Upcycling Spent Graphite into Fluorine-Doped Reduced Graphene Oxide Anodes for High-Performance Lithium-Ion Batteries

Fei Li , Baolin Xing , Zhenshuai Wang , Yida Hou , Lei Yang , Huihui Zeng , Qiaoqiao Pan

Journal of Wuhan University of Technology Materials Science Edition ›› 2026, Vol. 41 ›› Issue (3) : 623 -638.

PDF
Journal of Wuhan University of Technology Materials Science Edition ›› 2026, Vol. 41 ›› Issue (3) :623 -638. DOI: 10.1007/s11595-026-3281-2
Advanced Materials
research-article
Upcycling Spent Graphite into Fluorine-Doped Reduced Graphene Oxide Anodes for High-Performance Lithium-Ion Batteries
Author information +
History +
PDF

Abstract

Fluorine-doped reduced graphene oxide (FRGO) was synthesized from spent graphite (SG) by first producing reduced graphene oxide (RGO) via potassium permanganate-assisted oxidation and thermal reduction, followed by fluorination with lithium hexafluorophosphate. The optimized material, FRGO-3, exhibited an expanded interlayer spacing of 0.375 nm, an ultrahigh specific surface area of 1 433.86 m2·g−1, and a high fluorine doping content of 3.6%. Fluorine incorporation was predominantly achieved in semi-ionic and co-valent C-F configurations. Owing to these structural and chemical characteristics, FRGO-3 demonstrated remarkable lithium storage performance, including a high reversible capacity of 1 323 mAh·g−1 at 50 mA·g−1 and a retained capacity of 489 and 318 mAh·g−1 even at a high current density of 1 000 and 2 000 mA·g−1, along with excellent cycling stability. These results underscore its potential as an advanced anode material for high-performance lithium-ion batteries(LIBs). This work presents an efficient and scalable approach for the regeneration of waste graphite while unlocking its promise for sustainable LIB applications.

Keywords

spent graphite / reduced graphene oxide / fluorine-doped / lithium-ion batteries

Cite this article

Download citation ▾
Fei Li, Baolin Xing, Zhenshuai Wang, Yida Hou, Lei Yang, Huihui Zeng, Qiaoqiao Pan. Upcycling Spent Graphite into Fluorine-Doped Reduced Graphene Oxide Anodes for High-Performance Lithium-Ion Batteries. Journal of Wuhan University of Technology Materials Science Edition, 2026, 41 (3) : 623-638 DOI:10.1007/s11595-026-3281-2

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

Shi F, Xing B, Zeng H, et al. Porous Carbon Nanorods Induced by Electrostatically Assembling Carbon Quantum Dots within the Confined Hollow Space of Halloysite for Lithium-Ion Battery Anodes[J]. Advanced Functional Materials, 2025: 2 501 751

[2]

Wu Y, Ye H, Li Y. Molecular Engineering of Organic Electrode Materials for Beyond Lithium-Ion Batteries. Advanced Functional Materials, 2025, 35(28): 2 424 329. J].

[3]

Fang J, Wan G, Zheng M, et al. Recycling of Spent Lithium-Ion Batteries in View of Lithium[J]. Advanced Energy Materials, 2025, 2 501 318

[4]

Lai Z, Long J, Lu Y, et al.. Direct Recycling of Retired Lithium-Ion Batteries: Emerging Methods for Sustainable Reuse. Advanced Energy Materials, 2025, 15(21): 2 501 009. J].

[5]

Zhou J, Zhou X, Yu W, et al.. Towards Greener Recycling: Direct Repair of Cathode Materials in Spent Lithium-Ion Batteries. Electrochemical Energy Reviews, 2024, 7(1): 13. J].

[6]

Natarajan S, Noda S. Advancements in Direct Recycling Technologies for Lithium-Ion Battery Cathodes: Overcoming Challenges in Cathode Regeneration. Materials Science and Engineering: R: Reports, 2025, 164: 100 976. J].

