Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments
Abstract
The solar photoelectrochemical generation of hydrogen and carbon-containing fuels comprises a critical energy technology for establishing sustainable energy resources. The photoanode, which is responsible for solar-driven oxygen evolution, has persistently limited technology advancement due to the lack of materials that exhibit both the requisite electronic properties and operational stability. Efforts to extend the lifetime of solar fuel devices increasingly focus on mitigating corrosion in the highly oxidizing oxygen evolution environment, motivating our development of a photoanode discovery pipeline that combines electronic structure calculations, Pourbaix stability screening, and high-throughput experiments. By applying the pipeline to ternary metal oxides containing manganese, we identify a promising class of corrosion-resistant materials and discover five oxygen evolution photoanodes, including the first demonstration of photoelectrocatalysis with Mn-based ternary oxides and the introduction of alkaline earth manganates as promising photoanodes for establishing a durable solar fuels technology.
Additional Information
© 2017 American Chemical Society. Received: July 10, 2017; Accepted: September 7, 2017; Published: September 7, 2017. 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 under Award Number DE-SC0004993. Computational work was additionally supported by the Materials Project (Grant No. EDCBEE) through the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC02-05CH11231. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. DOE under Contract DE-AC02-05CH11231. Computational resources were also provided by the DOE through the National Energy Supercomputing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract DE-AC02-05CH11231. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The authors declare no competing financial interest.Attached Files
Supplemental Material - nz7b00607_si_001.pdf
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Additional details
- Eprint ID
- 81445
- Resolver ID
- CaltechAUTHORS:20170914-131954119
- Department of Energy (DOE)
- DE-SC0004993
- Department of Energy (DOE)
- DE-AC02-05CH11231
- Department of Energy (DOE)
- DE-AC02-76SF00515
- Created
-
2017-09-14Created from EPrint's datestamp field
- Updated
-
2021-11-15Created from EPrint's last_modified field
- Caltech groups
- JCAP