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author：

Liu, Yinan (Liu, Yinan.) [1] | Zheng, Yun (Zheng, Yun.) [2] | Yan, Kunye (Yan, Kunye.) [3] | Wang, Jun (Wang, Jun.) [4] | Qian, Yunxian (Qian, Yunxian.) [5] | Guo, Junpo (Guo, Junpo.) [6] | Zhang, Qi (Zhang, Qi.) [7] | Zhang, Congcong (Zhang, Congcong.) [8] | Jia, Pingshan (Jia, Pingshan.) [9] | Zhang, Zhiyuan (Zhang, Zhiyuan.) [10] | Dong, Shengyang (Dong, Shengyang.) [11] | Jiang, Jiangmin (Jiang, Jiangmin.) [12] | Guo, Yan (Guo, Yan.) [13] | Chen, Rong (Chen, Rong.) [14] | Huang, Yike (Huang, Yike.) [15] | Shen, Yingying (Shen, Yingying.) [16] | Xu, Jincheng (Xu, Jincheng.) [17] | Zheng, Ruifeng (Zheng, Ruifeng.) [18] | Tang, Yuxin (Tang, Yuxin.) [19] | Jiang, Wei (Jiang, Wei.) [20] | Shao, Huaiyu (Shao, Huaiyu.) [21]

Indexed by：

EI

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：

Additives Chemical bonds Chemical stability Density functional theory Lithium alloys Lithium Fluoride Lithium-ion batteries Phase interfaces Phosphorus compounds Seebeck effect Silicon alloys Silicon batteries Solid electrolytes

Community：

  • [ 1 ] [Liu, Yinan]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, China
  • [ 2 ] [Zheng, Yun]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, China
  • [ 3 ] [Yan, Kunye]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, China
  • [ 4 ] [Yan, Kunye]Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China
  • [ 5 ] [Wang, Jun]Department of Materials Science & Engineering, School of Innovation and Entrepreneurship, University of Science and Technology, Shenzhen, China
  • [ 6 ] [Qian, Yunxian]Shenzhen CAPCHEM Technology Co. Ltd., Shenzhen, China
  • [ 7 ] [Guo, Junpo]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, China
  • [ 8 ] [Guo, Junpo]School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, China
  • [ 9 ] [Zhang, Qi]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, China
  • [ 10 ] [Zhang, Congcong]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, China
  • [ 11 ] [Jia, Pingshan]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, China
  • [ 12 ] [Zhang, Zhiyuan]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, China
  • [ 13 ] [Dong, Shengyang]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, China
  • [ 14 ] [Jiang, Jiangmin]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, China
  • [ 15 ] [Guo, Yan]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, China
  • [ 16 ] [Chen, Rong]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, China
  • [ 17 ] [Chen, Rong]Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China
  • [ 18 ] [Huang, Yike]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, China
  • [ 19 ] [Shen, Yingying]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, China
  • [ 20 ] [Xu, Jincheng]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, China
  • [ 21 ] [Zheng, Ruifeng]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, China
  • [ 22 ] [Tang, Yuxin]College of Chemical Engineering, Fuzhou University, Fuzhou, China
  • [ 23 ] [Jiang, Wei]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, China
  • [ 24 ] [Shao, Huaiyu]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, China

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Carbon Energy

Year： 2025

Issue： 9

Volume： 7

1 9 . 5 0 0

JCR@2023

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ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 1

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