[7]

Zhang D, Wang Z, Bao X, et al.. A Green and Low-Cost Approach to Recover Graphite for High-Performance Aluminum Ion Battery Cathode. Materials Today Sustainability, 2024, 28: 100 957. J].

[8]

Niu B, Xiao J, Xu Z. Advances and Challenges in Anode Graphite Recycling from Spent Lithium-Ion Batteries. Journal of Hazardous Materials, 2022, 439: 129 678. J].

[9]

Tian H, Graczyk-Zajac M, Kessler A, et al.. Recycling and Reusing of Graphite from Retired Lithium-ion Batteries: A Review. Advanced Materials, 2024, 36(13): 2 308 494. J].

[10]

Zhu X, Chen Y, Xiao J, et al.. The Strategy for Comprehensive Recovery and Utilization of the Graphite Anode Materials from the End-of-Life Lithium-Ion Batteries: Urgent Status and Policies. Journal of Energy Storage, 2023, 68: 107 798. J].

[11]

Perumal P, Andersen S M, Nikoloski A, et al.. Leading Strategies and Research Advances for the Restoration of Graphite from Expired Li+ Energy Storage Devices. Journal of Environmental Chemical Engineering, 2021, 9(6): 106 455. J].

[12]

Hou Y, Guo H, Xing B, et al.. Purification of Spent Graphite and Surface Modification with Amorphous Carbons as Anodes for High-Performance Lithium-Ion Batteries. Fuel, 2024, 374: 132 488. J].

[13]

Khamaru S, Ghosh S, Martha S. Autogenous Pressure Assisted Aqua-Thermal Regeneration of Spent Graphite in a Designed Reactor: Second-Life Electrochemistry and Technoenvironmental Benefits. Advanced Energy Materials, 2025, 15(34): 2 501 921. J].

[14]

Li J, Zhou H, Gou Y, et al.. Quenching of Spent Graphite: Upcycling Regeneration with Tailoring Subsurface and in-Plane Defects Towards High-Rate Properties. Journal of Power Sources, 2025, 641: 236 890. J].

[15]

Wang Y, Zhang Y, Kimura H, et al.. Nitrogen-Doped Expanded Graphite Derived from Spent Graphite Induce Uniform Growth of Lithium Peroxide for High-Performance Li-Oxygen Battery. Journal of Cleaner Production, 2023, 414: 137 703. J].

[16]

Xie X, Zhang J, Chen Y, et al.. A Method for The Preparation of Graphene from Spent Graphite of Retired Lithium-Ion Batteries. Journal of Power Sources, 2024, 594: 234 023. J].

[17]

Wang X, Yu H, Zhou J, et al.. Upgrading Anode Graphite from Retired Lithium Ion Batteries via Solid-Phase Exfoliation by Mechanochemical Strategy. Waste Management, 2024, 182: 102-112. J].

[18]

Bejigo K S, Fikadu B, Raaju Sundhar A S, et al.. Waste to Wealth: Upgrading Spent Graphite Towards Defect-rich Nitrogen-Doped Graphene for Lithium Storage and Oxygen Electrocatalysis. Carbon, 2025, 238: 120 261. J].

[19]

Nazari P, Hamidi A, Golmohammadzadeh R, et al.. Upcycling Spent Graphite in LIBs into Battery-Grade Graphene: Managing the Produced Waste and Environmental Impacts Analysis. Waste Management, 2024, 174: 140-152. J].

[20]

Chen S, Zheng F, Feng J, et al.. Theoretical Study on Single-Side Fluorinated Graphene for Lithium Storage. Applied Surface Science, 2021, 560: 150 033. J].

[21]

Li Y-Y, Liu C, Chen L, et al.. Multi-Layered Fluorinated Graphene Cathode Materials for Lithium and Sodium Primary Batteries. Rare Metals, 2023, 42(3): 940-953. J].

[22]

Feng W, Long P, Feng Y, et al.. Two-Dimensional Fluorinated Graphene: Synthesis, Structures, Properties and Applications. Advanced Science, 2016, 3(7): 1 500 413. J].

