Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts
Abstract
Achieving stable, low-cost electrocatalysts represents a daunting challenge towards practical water oxidation reactions. Here, we report that a degraded electrocatalyst can be revivified under catalytic operating conditions by manipulating reversible phase segregation. Under the oxygen evolution reaction conditions, Fe segregation develops in the Ni–Fe hydroxide host lat- tice, with the formation of FeOOH, resulting in an interface between the FeOOH and the host lattice. A dynamic metal dissolu- tion–redeposition process accelerates the Fe segregation and formation of the FeOOH secondary phase, resulting in catalyst deactivation. Operando synchrotron spectroscopic and microscopic analyses suggest that the phase segregation is revers- ible between the water oxidation potential and the catalyst reduction potential. Therefore, we have developed an intermittent reduction methodology to revivify the catalytic activity under the operating conditions, enhancing catalyst durability. The pres- ent study highlights that tailoring phase segregation at the catalyst/electrolyte interface constitutes an important strategy for revivifying and stabilizing catalytic activity.
- Authors:
-
[1];
[5];
[7];
[3];
[2]
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Tianjin Univ. (China)
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Tianjin Univ. (China)
- Tianjin Univ. (China); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Univ. of Adelaide, SA (Australia)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Science Foundation of China; Institute for Critical Technology and Applied Science
- OSTI Identifier:
- 1671340
- Grant/Contract Number:
- AC02-06CH11357; AC02-76SF00515; 51871160; 51671141; 51471115
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Catalysis
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2520-1158
- Publisher:
- Springer Nature
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Kuai, Chunguang, Xu, Zhengrui, Xi, Cong, Hu, Anyang, Yang, Zhijie, Zhang, Yan, Sun, Cheng-Jun, Li, Luxi, Sokaras, Dimosthenis, Dong, Cunku, Qiao, Shi-Zhang, Du, Xi-Wen, and Lin, Feng. Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts. United States: N. p., 2020.
Web. doi:10.1038/s41929-020-0496-z.
Kuai, Chunguang, Xu, Zhengrui, Xi, Cong, Hu, Anyang, Yang, Zhijie, Zhang, Yan, Sun, Cheng-Jun, Li, Luxi, Sokaras, Dimosthenis, Dong, Cunku, Qiao, Shi-Zhang, Du, Xi-Wen, & Lin, Feng. Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts. United States. https://doi.org/10.1038/s41929-020-0496-z
Kuai, Chunguang, Xu, Zhengrui, Xi, Cong, Hu, Anyang, Yang, Zhijie, Zhang, Yan, Sun, Cheng-Jun, Li, Luxi, Sokaras, Dimosthenis, Dong, Cunku, Qiao, Shi-Zhang, Du, Xi-Wen, and Lin, Feng. Mon .
"Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts". United States. https://doi.org/10.1038/s41929-020-0496-z. https://www.osti.gov/servlets/purl/1671340.
@article{osti_1671340,
title = {Phase segregation reversibility in mixed-metal hydroxide water oxidation catalysts},
author = {Kuai, Chunguang and Xu, Zhengrui and Xi, Cong and Hu, Anyang and Yang, Zhijie and Zhang, Yan and Sun, Cheng-Jun and Li, Luxi and Sokaras, Dimosthenis and Dong, Cunku and Qiao, Shi-Zhang and Du, Xi-Wen and Lin, Feng},
abstractNote = {Achieving stable, low-cost electrocatalysts represents a daunting challenge towards practical water oxidation reactions. Here, we report that a degraded electrocatalyst can be revivified under catalytic operating conditions by manipulating reversible phase segregation. Under the oxygen evolution reaction conditions, Fe segregation develops in the Ni–Fe hydroxide host lat- tice, with the formation of FeOOH, resulting in an interface between the FeOOH and the host lattice. A dynamic metal dissolu- tion–redeposition process accelerates the Fe segregation and formation of the FeOOH secondary phase, resulting in catalyst deactivation. Operando synchrotron spectroscopic and microscopic analyses suggest that the phase segregation is revers- ible between the water oxidation potential and the catalyst reduction potential. Therefore, we have developed an intermittent reduction methodology to revivify the catalytic activity under the operating conditions, enhancing catalyst durability. The pres- ent study highlights that tailoring phase segregation at the catalyst/electrolyte interface constitutes an important strategy for revivifying and stabilizing catalytic activity.},
doi = {10.1038/s41929-020-0496-z},
journal = {Nature Catalysis},
number = 9,
volume = 3,
place = {United States},
year = {2020},
month = {8}
}
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