A Fluorine-free Polysulfone-Polyamide-Polyimide Copolymer Binder for LiNi0.8Co0.1Mn0.1O2 Cathode in Lithium-ion Battery

Hao Peng; Lin Liu; Qiao Zhang; Shuhao Liu; Man Lin; Hao Li; Yonghong Deng; Chuanlai Jiao; Chaoyang Wang; Hongli Xu

doi:10.1007/s10118-025-3281-2

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A Fluorine-free Polysulfone-Polyamide-Polyimide Copolymer Binder for LiNi_0.8Co_0.1Mn_0.1O₂ Cathode in Lithium-ion Battery

RESEARCH ARTICLE | Updated：2025-07-15

- A Fluorine-free Polysulfone-Polyamide-Polyimide Copolymer Binder for LiNi_0.8Co_0.1Mn_0.1O₂ Cathode in Lithium-ion Battery
- Chinese Journal of Polymer Science Vol. 43, Issue 7, Pages: 1146-1154(2025)
- Affiliations：
  
  a.School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
  b.Department of Materials Science and Engineering, School of Innovation and Entrepreneurship, Institute of Innovative Materials, Southern University of Science and Technology, Shenzhen 518055, China
  c.Research Institute of Materials Science, South China University of Technology, Guangzhou 510640, China
- Author bio：
  
  jiaocl@sustech.edu.cn (C.L.J.)
  zhywang@scut.edu.cn (C.Y.W.)
  xuhl3@sustech.edu.cn (H.L.X.)
- Funds：
- DOI：10.1007/s10118-025-3281-2
  CLC：
- Received：30 October 2024，
  
  Revised：2024-11-29，
  
  Accepted：09 December 2024，
  
  Online First：10 February 2025，
  
  Published：01 July 2025
- Accepted：
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Peng, H.; Liu, L.; Zhang, Q.; Liu, S. H.; Lin, M.; Li, H.; Deng, Y. H.; Jiao, C. L.; Wang, C. Y.; Xu, H. L. A fluorine-free polysulfone-polyamide-polyimide copolymer binder for LiNi_0.8Co_0.1Mn_0.1O₂ cathode in lithium-ion battery. Chinese J. Polym. Sci. 2025, 43, 1146–1154 DOI: 10.1007/s10118-025-3281-2.

Hao Peng, Lin Liu, Qiao Zhang, et al. A Fluorine-free Polysulfone-Polyamide-Polyimide Copolymer Binder for LiNi_0.8Co_0.1Mn_0.1O₂ Cathode in Lithium-ion Battery[J]. Chinese Journal of Polymer Science, 2025, 43(7): 1146-1154. DOI: 10.1007/s10118-025-3281-2.
Peng, H.; Liu, L.; Zhang, Q.; Liu, S. H.; Lin, M.; Li, H.; Deng, Y. H.; Jiao, C. L.; Wang, C. Y.; Xu, H. L. A fluorine-free polysulfone-polyamide-polyimide copolymer binder for LiNi_0.8Co_0.1Mn_0.1O₂ cathode in lithium-ion battery. Chinese J. Polym. Sci. 2025, 43, 1146–1154 DOI: 10.1007/s10118-025-3281-2. DOI：

Hao Peng, Lin Liu, Qiao Zhang, et al. A Fluorine-free Polysulfone-Polyamide-Polyimide Copolymer Binder for LiNi_0.8Co_0.1Mn_0.1O₂ Cathode in Lithium-ion Battery[J]. Chinese Journal of Polymer Science, 2025, 43(7): 1146-1154. DOI: 10.1007/s10118-025-3281-2. DOI：

摘要

The coating on the surface of the NCM811@PVDF and NCM811@SPIO electrode are 12 nm and 3 nm

respectively. The uniform and continuous SPIO coating layer acts as a multifunctional protective layer on the surface of the NCM811 particles

effectively enhancing the stability of the cathode/electrolyte interface structure and suppressing side reactions at the electrode/electrolyte interface.

Abstract

High-voltage LiNi

0.8

0.1

(NCM811) cathodes are critical for enhancing the energy density of lithium-ion batteries (LIBs). The development of binders compatible with high-voltage NCM811 cathode materials is crucial to enhance the electrochemical performance of LIBs. However

the traditional fluoropolymer binder

poly(vinylidene difluoride)

(PVDF)

can potentially leach components or break down into poly(fluoroalkyl substances) (PFAS) chemicals

thereby contributing to PFAS contamination. A novel fluorine-free polymer

polysulfone-polyamide-polyimide (SPIO)

was designed and synthesized as a binder for NCM811 cathodes. The SPIO binder exhibits exceptional mechanical properties and superior electrochemical characteristics. The cathode film fabricated with SPIO demonstrated a remarkable delamination force of 8 N (390 N·m

–1

)

indicating robust adhesion. The Li||NCM811 cell incorporating the SPIO binder retained 80% of its initial capacity after 300 cycles at a current density of 0.2 C. In comparison

the control cells assembled with the PVDF binder retained only 52% of their capacities under the same cycling conditions. Furthermore

the SPIO binder exhibited improved compatibility with the electrolyte. Transmission electron microscopy analysis of the cathode films after 100 cycles revealed the formation of a uniform

dense

and continuous chemical-electrochemical interface (CEI) by the SPIO binder on the surface of the NCM811 particles

which significantly contributed to the enhancement of the electrochemical performance. These results highlight the potential of SPIO as an advanced binder material for high-performance lithium-ion batteries.