[23]

Li P, Liu Y, Bao X, et al.. Nitrogen and Fluorine Co-Doped Graphene for Ultra-Stable Lithium Metal Anodes. Nano Research, 2024, 17(8): 7 212-7 220. J].

[24]

Yuan G, Wan T, BaQais A, et al.. Boron and Fluorine Co-Doped Laser-Induced Graphene Towards High-Performance Micro-Supercapacitors. Carbon, 2023, 212: 118 101. J].

[25]

Jeon I-Y, Ju M J, Xu J, et al.. Edge-Fluorinated Graphene Nanoplatelets as High Performance Electrodes for Dye-Sensitized Solar Cells and Lithium Ion Batteries. Advanced Functional Materials, 2015, 25(8): 1 170-1 179. J].

[26]

Huang S, Li Y, Feng Y, et al.. Nitrogen and Fluorine Co-Doped Graphene as A High-Performance Anode Material for Lithium-Ion Batteries. Journal of Materials Chemistry A, 2015, 3(46): 23 095-23 105. J].

[27]

Xing B, Zeng H, Huang G, et al.. Porous Graphene Prepared from Anthracite as High Performance Anode Materials for Lithium-Ion Battery Applications. Journal of Alloys and Compounds, 2019, 779: 202-211. J].

[28]

Hou D, Guo Z, Wang Y, et al.. Microwave-Assisted Reconstruction of Spent Graphite and Its Enhanced Energy-Storage Performance as LIB Anodes. Surfaces and Interfaces, 2021, 24: 101 098. J].

[29]

Ruan D, Wang F, Wu L, et al.. A High-Performance Regenerated Graphite Extracted from Discarded Lithium-Ion Batteries. New Journal of Chemistry, 2021, 45(3): 1 535-1 540. J].

[30]

Hwang M, Kim H-W, Jin J-U, et al.. Structural Control of Crumpled Sulfur-Assisted Reduced Graphene Oxide with Elemental Sulfur for Supercapacitor. International Journal of Energy Research, 2021, 45(15): 21 209-21 218. J].

[31]

Han X, Penki T R, Sekharappa S, et al.. Low-Temperature Thermal Exfoliated Reduced Graphene Oxide as An Anode Material for Li-Ion Batteries. Carbon Letters, 2025, 35: 2 847-2 862. J].

[32]

Tasdemir A, Bulut Kopuklu B, Kirlioglu A C, et al.. The Influence of Nitrogen Doping on Reduced Graphene Oxide as Highly Cyclable Li-Ion Battery Anode with Enhanced Performance. International Journal of Hydrogen Energy, 2021, 46(21): 11 865-11 877. J].

[33]

Min W, Chen X, Huang S, et al.. High Performance Lithium Ion Battery Cathode Based Reduced Holey Graphene Oxides from Spent Lithium Ion Batteries. Carbon, 2023, 210: 118 038. J].

[34]

Fan K, Fu J, Liu X, et al.. Dependence of the Fluorination Intercalation of Graphene Toward High-Quality Fluorinated Graphene Formation. Chemical Science, 2019, 10(21): 5 546-5 555. J].

[35]

Zeng H, Sun H, Xing B, et al.. Modifier-Assisted Co-Thermal Carbonization of Lignite for Hard Carbon with Enriched Pseudo-Graphitic Domains and Closed Pores Toward Enhanced Sodium Storage. Carbon, 2025, 244: 120 694. J].

[36]

Wang Z, Xing B, Zeng H, et al.. Space-Confined Carbonization Strategy for Synthesis of Carbon Nanosheets from Glucose and Coal Tar Pitch for High-Performance Lithium-Ion Batteries. Applied Surface Science, 2021, 547: 149 228. J].

[37]

Mahmood A, Yuan Z, Sui X, et al.. Foldable and Scrollable Graphene Paper with Tuned Interlayer Spacing as High Areal Capacity Anodes for Sodium-Ion Batteries. Energy Storage Materials, 2021, 41: 395-403. J].

