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  In Situ Exploring of the Origin of the Enhanced Oxygen Evolution Reaction Efficiency of Metal(Co/Fe)-Organic Framework Catalysts Via Postprocessing

Zhou, J., Hu, Y., Chang, Y.-C., Hu, Z., Huang, Y.-C., Fan, Y., et al. (2022). In Situ Exploring of the Origin of the Enhanced Oxygen Evolution Reaction Efficiency of Metal(Co/Fe)-Organic Framework Catalysts Via Postprocessing. ACS Catalysis, 12(5), 3138-3148. doi:10.1021/acscatal.1c05532.

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 Creators:
Zhou, Jing1, Author
Hu, Yitian1, Author
Chang, Yu-Chung1, Author
Hu, Zhiwei2, Author              
Huang, Yu-Cheng1, Author
Fan, YaLei1, Author
Lin, Hong-Ji1, Author
Pao, Chih-Wen1, Author
Dong, Chung-Li1, Author
Lee, Jyh-Fu1, Author
Chen, Chien-Te1, Author
Wang, Jian-Qiang1, Author
Zhang, Linjuan1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863461              

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 Abstract: The oxygen evolution reaction (OER) is of vital importance for electrochemical energy conversion technologies. The use of metal-organic framework (MOF) catalysts after postprocessing is an important method to optimize catalytic activity; however, little attention has been paid to the transformation of the electronic structure and coordinated ions under operando conditions. Here, we focus on a Prussian blue analogue (PBA) with the formula Na2Co2+[Fe2+(CN)(6)]center dot nH(2)O after postprocessing at a temperature of 400 degrees C. The catalysts exhibit a significant improvement in the OER activity with an overpotential of 254 mV against 320 mV for the initial PBA at 10 mA cm(-2) in 1 M KOH. Our ex situ soft X-ray absorption spectroscopy (XAS) results demonstrate that some of the high-spin Co2+ and low-spin Fe2+ ions of PBA exhibit exchange with N and C ligands. Our fast operando hard XAS study revealed a dynamic evolution process of the transformation of ligands from N(C) in the initial Na2Co[Fe(CN)(6)]center dot nH(2)O to oxygen and the formation of pure low-spin Co3+ oxide and high-spin Fe3+ oxide after OER. The amorphous (Co,Fe)OOH chemical state was identified as the catalytically active state based on our operando X-ray spectroscopy results. The results of this study provide insights into a dynamic evolution process of MOFs after postprocessing and the formation of real active sites during electrocatalysis.

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Language(s): eng - English
 Dates: 2022-02-222022-02-22
 Publication Status: Published in print
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 Rev. Type: -
 Identifiers: ISI: 000773693300039
DOI: 10.1021/acscatal.1c05532
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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 12 (5) Sequence Number: - Start / End Page: 3138 - 3148 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435