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Title: 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 have identified 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.

Authors:
 [1]; ORCiD logo [1];  [2];  [1];  [3];  [4];  [5];  [6]; ORCiD logo [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Temple Univ., Philadelphia, PA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  4. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Temple Univ., Philadelphia, PA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division and Joint Center for Artificial Photosynthesis (JCAP)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry and Joint Center for Artificial Photosynthesis (JCAP); Univ. of California, Berkeley, CA (United States). Kavli Energy NanoSciences Inst. and Dept. of Physics
Publication Date:
Research Org.:
California Inst. of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Contributing Org.:
[SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)]
OSTI Identifier:
1468640
Alternate Identifier(s):
OSTI ID: 1476554
Grant/Contract Number:  
[SC0004993; EDCBEE; AC02-05CH11231; AC02-76SF00515]
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
[ Journal Volume: 2; Journal Issue: 10]; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
10 SYNTHETIC FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Shinde, Aniketa, Suram, Santosh K., Yan, Qimin, Zhou, Lan, Singh, Arunima K., Yu, Jie, Persson, Kristin A., Neaton, Jeffrey B., and Gregoire, John M. Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments. United States: N. p., 2017. Web. doi:10.1021/acsenergylett.7b00607.
Shinde, Aniketa, Suram, Santosh K., Yan, Qimin, Zhou, Lan, Singh, Arunima K., Yu, Jie, Persson, Kristin A., Neaton, Jeffrey B., & Gregoire, John M. Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments. United States. doi:10.1021/acsenergylett.7b00607.
Shinde, Aniketa, Suram, Santosh K., Yan, Qimin, Zhou, Lan, Singh, Arunima K., Yu, Jie, Persson, Kristin A., Neaton, Jeffrey B., and Gregoire, John M. Thu . "Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments". United States. doi:10.1021/acsenergylett.7b00607. https://www.osti.gov/servlets/purl/1468640.
@article{osti_1468640,
title = {Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments},
author = {Shinde, Aniketa and Suram, Santosh K. and Yan, Qimin and Zhou, Lan and Singh, Arunima K. and Yu, Jie and Persson, Kristin A. and Neaton, Jeffrey B. and Gregoire, John M.},
abstractNote = {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 have identified 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.},
doi = {10.1021/acsenergylett.7b00607},
journal = {ACS Energy Letters},
number = [10],
volume = [2],
place = {United States},
year = {2017},
month = {9}
}

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Figures / Tables:

Figure 1 Figure 1: Tiered screening pipeline for accelerated discovery of solar fuels photoanodes. The number of compounds (bold) and screening criteria used in this study for the seven-tier pipeline that integrates database mining (gray), high throughput computational screening (blue), and high throughput experimental screening (yellow).

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.