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author：

Liu, Y. (Liu, Y..) [1] | Zheng, Y. (Zheng, Y..) [2] | Yan, K. (Yan, K..) [3] | Wang, J. (Wang, J..) [4] | Qian, Y. (Qian, Y..) [5] | Guo, J. (Guo, J..) [6] | Zhang, Q. (Zhang, Q..) [7] | Zhang, C. (Zhang, C..) [8] | Jia, P. (Jia, P..) [9] | Zhang, Z. (Zhang, Z..) [10] | Dong, S. (Dong, S..) [11] | Jiang, J. (Jiang, J..) [12] | Guo, Y. (Guo, Y..) [13] | Chen, R. (Chen, R..) [14] | Huang, Y. (Huang, Y..) [15] | Shen, Y. (Shen, Y..) [16] | Xu, J. (Xu, J..) [17] | Zheng, R. (Zheng, R..) [18] | Tang, Y. (Tang, Y..) [19] | Jiang, W. (Jiang, W..) [20] | Shao, H. (Shao, H..) [21]

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Scopus

Abstract：

Considering　the　growing　pre-lithiation　demand　for　high-performance　Si-based　anodes　and　consequent　additional　costs　caused　by　the　strict　pre-lithiation　environment,　developing　effective　and　environmentally　stable　pre-lithiation　additives　is　a　challenging　research　hotspot.　Herein,　interfacial　engineered　multifunctional　Li13Si4@perfluoropolyether　(PFPE)/LiF　micro/nanoparticles　are　proposed　as　anode　pre-lithiation　additives,　successfully　constructed　with　the　hybrid　interface　on　the　surface　of　Li13Si4　through　PFPE-induced　nucleophilic　substitution.　The　synthesized　multifunctional　Li13Si4@PFPE/LiF　realizes　the　integration　of　active　Li　compensation,　long-term　chemical　structural　stability　in　air,　and　solid　electrolyte　interface　(SEI)　optimization.　In　particular,　the　Li13Si4@PFPE/LiF　with　a　high　pre-lithiation　capacity　(1102.4　mAh　g−1)　is　employed　in　the　pre-lithiation　Si-based　anode,　which　exhibits　a　superior　initial　Coulombic　efficiency　of　102.6%.　Additionally,　in　situ　X-ray　diffraction/Raman,　density　functional　theory　calculation,　and　finite　element　analysis　jointly　illustrate　that　PFPE-predominant　hybrid　interface　with　modulated　abundant　highly　electronegative　F　atoms　distribution　reduces　the　water　adsorption　energy　and　oxidation　kinetics　of　Li13Si4@PFPE/LiF,　which　delivers　a　high　pre-lithiation　capacity　retention　of　84.39%　after　exposure　to　extremely　moist　air　(60%　relative　humidity).　Intriguingly,　a　LiF-rich　mechanically　stable　bilayer　SEI　is　constructed　on　anodes　through　a　pre-lithiation-driven　regulation　for　the　behavior　of　electrolyte　decomposition.　Benefitting　from　pre-lithiation　via　multifunctional　Li13Si4@PFPE/LiF,　the　full　cell　and　pouch　cell　assembled　with　pre-lithiated　anodes　operate　with　long-time　stability　of　86.5%　capacity　retention　over　200　cycles　and　superior　energy　density　of　549.9　Wh　kg–1,　respectively.　The　universal　multifunctional　pre-lithiation　additives　provide　enlightenment　on　promoting　large-scale　applications　of　pre-lithiation　on　commercial　high-energy-density　and　long-cycle-life　lithium-ion　batteries.　©　2025　The　Author(s).　Carbon　Energy　published　by　Wenzhou　University　and　John　Wiley　&　Sons　Australia,　Ltd.

Keyword：

interfacial functionalization lithium-silicon alloys multifunctional pre-lithiation additives Si-based anodes solid electrolyte interface

Community：

  • [ 1 ] [Liu Y.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 2 ] [Zheng Y.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 3 ] [Yan K.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 4 ] [Yan K.]Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China
  • [ 5 ] [Wang J.]Department of Materials Science & Engineering, School of Innovation and Entrepreneurship, University of Science and Technology, Shenzhen, China
  • [ 6 ] [Qian Y.]Shenzhen CAPCHEM Technology Co. Ltd., Shenzhen, China
  • [ 7 ] [Guo J.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 8 ] [Guo J.]School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, China
  • [ 9 ] [Zhang Q.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 10 ] [Zhang C.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 11 ] [Jia P.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 12 ] [Zhang Z.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 13 ] [Dong S.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 14 ] [Jiang J.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 15 ] [Guo Y.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 16 ] [Chen R.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 17 ] [Chen R.]Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China
  • [ 18 ] [Huang Y.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 19 ] [Shen Y.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 20 ] [Xu J.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 21 ] [Zheng R.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 22 ] [Tang Y.]College of Chemical Engineering, Fuzhou University, Fuzhou, China
  • [ 23 ] [Jiang W.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao
  • [ 24 ] [Shao H.]Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macao

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Carbon Energy

ISSN： 2637-9368

Year： 2025

1 9 . 5 0 0

JCR@2023

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