[38]

Kudin K N, Ozbas B, Schniepp H C, et al.. Raman Spectra of Graphite Oxide and Functionalized Graphene Sheets. Nano Letters, 2008, 8(1): 36-41. J].

[39]

Shang N G, Silva S R P, Jiang X, et al.. Directly Observable G Band Splitting in Raman Spectra from Individual Tubular Graphite Cones. Carbon, 2011, 49(9): 3 048-3 054. J].

[40]

Silva D L, Campos J L E, Fernandes T F D, et al.. Raman Spectroscopy Analysis of Number of Layers in Mass-Produced Graphene Flakes. Carbon, 2020, 161: 181-189. J].

[41]

Xiao H, Ji G, Ye L, et al.. Efficient Regeneration and Reutilization of Degraded Graphite as Advanced Anode for Lithium-Ion Batteries. Journal of Alloys and Compounds, 2021, 888: 161 593. J].

[42]

Dedryvère R, Martinez H, Leroy S, et al.. Surface Film Formation on Electrodes in A LiCoO2/Graphite Cell: A Step by Step XPS Study. Journal of Power Sources, 2007, 174(2): 462-468. J].

[43]

Zhang J, Ji G, Zhao R, et al.. Construction of TiP2O7 Nanosheets/rGO Hierarchical Flower-like Heterostructures for Superfast and Ultralong Lithiation/Delithiation Process. Applied Surface Science, 2020, 513: 145 854. J].

[44]

Wen Y, Liu H, Jiang X. Preparation of Graphene by Exfoliation and Its Application in Lithium-Ion Batteries. Journal of Alloys and Compounds, 2023, 961: 170 885. J].

[45]

Wang Z, Zhang D, Chen J, et al.. High-Performance Aluminum-Ion Batteries Enabled by Architected Reduced Graphene Oxide Electrodes. Surfaces and Interfaces, 2025, 63: 106 348. J].

[46]

Wu Y, Zhao W, Qiang Y, et al.. π-π Interaction Between Fluorinated Reduced Graphene Oxide and Acridizinium Ionic Liquid: Synthesis and Anti-Corrosion Application. Carbon, 2020, 159: 292-302. J].

[47]

Nakajima T, Gupta V, Ohzawa Y, et al.. Influence of Cointercalated HF on The Electrochemical Behavior of Highly Fluorinated Graphite. Journal of Power Sources, 2004, 137(1): 80-87. J].

[48]

Wang Z, Zhang D, Bao X, et al.. Space-Confined Intercalation Expansion Strategy for Simple and Rapid Synthesis of Kish-Based Expanded Graphite for Aluminum Ion Batteries. Carbon, 2024, 223: 119 016. J].

[49]

Quan Y, Liu Q, Li K, et al.. Simultaneous Fluorination and Purification of Natural Block Coaly Graphite into Fluorinated Graphene with Tunable Fluorination Degree. Materials Today Communications, 2022, 32: 104 130. J].

[50]

Zhai P, Yang Z, Wei Y, et al.. Two-Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High-Performance Solid-State Lithium Batteries. Advanced Energy Materials, 2022, 12(42): 2 200 967. J].

[51]

Wang Z, Bao X, Zhang D, et al.. Application of Purified Kish Flake Graphite as A Potential Cathode Material for High-Performance Aluminum Ion Batteries. Journal of Alloys and Compounds, 2023, 954: 170 197. J].

[52]

Xu Y, Zhan L, Wang Y, et al.. Fluorinated Grapheneasa Cathode Material for High Performance Primary Lithium Ion Batteries. New Carbon Materials, 2015, 30(1): 79-85. J].

[53]

Liu X, Yang H. Kinetics of Thermal Decomposition of Lithium Hexafluorophosphate. Chinese Journal of Chemical Physics, 2013, 26(4): 467-470. J].

[54]

Yang X, Xing B, Zeng H, et al.. Sulfur-Doped Porous Carbon Nanosheets from Ice Template-Induced Assembly of Sulfonated Naphthalene for Lithium-Ion Battery Anodes. Applied Surface Science, 2025, 708: 163 748. J].

