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Title: A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction

Abstract

The efficiency of sunlight-driven reduction of carbon dioxide (CO2), a process mimicking the photosynthesis in nature that integrates the light harvester and electrolysis cell to convert CO2 into valuable chemicals, is greatly limited by the sluggish kinetics of oxygen evolution in pH-neutral conditions. Current non-noble metal oxide catalysts developed to drive oxygen evolution in alkaline solution have poor performance in neutral solutions. Here we report a highly active and stable oxygen evolution catalyst in neutral pH, Brownmillerite Sr2GaCoO5, with the specific activity about one order of magnitude higher than that of widely used iridium oxide catalyst. Using Sr2GaCoO5 to catalyze oxygen evolution, the integrated CO2 reduction achieves the average solar-to-CO efficiency of 13.9% with no appreciable performance degradation in 19h of operation. Our results not only set a record for the efficiency in sunlight-driven CO2 reduction, but open new opportunities towards the realization of practical CO2 reduction systems.

Authors:
 [1];  [1]; ORCiD logo [2];  [3];  [4];  [1]; ORCiD logo [5];  [1];  [1];  [2]; ORCiD logo [6];  [7]; ORCiD logo [8]; ORCiD logo [1]
  1. Toyota Research Inst. of North America, Ann Arbor, MI (United States)
  2. Binghamton Univ., NY (United States)
  3. Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
  4. Enli Technology Co. Ltd., Kaohsiung City (Taiwan)
  5. Univ., of Houston, TX (United States). Texas Center for Superconductivity and Dept. of Physics
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  7. Univ. of Houston, TX (United States). Texas Center for Superconductivity and Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  8. Univ. of Houston, TX (United States). Texas Center for Superconductivity (TcSUH)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES); U.S. Air Force Office of Scientific Research; Scialog
OSTI Identifier:
1638489
Report Number(s):
PNNL-SA-146421
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830; SC0012583; FA9550-15-1-0236; 25751
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Atomistic models; catalyst synthesis; electrocatalysis; solar fuels

Citation Formats

Zhou, Li Qin, Ling, Chen, Zhou, Hui, Wang, Xiang, Liao, Joseph, Reddy, Gunugunuri K., Deng, Liangzi, Peck, Torin C., Zhang, Ruigang, Whittingham, M. Stanley, Wang, Chongmin, Chu, Ching-Wu, Yao, Yan, and Jia, Hongfei. A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction. United States: N. p., 2019. Web. https://doi.org/10.1038/s41467-019-12009-8.
Zhou, Li Qin, Ling, Chen, Zhou, Hui, Wang, Xiang, Liao, Joseph, Reddy, Gunugunuri K., Deng, Liangzi, Peck, Torin C., Zhang, Ruigang, Whittingham, M. Stanley, Wang, Chongmin, Chu, Ching-Wu, Yao, Yan, & Jia, Hongfei. A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction. United States. https://doi.org/10.1038/s41467-019-12009-8
Zhou, Li Qin, Ling, Chen, Zhou, Hui, Wang, Xiang, Liao, Joseph, Reddy, Gunugunuri K., Deng, Liangzi, Peck, Torin C., Zhang, Ruigang, Whittingham, M. Stanley, Wang, Chongmin, Chu, Ching-Wu, Yao, Yan, and Jia, Hongfei. Mon . "A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction". United States. https://doi.org/10.1038/s41467-019-12009-8. https://www.osti.gov/servlets/purl/1638489.
@article{osti_1638489,
title = {A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction},
author = {Zhou, Li Qin and Ling, Chen and Zhou, Hui and Wang, Xiang and Liao, Joseph and Reddy, Gunugunuri K. and Deng, Liangzi and Peck, Torin C. and Zhang, Ruigang and Whittingham, M. Stanley and Wang, Chongmin and Chu, Ching-Wu and Yao, Yan and Jia, Hongfei},
abstractNote = {The efficiency of sunlight-driven reduction of carbon dioxide (CO2), a process mimicking the photosynthesis in nature that integrates the light harvester and electrolysis cell to convert CO2 into valuable chemicals, is greatly limited by the sluggish kinetics of oxygen evolution in pH-neutral conditions. Current non-noble metal oxide catalysts developed to drive oxygen evolution in alkaline solution have poor performance in neutral solutions. Here we report a highly active and stable oxygen evolution catalyst in neutral pH, Brownmillerite Sr2GaCoO5, with the specific activity about one order of magnitude higher than that of widely used iridium oxide catalyst. Using Sr2GaCoO5 to catalyze oxygen evolution, the integrated CO2 reduction achieves the average solar-to-CO efficiency of 13.9% with no appreciable performance degradation in 19h of operation. Our results not only set a record for the efficiency in sunlight-driven CO2 reduction, but open new opportunities towards the realization of practical CO2 reduction systems.},
doi = {10.1038/s41467-019-12009-8},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {9}
}

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    Works referencing / citing this record:

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