Royal Society of Chemistry. Received 6th June 2016; Accepted 26th August 2016; First published online 09 Sep 2016. This material 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 U.S. Department of Energy (Award No. DE-SC0004993). A. Shinde, G. Li and L. Zhou contributed equally to this work. The authors thank Ian Sharp for insightful discussions and Xinghao Zhou for assistance with AFM experiments.

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