This study introduces a multifunctional carbon fiber–carbon nanotube (CFCNT) architecture as a lightweight, thermally stable, and recyclable current collector for lithium-ion batteries (LIBs). Compatible with both graphite anodes and LiFePO4 cathodes, the CFCNT platform reduces collector mass to 4.4 mg/cm2—substantially lower than conventional copper (10.1 mg/cm2) and aluminum (5.1 mg/cm2) while enhancing electrical conductivity and interfacial stability. Full pouch cells employing CFCNT collectors achieve an initial capacity of 153 mAh/g and retain 126 mAh/g after 150 cycles (0.11% fade per cycle), with >91% coulombic efficiency. Safety testing reveals minimal thermal response (< 2°C rise) during nail penetration, underscoring robust mechanical and electrochemical resilience. Critically, the architecture enables direct recovery and reuse of electrodes and current collectors, supporting a closed-loop recycling strategy. These results position CFCNT collectors as a viable pathway toward safer, high-performance, and circular energy storage technologies.
| [1] |
S. Chu, Y. Cui, and N. Liu, “The Path Towards Sustainable Energy,” Nature Materials16, no. 1 (2016): 16-22, https://doi.org/10.1038/nmat4834.
|
| [2] |
J. Xiao, F. Shi, T. Glossmann, C. Burnett, and Z. Liu, “From Laboratory Innovations to Materials Manufacturing for Lithium-Based Batteries,” Nature Energy8, no. 4 (2023): 329-339, https://doi.org/10.1038/s41560-023-01221-y.
|
| [3] |
C. Yuan, “Sustainable Battery Manufacturing in the Future,” Nature Energy8, no. 11 (2023): 1180-1181, https://doi.org/10.1038/s41560-023-01374-w.
|
| [4] |
C. Yan, H. Yuan, H. S. Park, and J. Q. Huang, “Perspective on the Critical Role of Interface for Advanced Batteries,” Journal of Energy Chemistry47 (2020): 217-220, https://doi.org/10.1016/J.JECHEM.2019.09.034.
|
| [5] |
Y. Zhang, S. Jing, H. Shen, et al., “Developments, Novel Concepts, and Challenges of Current Collectors: From Conventional Lithium Batteries to All-Solid-State Batteries,” ChemElectroChem11, no. 14 (2024): e202300739, https://doi.org/10.1002/CELC.202300739.
|
| [6] |
S. Chen, C. Pan, Q. Wang, J. L. Luo, and X. Z. Fu, “Advancements in Current Collectors for Composite Lithium Metal Anodes,” Advanced Functional Materials34, no. 51 (2024): 2409812, https://doi.org/10.1002/ADFM.202409812.
|
| [7] |
S. J. Yang, J. K. Hu, F. N. Jiang, H. Yuan, H. S. Park, and J. Q. Huang, “Safer Solid-State Lithium Metal Batteries: Mechanisms and Strategies,” InfoMat6, no. 2 (2024): e12512, https://doi.org/10.1002/INF2.12512.
|
| [8] |
P. Zhu, D. Gastol, J. Marshall, R. Sommerville, V. Goodship, and E. Kendrick, “A Review of Current Collectors for Lithium-Ion Batteries,” Journal of Power Sources485 (2021): 229321, https://doi.org/10.1016/J.JPOWSOUR.2020.229321.
|
| [9] |
X. Zhang, Z. Ju, Y. Zhu, et al., “Multiscale Understanding and Architecture Design of High Energy/Power Lithium-Ion Battery Electrodes,” Advanced Energy Materials11, no. 2 (2021): 2000808, https://doi.org/10.1002/AENM.202000808.
|
| [10] |
J. F. Ding, Y. T. Zhang, R. Xu, et al., “Review on Lithium Metal Anodes Towards High Energy Density Batteries,” Green Energy & Environment8, no. 6 (2023): 1509-1530, https://doi.org/10.1016/J.GEE.2022.08.002.
|
| [11] |
J. Zhou, J. Qin, and H. Zhan, “Copper Current Collector: The Cornerstones of Practical Lithium Metal and Anode–Free Batteries,” Chemphyschem25, no. 8 (2024): e202400007, https://doi.org/10.1002/CPHC.202400007.
