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  Single-Atom Reversible Lithiophilic Sites toward Stable Lithium Anodes

Yang, Z., Dang, Y., Zhai, P., Wei, Y., Chen, Q., Zuo, J., et al. (2022). Single-Atom Reversible Lithiophilic Sites toward Stable Lithium Anodes. Advanced Energy Materials, 12(8): 2103368. doi:10.1002/aenm.202103368.

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Advanced Energy Materials - 2022 - Yang - Single‐Atom Reversible Lithiophilic Sites toward Stable Lithium Anodes.pdf (Publisher version), 3MB
 
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https://doi.org/10.1002/aenm.202103368 (Publisher version)
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 Creators:
Yang, Z.1, 2, Author
Dang, Y.1, Author
Zhai, P.3, Author
Wei, Y.4, Author
Chen, Q.1, Author
Zuo, J.1, Author
Gu, X.1, Author
Yao, Y.1, Author
Wang, X.1, Author
Zhao, F.1, Author
Wang, J.2, Author
Yang, S.1, Author
Tang, P.1, 5, 6, Author              
Gong, Y.1, 7, Author
Affiliations:
1School of Materials Science and Engineering, Beihang University, ou_persistent22              
2School of Physics, Beihang University, ou_persistent22              
3College of Physics, Qingdao University, ou_persistent22              
4Beijing Key Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, ou_persistent22              
5Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
6Center for Free-Electron Laser Science, ou_persistent22              
7Center for Micro-Nano Innovation, Beihang University, ou_persistent22              

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 Abstract: Lithiophilic sites with high binding energy to Li have shown the capability to guide uniform Li deposition, however, the irreversible reaction between Li and lithiophilic sites causes a loss of lithiophilicity. Herein, the concept of using reversible lithiophilic sites, such as single-atoms (SAs) doped graphene, as a host, is systematically inspected in the context of Li metal battery (LMB) performance. Here, it is proposed that the binding energy to Li atoms should be within a certain threshold range, i.e., strong enough to inhibit Li dendrite growth and weak enough to avoid host structure collapse. Six kinds of SAs are utilized; doped 3D graphene, nitrogen-doped 3D graphene, and pure 3D graphene, whose performance in LMBs are compared with each other. It is discovered that the SA-Mn doped 3D graphene (SAMn@NG) has the most reversible lithiophilic site, in which adsorption strength with Li is suitable to guide uniform deposition and keep the structure stable. During Li plating/stripping, the changes of the atomic structures in SAMn@NG, such as change of bond length and bond angle around Mn atoms are much smaller than those on SAZr@NG, although its binding energy is higher, enabling a much-improved battery performance in SAMn@NG. This work provides a new insight to design lithiophilic sites in LMBs.

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Language(s): eng - English
 Dates: 2021-12-102021-10-282022-01-122022-02-24
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/aenm.202103368
 Degree: -

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Title: Advanced Energy Materials
  Abbreviation : Adv. Energy Mater.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 12 (8) Sequence Number: 2103368 Start / End Page: - Identifier: ISSN: 1614-6832
CoNE: https://pure.mpg.de/cone/journals/resource/1614-6832