Homogeneously dispersed multimetal oxygen-evolving catalysts
Abstract
Earth-abundant first-row (3d) transition-metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials significantly above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing near-optimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxy-hydroxide materials with an atomically homogeneous metal distribution. These gelled FeCoW oxy-hydroxide exhibits the lowest overpotential (191 mV) reported at 10 mA per square centimeter in alkaline electrolyte. Here, the catalyst shows no evidence of degradation following more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between W, Fe and Co in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.
- Authors:
- more »
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1355859
- Alternate Identifier(s):
- OSTI ID: 1245398; OSTI ID: 1248381
- Report Number(s):
- BNL-111992-2016-JA
Journal ID: ISSN 0036-8075; science.aaf1525
- Grant/Contract Number:
- SC0012704; AC02-76SF00515
- Resource Type:
- Published Article
- Journal Name:
- Science
- Additional Journal Information:
- Journal Name: Science Journal Volume: 352 Journal Issue: 6283; Journal ID: ISSN 0036-8075
- Publisher:
- American Association for the Advancement of Science (AAAS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Zhang, B., Zheng, X., Voznyy, O., Comin, R., Bajdich, M., Garcia-Melchor, M., Han, L., Xu, J., Liu, M., Zheng, L., Garcia de Arquer, F. P., Dinh, C. T., Fan, F., Yuan, M., Yassitepe, E., Chen, N., Regier, T., Liu, P., Li, Y., De Luna, P., Janmohamed, A., Xin, H. L., Yang, H., Vojvodic, A., and Sargent, E. H. Homogeneously dispersed multimetal oxygen-evolving catalysts. United States: N. p., 2016.
Web. doi:10.1126/science.aaf1525.
Zhang, B., Zheng, X., Voznyy, O., Comin, R., Bajdich, M., Garcia-Melchor, M., Han, L., Xu, J., Liu, M., Zheng, L., Garcia de Arquer, F. P., Dinh, C. T., Fan, F., Yuan, M., Yassitepe, E., Chen, N., Regier, T., Liu, P., Li, Y., De Luna, P., Janmohamed, A., Xin, H. L., Yang, H., Vojvodic, A., & Sargent, E. H. Homogeneously dispersed multimetal oxygen-evolving catalysts. United States. https://doi.org/10.1126/science.aaf1525
Zhang, B., Zheng, X., Voznyy, O., Comin, R., Bajdich, M., Garcia-Melchor, M., Han, L., Xu, J., Liu, M., Zheng, L., Garcia de Arquer, F. P., Dinh, C. T., Fan, F., Yuan, M., Yassitepe, E., Chen, N., Regier, T., Liu, P., Li, Y., De Luna, P., Janmohamed, A., Xin, H. L., Yang, H., Vojvodic, A., and Sargent, E. H. Thu .
"Homogeneously dispersed multimetal oxygen-evolving catalysts". United States. https://doi.org/10.1126/science.aaf1525.
@article{osti_1355859,
title = {Homogeneously dispersed multimetal oxygen-evolving catalysts},
author = {Zhang, B. and Zheng, X. and Voznyy, O. and Comin, R. and Bajdich, M. and Garcia-Melchor, M. and Han, L. and Xu, J. and Liu, M. and Zheng, L. and Garcia de Arquer, F. P. and Dinh, C. T. and Fan, F. and Yuan, M. and Yassitepe, E. and Chen, N. and Regier, T. and Liu, P. and Li, Y. and De Luna, P. and Janmohamed, A. and Xin, H. L. and Yang, H. and Vojvodic, A. and Sargent, E. H.},
abstractNote = {Earth-abundant first-row (3d) transition-metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials significantly above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing near-optimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxy-hydroxide materials with an atomically homogeneous metal distribution. These gelled FeCoW oxy-hydroxide exhibits the lowest overpotential (191 mV) reported at 10 mA per square centimeter in alkaline electrolyte. Here, the catalyst shows no evidence of degradation following more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between W, Fe and Co in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.},
doi = {10.1126/science.aaf1525},
journal = {Science},
number = 6283,
volume = 352,
place = {United States},
year = {Thu Mar 24 00:00:00 EDT 2016},
month = {Thu Mar 24 00:00:00 EDT 2016}
}
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