|
| [12] |
B. Zhou, A. Bonakdarpour, I. Stoševski, B. Fang, and D. P. Wilkinson, “Modification of Cu Current Collectors for Lithium Metal Batteries—A Review,” Progress in Materials Science130 (2022): 100996, https://doi.org/10.1016/J.PMATSCI.2022.100996.
|
| [13] |
A. Gabryelczyk, S. Ivanov, A. Bund, and G. Lota, “Corrosion of Aluminium Current Collector in Lithium-Ion Batteries: A Review,” Journal of Energy Storage43 (2021): 103226, https://doi.org/10.1016/J.EST.2021.103226.
|
| [14] |
E. Yoon, J. Lee, S. Byun, D. Kim, and T. Yoon, “Passivation Failure of Al Current Collector in LiPF6-Based Electrolytes for Lithium-Ion Batteries,” Advanced Functional Materials32, no. 22 (2022): 2200026, https://doi.org/10.1002/ADFM.202200026.
|
| [15] |
H. Li, A. Berbille, X. Zhao, Z. Wang, W. Tang, and Z. L. Wang, “A Contact-Electro-Catalytic Cathode Recycling Method for Spent Lithium-Ion Batteries,” Nature Energy8, no. 10 (2023): 1137-1144, https://doi.org/10.1038/s41560-023-01348-y.
|
| [16] |
F. Matsumoto and M. Fukunishi, “Review of Current Collector-, Binder-, Conductive Additive-Free, and Freestanding Electrodes in Lithium and Related Batteries,” Batteries10, no. 9 (2024): 330, https://doi.org/10.3390/BATTERIES10090330.
|
| [17] |
H. Chen, Y. Yang, D. T. Boyle, et al., “Free-Standing Ultrathin Lithium Metal–Graphene Oxide Host Foils With Controllable Thickness for Lithium Batteries,” Nature Energy6, no. 8 (2021): 790-798, https://doi.org/10.1038/s41560-021-00833-6.
|
| [18] |
Z. Ouyang, S. Wang, Y. Wang, et al., “An Ultralight Composite Current Collector Enabling High-Energy-Density and High-Rate Anode-Free Lithium Metal Battery,” Advanced Materials36, no. 33 (2024): 2407648, https://doi.org/10.1002/ADMA.202407648.
|
| [19] |
Z. Wang, C. Wei, H. Jiang, et al., “MXene-Based Current Collectors for Advanced Rechargeable Batteries,” Advanced Materials36, no. 2 (2024): 2306015, https://doi.org/10.1002/ADMA.202306015.
|
| [20] |
H. Kim, Y. Son, and C. Jo, “Free-Standing Carbon Materials for Lithium Metal Batteries,” ChemElectroChem11, no. 18 (2024): e202400209, https://doi.org/10.1002/CELC.202400209.
|
| [21] |
S. Zhang, S. Xiao, D. Li, et al., “Commercial Carbon Cloth: An Emerging Substrate for Practical Lithium Metal Batteries,” Energy Storage Materials48 (2022): 172-190, https://doi.org/10.1016/J.ENSM.2022.03.014.
|
| [22] |
Z. Qiao, K. Bian, C. Ding, and Y. Zhao, “Recent Progress of Carbon-Fiber-Based Electrode Materials for Energy Storage,” Diamond and Related Materials138 (2023): 110208, https://doi.org/10.1016/J.DIAMOND.2023.110208.
|
| [23] |
H. Zhuang, T. Zhang, H. Xiao, et al., “3D Free-Standing Carbon Nanofibers Modified by Lithiophilic Metals Enabling Dendrite-Free Anodes for Li Metal Batteries,” Energy & Environmental Materials6, no. 3 (2023): e12470, https://doi.org/10.1002/EEM2.12470.
|
| [24] |
Y. H. Liu, H. H. Lin, T. Y. Tsai, and C. H. Hsu, “Electrochemical Fabrication and Evaluation of a Self-Standing Carbon Nanotube/Carbon Fiber Composite Electrode for Lithium-Ion Batteries,” RSC Advances9, no. 57 (2019): 33117-33123, https://doi.org/10.1039/C9RA05876A.
