Title: Solar fuels photoanode materials discovery by integrating high-throughput theory and experiment

Abstract

The limited number of known low-band-gap photoelectrocatalytic materials poses a significant challenge for the generation of chemical fuels from sunlight. Here, using high-throughput ab initio theory with experiments in an integrated workflow, we find eight ternary vanadate oxide photoanodes in the target band-gap range (1.2-2.8 eV). Detailed analysis of these vanadate compounds reveals the key role of VO₄ structural motifs and electronic band-edge character in efficient photoanodes, initiating a genome for such materials and paving the way for a broadly applicable high-throughput-discovery and materials-by-design feedback loop. Considerably expanding the number of known photoelectrocatalysts for water oxidation, our study establishes ternary metal vanadates as a prolific class of photoanodematerials for generation of chemical fuels from sunlight and demonstrates our high-throughput theory-experiment pipeline as a prolific approach to materials discovery.

Authors:

Yan, Qimin ^[1]; Yu, Jie ^[2]; Suram, Santosh K. ^[3]; Zhou, Lan ^[3]; Shinde, Aniketa ^[3]; Newhouse, Paul F. ^[3]; Chen, Wei ^[4]; Li, Guo ^[5]; Persson, Kristin A. ^[6]; Gregoire, John M. ^[3]; Neaton, Jeffrey B. ^[7]

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+ Show Author Affiliations

1. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Physics, University of California, Berkeley, CA 94720,
2. Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, CA 91125,, Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
3. Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, CA 91125,
4. Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
5. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Physics, University of California, Berkeley, CA 94720,, Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,
6. Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Materials Science and Engineering, University of California, Berkeley, CA 94720,
7. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Department of Physics, University of California, Berkeley, CA 94720,, Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720,, Kavli Energy NanoSciences Institute at Berkeley, Berkeley, CA 94720

Publication Date:

Mon Mar 06 00:00:00 EST 2017

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1345845

Alternate Identifier(s):

OSTI ID: 1409431

Grant/Contract Number:  

AC02-05CH11231; SC0004993

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 12; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; photocatalysis; solar fuels materials; density-functional theory; high-throughput experiments; complex oxides