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  Regulating electron transfer over asymmetric low-spin Co(II) for highly selective electrocatalysis

Wu, K.-H., Liu, Y., Tan, X., Liu, Y., Lin, Y., Huang, X., et al. (2022). Regulating electron transfer over asymmetric low-spin Co(II) for highly selective electrocatalysis. Chem Catalysis, 2(2), 372-385. doi:10.1016/j.checat.2021.12.005.

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 Creators:
Wu, Kuang-Hsu1, 2, 3, Author
Liu, Yuefeng4, Author
Tan, Xin5, Author
Liu, Yangyang3, Author
Lin, Yangming6, Author
Huang, Xing7, Author           
Ding, Yuxiao6, Author
Su, Bing-Jian8, Author
Zhang, Bingsen2, Author
Chen, Jin-Ming8, Author
Yan, Wensheng9, Author
C.Smith, Sean5, Author
Gentle, Ian R.1, Author
Zhao, Shenlong3, Author
Affiliations:
1School of Chemistry and Molecular Bioscience, The University of Queensland, St. Lucia, Brisbane, QLD 4109, Australia, ou_persistent22              
2Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning 110016, China, ou_persistent22              
3School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia, ou_persistent22              
4Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China, ou_persistent22              
5National Computational Infrastructure, Australian National University, Canberra, ACT 2601, Australia, ou_persistent22              
6Max-Planck Institute for Chemical Energy Conversion, Stiftstrasse 34–36, 45470 Mülheim, Germany, ou_persistent22              
7Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
8National Synchrotron Radiation Research Centre, Hsinchu 30076, Taiwan, ou_persistent22              
9National Synchrotron Research Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, China, ou_persistent22              

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 Abstract: The majority of energy conversion processes such as hydrogen peroxide production, nitrogen fixation, and CO2 reduction generally involve multi-electron transfer, resulting in multiple by-products and requiring tedious purification process. The development of highly selective electrocatalysts can not only reduce the energy consumption in the production process but also benefit to promote their large-scale application. Here, we report an asymmetric ligand design of molecular “Venus flytrap” at atomic CoII catalysts on a heterogeneous carbon surface for oxygen electrocatalysis with controlled selectivity. Our XAFS and DFT calculations show that the strong-field ligand-induced LS CoII centers offer inimitable steric-electronic advantages in capturing O2 and the capability to regulate reaction pathways through an H-bonding interaction between the ligands and peroxo intermediate. The proposed concept completes the picture of designer single-atom catalyst by covering the often overlooked exterior coordination sites, and is expected to be generally applicable to other heterogeneous catalyst systems.

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Language(s): eng - English
 Dates: 2021-07-232021-12-132022-01-312022-02-17
 Publication Status: Issued
 Pages: 14
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.checat.2021.12.005
 Degree: -

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Title: Chem Catalysis
  Abbreviation : Chem Catal.
Source Genre: Journal
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Publ. Info: New York : New York Elsevier Inc.
Pages: 14 Volume / Issue: 2 (2) Sequence Number: - Start / End Page: 372 - 385 Identifier: ISSN: 2667-1107
CoNE: https://pure.mpg.de/cone/journals/resource/3667-1107