|
| [25] |
L. Deng, Y. Wang, D. Li, X. Ni, and A. Ju, “Fecoo Nanosheet Grown on Free-Standing Carbon Fiber Paper for Boosting the Oxygen Evolution Reaction and Lithium-Ion Batteries,” ACS Applied Energy Materials7, no. 7 (2024): 2825-2836, https://doi.org/10.1021/ACSAEM.4C00009.
|
| [26] |
X. Li, X. Zhang, J. Xu, et al., “Potassium-Rich Iron Hexacyanoferrate/Carbon Cloth Electrode for Flexible and Wearable Potassium-Ion Batteries,” Advanced Science11, no. 5 (2024): 2305467, https://doi.org/10.1002/ADVS.202305467.
|
| [27] |
A. del Bosque, D. Vergara, G. Lampropoulos, and P. Fernández-Arias, “Energy Storage in Carbon Fiber-Based Batteries: Trends and Future Perspectives,” Applied Sciences14, no. 21 (2024): 10034, https://doi.org/10.3390/APP142110034.
|
| [28] |
X. Xia, J. Yang, Y. Liu, et al., “Material Choice and Structure Design of Flexible Battery Electrode,” Advanced Science10, no. 3 (2023): 2204875, https://doi.org/10.1002/ADVS.202204875.
|
| [29] |
Q. Xu, J. Chen, J. R. Loh, et al., “Fiber-Shaped Batteries Towards High Performance and Perspectives of Corresponding Integrated Battery Textiles,” Advanced Energy Materials14, no. 3 (2024): 2302536, https://doi.org/10.1002/AENM.202302536.
|
| [30] |
H. Hong, H. Tu, L. Jiang, Y. Du, and C. Wong, “Advances in Fabric-Based Supercapacitors and Batteries: Harnessing Textiles for Next-Generation Energy Storage,” Journal of Energy Storage75 (2024): 109561, https://doi.org/10.1016/J.EST.2023.109561.
|
| [31] |
B. Liu, Q. Gan, and Y. Fu, “Perspectives on Emerging Dual Carbon Fiber Batteries: Advantages, Challenges and Prospects,” RSC Advances14, no. 9 (2024): 6462-6469, https://doi.org/10.1039/D4RA00677A.
|
| [32] |
S. A. Thomas, J. Cherusseri, and D. N. Rajendran, “Recent Advancements in Carbon Fiber-Based Sustainable Electrodes for Flexible and Wearable Supercapacitors,” RSC Sustainability2, no. 9 (2024): 2403-2443, https://doi.org/10.1039/D4SU00146J.
|
| [33] |
H. Yang, T. Xiong, Z. Zhu, et al., “Deciphering the Lithium Storage Chemistry in Flexible Carbon Fiber-Based Self-Supportive Electrodes,” Carbon Energy4, no. 5 (2022): 820-832, https://doi.org/10.1002/CEY2.173.
|
| [34] |
X. Yan, L. Lin, Q. Chen, et al., “Multifunctional Roles of Carbon-Based Hosts for Li-Metal Anodes: A Review,” Carbon Energy3, no. 2 (2021): 303-329, https://doi.org/10.1002/CEY2.95.
|
| [35] |
X. M. Liu, Z. Huang, S. Oh, et al., “Carbon Nanotube (CNT)-Based Composites as Electrode Material for Rechargeable Li-Ion Batteries: A Review,” Composites Science and Technology72, no. 2 (2012): 121-144, https://doi.org/10.1016/J.COMPSCITECH.2011.11.019.
|
| [36] |
J. Y. Cheong, S. H. Cho, J. Lee, J. W. Jung, C. Kim, and I. D. Kim, “Multifunctional 1D Nanostructures Toward Future Batteries: A Comprehensive Review,” Advanced Functional Materials32, no. 49 (2022): 2208374, https://doi.org/10.1002/ADFM.202208374.
|
| [37] |
X. M. Liu, Z. Huang, S. Oh, et al., “Carbon Nanotube (CNT)-Based Composites as Electrode Material for Rechargeable Li-Ion Batteries: A Review,” Composites Science and Technology72, no. 2 (2012): 121-144, https://doi.org/10.1016/J.COMPSCITECH.2011.11.019.