[55]

Ma H, Jiang H, Jin Y, et al.. Carbon Nanocages@Ultrathin Carbon Nanosheets: One-Step Facile Synthesis and Application as Anode Material for Lithium-Ion Batteries. Carbon, 2016, 105: 586-592. J].

[56]

Xing B, Zhang C, Cao Y, et al.. Preparation of Synthetic Graphite from Bituminous Coal as Anode Materials for High Performance Lithium-Ion Batteries. Fuel Processing Technology, 2018, 172: 162-171. J].

[57]

Wang Y, Zhang Q, Jia M, et al.. Porous Graphene for High Capacity Lithium Ion Battery Anode Material. Applied Surface Science, 2016, 363: 318-322. J].

[58]

Hou L, Xing B, Zeng H, et al.. Aluminothermic Reduction Synthesis of Si/C Composite Nanosheets from Waste Vermiculite as High-Performance Anode Materials for Lithium-ion Batteries. Journal of Alloys and Compounds, 2022, 922: 166 134. J].

[59]

Jang W, Kim J, Lee S, et al.. N/S Co-Doped Nanocomposite of Graphene Oxide and Graphene-Like Organic Molecules as All-Carbonaceous Anode Material for High-Performance Li-Ion Batteries. Composites Part B: Engineering, 2025, 291: 111 994. J].

[60]

Zeng H, Xing B, Zhang C, et al.. Edge-Boron-Functionalized Coal-Derived Graphite Nanoplatelets Prepared via Mechanochemical Modification for Enhanced Li-Ion Storage at Low-Voltage Plateau. Applied Surface Science, 2023, 621: 156 870. J].

[61]

Inamoto J, Komiyama S, Uchida S, et al.. Insight into the Origin of the Rapid Charging Ability of Graphene-Like Graphite as A Lithium-Ion Battery Anode Material Using Electrochemical Impedance Spectroscopy. The Journal of Physical Chemistry C, 2022, 126(38): 16 100-16 108. J].

[62]

Sun Y, Xing B, Zhang Y, et al.. Ice Template-Induced Assembly Coupled with Carbonization Strategy for Preparation of Sulfur-Doped Porous Carbon Nanosheets from Lignite as High-Capacity Anode for Lithium-Ion Batteries. Fuel, 2024, 372: 132 163. J].

[63]

Liu D, Wang J, Li Z, et al.. Ultrathin Nitrogen-Rich Porous Carbon Nanosheets with Fluorine Doping for High-Performance Potassium Storage. Electrochimica Acta, 2022, 411: 140 094. J].

[64]

Xing B, Shi F, Jin Z, et al.. A Facile Ice-Templating-Induced Puzzle Coupled with Carbonization Strategy for Kilogram-Level Production of Porous Carbon Nanosheets as High-Capacity Anode for Lithium-Ion Batteries. Carbon Energy, 2024, 6(12): e633. J].

[65]

Shi Y, Wang M, Yang Z, et al.. Plasma-Induced Synthesis of N-Doped Graphene Microsheets on Graphite Surface for Lithium Battery Anode: Physicochemical Properties and Electrochemical Performance. Applied Surface Science, 2025, 714: 164 449. J].

[66]

Xing B, Meng W, Liang H, et al.. Flexible Coal-Derived Carbon Fibers via Electrospinning for Self-standing Lithium-Ion Battery Anodes. International Journal of Mining Science and Technology, 2024, 34(12): 1 753-1 763. J].

[67]

An H, Li Y, Feng Y, et al.. Reduced Graphene Oxide Doped Predominantly with CF2 Groups as A Superior Anode Material for Long-Life Lithium-Ion Batteries. Chemical Communications, 2018, 54(22): 2 727-2 730. J].

RIGHTS & PERMISSIONS

Wuhan University of Technology and Springer-Verlag GmbH Germany, Part of Springer Nature

PDF

0

Accesses

0

Citation

Detail

Sections
Recommended

/