|
| [38] |
L. Li, Y. Wang, T. Lei, Z. Xie, and Y. Liang, “Structure and Properties of Carbon Fiber Paper With Gradient Porous Structure,” Journal of Porous Materials31, no. 3 (2024): 887-895, https://doi.org/10.1007/S10934-024-01566-Z/.
|
| [39] |
M. M. Ngoma, M. Mathaba, and K. Moothi, “Effect of Carbon Nanotubes Loading and Pressure on the Performance of a Polyethersulfone (PES)/Carbon Nanotubes (CNT) Membrane,” Scientific Reports11, no. 1 (2021): 23805, https://doi.org/10.1038/s41598-021-03042-z.
|
| [40] |
A. Popa, D. Toloman, M. Stan, et al., “Tailoring the RhB Removal Rate by Modifying the PVDF Membrane Surface Through ZnO Particles Deposition,” Journal of Inorganic and Organometallic Polymers and Materials31, no. 4 (2021): 1642-1652, https://doi.org/10.1007/S10904-020-01795-0.
|
| [41] |
M. S. Dresselhaus, A. Jorio, A. G. Souza Filho, and R. Saito, “Defect Characterization in Graphene and Carbon Nanotubes Using Raman Spectroscopy,” Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences368, no. 1932 (2010): 5355-5377, https://doi.org/10.1098/RSTA.2010.0213;REQUESTEDJOURNAL:JOURNAL:RSTA;PAGE:STRING:ARTICLE/CHAPTER.
|
| [42] |
R. Saito, M. Hofmann, G. Dresselhaus, A. Jorio, and M. S. Dresselhaus, “Raman Spectroscopy of Graphene and Carbon Nanotubes,” Advances in Physics60, no. 3 (2011): 413-550, https://doi.org/10.1080/00018732.2011.582251.
|
| [43] |
A. Jorio, R. Saito, G. Dresselhaus, and M. S. Dresselhaus, “Raman Spectroscopy in Graphene Related Systems,” 2011, https://doi.org/10.1002/9783527632695.
|
| [44] |
C. Yuan, S. Chen, C. Wang, et al., “Reinforcing and Toughening Carbon Fiber/Epoxy Composites With Styrene–Butadiene–Styrene Copolymer Grafted Carbon Nanotubes,” Composite Interfaces27, no. 1 (2020): 143-159, https://doi.org/10.1080/09276440.2019.1601949.
|
| [45] |
J. Y. Kim, S. R. Lee, G. W. Lee, D. H. Park, K. H. An, and W. S. Kim, “Electrical, Mechanical, and Thermal Characteristics of Nonwoven Fabric Heating Sheets Containing Chopped Carbon Fibers,” SN Applied Sciences2, no. 8 (2020): 1397, https://doi.org/10.1007/S42452-020-3004-9.
|
| [46] |
L. Xiong, F. Zhan, H. Liang, L. Chen, and D. Lan, “Chemical Grafting of Nano-TiO2 Onto Carbon Fiber via Thiol–Ene Click Chemistry and Its Effect on the Interfacial and Mechanical Properties of Carbon Fiber/Epoxy Composites,” Journal of Materials Science53, no. 4 (2018): 2594-2603, https://doi.org/10.1007/S10853-017-1739-5.
|
| [47] |
J. Sharma, Z. Demchuk, G. Polizos, et al., “Aligned Carbon Fibers-Carbon Nanotube-Polymer-Based Composite as Lithium-Ion Battery Current Collector,” Journal of Materials Processing Technology318 (2023): 118015, https://doi.org/10.1016/J.JMATPROTEC.2023.118015.
|
| [48] |
J. Sharma, R. Tao, G. Polizos, N. Kanbargi, B. LaRiviere, and J. Li, “A Lightweight and Metal-Free Current Collector for Battery Anode Applications,” Journal of Energy Storage79 (2024): 110161, https://doi.org/10.1016/J.EST.2023.110161.
|
| [49] |
C. Pang, G. Xu, W. An, et al., “Three-Component Functional Additive in a LiPF6-Based Carbonate Electrolyte for a High-Voltage LiCoO2/Graphite Battery System,” Energy Technology5, no. 11 (2017): 1979-1989, https://doi.org/10.1002/ENTE.201700118.
|
| [50] |
H. Xiang, J. Chen, and H. Wang, “Effect of Vinyl Ethylene Carbonate on the Compatibility Between Graphite and the Flame-Retarded Electrolytes Containing Dimethyl Methyl Phosphonate,” Ionics17, no. 5 (2011): 415-420, https://doi.org/10.1007/S11581-011-0527-5.
|
| [51] |
V. K. Tomer, O. A. T. Dias, A. M. Gouda, R. Malik, and M. Sain, “Advancing Lithium–Sulfur Battery Efficiency: Utilizing a 2D/2D g-C3N4@MXene Heterostructure to Enhance Sulfur Evolution Reactions and Regulate Polysulfides Under Lean Electrolyte Conditions,” Materials Horizons11, no. 13 (2024): 3090-3103, https://doi.org/10.1039/D4MH00200H.
|
| [52] |
V. K. Tomer, R. L. Kumawat, O. A. Titton Dias, R. Malik, G. C. Schatz, and M. Sain, “Synergistic Design of g-C3N4-Supported Cnts: Experimental and DFT Insights for Enhanced Electrochemical Performance in Flexible Li–S Batteries,” Journal of Materials Chemistry A12, no. 26 (2024): 15814-15828, https://doi.org/10.1039/D4TA00918E.
|
| [53] |
C. Gao, J. Zhou, G. Liu, and L. Wang, “Microwave-Assisted Synthesis and Surface Decoration of LiFePO4 Hexagonal Nanoplates for Lithium-Ion Batteries With Excellent Electrochemical Performance,” Journal of Materials Science52, no. 3 (2017): 1590-1602, https://doi.org/10.1007/S10853-016-0453-Z.
|
| [54] |
X. Wang, Z. Feng, X. Hou, et al., “Fluorine Doped Carbon Coating of LiFePO4 as a Cathode Material for Lithium-Ion Batteries,” Chemical Engineering Journal379 (2020): 122371, https://doi.org/10.1016/J.CEJ.2019.122371.
|
| [55] |
C. Li, Y. Xie, N. Zhang, et al., “Optimization of LiFePO 4 Cathode Material Based on Phosphorus Doped Graphite Network Structure for Lithium Ion Batteries,” Ionics25, no. 3 (2019): 927-937, https://doi.org/10.1007/S11581-018-2744-7.
|
| [56] |
O. A. T. Dias, F. Azarnia, K. Rathi, V. Pakharenko, V. K. Tomer, and M. Sain, “Rational Design of Dual-Ion Doped Cobalt-Free Li-Rich Cathode Materials for Enhanced Cycle Stability of Lithium-Ion Pouch Cell Batteries,” Nanoscale16 (2024): 16003-16014, https://doi.org/10.1039/D4NR01489H.
|
| [57] |
J. Y. Shih, G. Y. Lin, Y. J. J. Li, et al., “Operando Investigation on the Fast Two-Phase Transition Kinetics of LiFePO4/C Composite Cathodes With Carbon Additives for Lithium-Ion Batteries,” Electrochimica Acta419 (2022): 140356, https://doi.org/10.1016/J.ELECTACTA.2022.140356.
|
| [58] |
K. Kaneko, M. Li, and S. Noda, “Appropriate Properties of Carbon Nanotubes for the Three-Dimensional Current Collector in Lithium-Ion Batteries,” Carbon Trends10 (2023): 100245, https://doi.org/10.1016/J.CARTRE.2022.100245.
|
| [59] |
Y. Yang, J. Xia, X. Guan, et al., “In Situ Growth of CoP Nanosheet Arrays on Carbon Cloth as Binder-Free Electrode for High-Performance Flexible Lithium-Ion Batteries,” Small18, no. 51 (2022): 2204970, https://doi.org/10.1002/SMLL.202204970.
|
| [60] |
A. Hu, W. Chen, F. Li, et al., “Nonflammable Polyfluorides-Anchored Quasi-Solid Electrolytes for Ultra-Safe Anode-Free Lithium Pouch Cells Without Thermal Runaway,” Advanced Materials35, no. 51 (2023): 2304762, https://doi.org/10.1002/ADMA.202304762.
|
| [61] |
F. Wu, G. T. Kim, T. Diemant, et al., “Reducing Capacity and Voltage Decay of Co-Free Li1.2Ni0.2Mn0.6O2 as Positive Electrode Material for Lithium Batteries Employing an Ionic Liquid-Based Electrolyte,” Advanced Energy Materials10, no. 34 (2020): 2001830, https://doi.org/10.1002/AENM.202001830.
|
| [62] |
X. Tang, G. Zhang, X. Wang, et al., “Investigating the Critical Characteristics of Thermal Runaway Process for LiFePO4/Graphite Batteries by a Ceased Segmented Method,” iScience24, no. 10 (2021): 103088, https://doi.org/10.1016/J.ISCI.2021.103088.
|
| [63] |
R. Malik, V. K. Tomer, and M. Sain, “Analytical Techniques for Studying Cell Aging in Lithium–Sulfur Batteries,” EES Batteries1, no. 1 (2025): 119-152, https://doi.org/10.1039/D4EB00006D.
|
| [64] |
J. Zhang, H. Yu, X. Zhang, et al., “Surface Chemistry of LiFePO4 Cathode Material as Unraveled by HRTEM and XPS,” Ionics27, no. 1 (2021): 31-37, https://doi.org/10.1007/S11581-020-03814-Z/.
|
| [65] |
Y. Zhu, J. Zhu, B. Jiang, X. Wang, X. Wei, and H. Dai, “Insights on the Degradation Mechanism for Large Format Prismatic graphite/LiFePO4 Battery Cycled Under Elevated Temperature,” Journal of Energy Storage60 (2023): 106624, https://doi.org/10.1016/J.EST.2023.106624.
|
| [66] |
W. Jiang, G. Zhang, and J. Deng, “Comparable Investigation of Phosphorus-Based Flame Retardant Electrolytes on LiFePO4 Cathodes,” Journal of the Electrochemical Society169, no. 5 (2022): 050532, https://doi.org/10.1149/1945-7111/AC707E.
|
| [67] |
A. Moretti, D. V. Carvalho, N. Ehteshami, et al., “A Post-Mortem Study of Stacked 16 Ah Graphite//LiFePO4 Pouch Cells Cycled at 5°C,” Batteries5, no. 2 (2019): 45, https://doi.org/10.3390/BATTERIES5020045.
|
| [68] |
X. Shen, T. Hu, Y. Zeng, X. Huang, P. Zhang, and J. Zhao, “Core-Shell Structured Gel Polymer Electrolyte With Single-Ion Conducting and Thermal Stability Bifunction for Lithium-Ion Batteries,” Journal of the Electrochemical Society169, no. 7 (2022): 070505, https://doi.org/10.1149/1945-7111/AC79D5.
|
| [69] |
S. Lenus, P. Thakur, S. S. Samantaray, T. N. Narayanan, and Z. Dai, “Two-Dimensional Iron Phosphorus Trisulfide as a High-Capacity Cathode for Lithium Primary Battery,” Molecules28, no. 2 (2023): 537, https://doi.org/10.3390/MOLECULES28020537.
|
| [70] |
Q. Chen, H. Liu, J. Hu, L. Wang, Y. Li, and Y. Yao, “Nitrogen-Doped Carbon Layer of LiFePO4 Improves the Electrochemical Performance for Lithium Ion Batteries,” Ionics29, no. 11 (2023): 4537-4545, https://doi.org/10.1007/S11581-023-05188-4.
|
| [71] |
S. Qi, J. He, J. Liu, et al., “Phosphonium Bromides Regulating Solid Electrolyte Interphase Components and Optimizing Solvation Sheath Structure for Suppressing Lithium Dendrite Growth,” Advanced Functional Materials31, no. 11 (2021): 2009013, https://doi.org/10.1002/ADFM.202009013.
|
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2025 The Author(s). Battery Energy published by Xijing University and John Wiley & Sons Australia, Ltd.