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references

Koech, A. K.; Mwandila, G.; Mulolani, F.; Mwaanga, P. Lithium-ion battery fundamentals and exploration of cathode materials: a review. South African J. Chem. Eng. 2024 , 50 , 321−339..

Armand, M.; Axmann, P.; Bresser, D.; Copley, M.; Edström, K.; Ekberg, C.; Guyomard, D.; Lestriez, B.; Novák, P.; Petranikova, M.; Porcher, W.; Trabesinger, S.; Wohlfahrt-Mehrens, M.; Zhang, H. Lithium-ion batteries – current state of the art and anticipated developments. J. Power Sources 2020 , 479 , 228708..

Kotal, M.; Jakhar, S.; Roy, S.; Sharma, H. K. Cathode materials for rechargeable lithium batteries: recent progress and future prospects. J. Energy Storage 2022 , 47 , 103534..

Yu, W.; Zhou, J.; Hu, J.; Shang, Z.; Zhou, X.; Xu, S. Exploring the energy and environmental sustainability of advanced lithium-ion battery technologies. Resour., Conserv. Recy. 2025 , 212 , 107963..

Ma, X. Z.; Zhu, H. R.; Xie, Z. L.; Ding, J.; Li, C. L. Research progress in modification of nickel-rich ternary cathode material LiNi 0.8 Co 0.1 Mn 0.1 O 2 for lithium-ion batteries. Mater. Sci. Forum 2021 , 1033 , 126−130..

Wu, Z.; Zhang, C.; Yuan, F.; Lyu, M.; Yang, P.; Zhang, L.; Zhou, M.; Wang, L.; Zhang, S.; Wang, L. Ni-rich cathode materials for stable high-energy lithium-ion batteries. Nano Energy 2024 , 126 , 109620..

Liang, G.; Zhu, J.; Chen, A.; Yang, Q.; Zhi, C. Adhesive and cohesive force matters in deformable batteries. Npj Flex. Electron. 2021 , 5 , 1−4..

Jeong, W. H.; Kim, H.; Kansara, S.; Lee, S.; Agostini, M.; Kim, K.; Hwang, J. Y.; Jung, Y. C. Stimulating the electrostatic interactions in composite cathodes using a slurry-fabricable polar binder for practical all-solid-state batteries. Energy Storage Mater . 2024 , 73, 103855..

Zhong, X.; Han, J.; Chen, L.; Liu, W.; Jiao, F.; Zhu, H.; Qin, W. Binding mechanisms of PVDF in lithium ion batteries. Appl. Surf. Sci. 2021 , 553 , 149564..

Xu, J.; Xiong, Q.; Liu, Q.; Jiang, Y.; Yue, X.; Yang, D.; Zhang, T.; Qiu, F. Sustainable recycling of waste poly(vinylidene fluoride) and rational design of Janus membrane with superhydrophilic/hydrophobic asymmetric wettability for efficient separation of surfactant-stabilized water-in-oil and oil-in-water emulsions. Colloid. Surface. A 2024 , 684 , 133237..

Veiga, A. G.; Dias, F. G. de A.; Batista, L. do N.; Rocco, M. L. M.; Costa, M. F. Reprocessed poly(vinylidene fluoride): a comparative approach for mechanical recycling purposes. Mater. Today Commun. 2020 , 25 , 101269..

Liu, T.; Parekh, R.; Mocny, P.; Bloom, B. P.; Zhao, Y.; An, S. Y.; Pan, B.; Yin, R.; Waldeck, D. H.; W hitacre, J. F.; Matyjaszewski, K. Tailored PVDF graft copolymers via ATRP as high-performance NCM811 cathode binders. ACS Mater. Lett. 2023 , 5 , 2594−2603..

Zhang, M.; Wang, L.; Xu, H.; Song, Y.; He, X. Polyimides as promising materials for lithium-ion batteries: a review. Nano-Micro Lett. 2023 , 15 , 135..

Bai, G. Y.; Sun, W. J.; Zhou, Y.; Li, J. T. Beyond binding: a review on binders in high-voltage transition metal oxide cathode of lithium ion battery. J. Energy Storage 2024 , 97 , 112816..

Zhang, Y.; Wang, C.; Yi, Y.; Wang, W.; Yang, J. Synthesis and properties of polyamide 6 random copolymers containing an aromatic imide structure. Polymers 2023 , 15 , 2812..

Park, G.; Park, J. S.; Kim, H. S.; Lee, K. J. Preparation of cathode slurry for lithium-ion battery by three-roll mill process. Carbon Lett. 2022 , 32 , 265–272..

Teo , J. H.; Strauss, F.; Tripković, Đ.; Schweidler, S.; Ma, Y.; Bianchini, M.; Janek, J.; Brezesinski, T. Design-of-experiments-guided optimization of slurry-cast cathodes for solid-state batteries. Cell Rep. Phys. Sci . 2021 , 2 , 100465..

Ryu, M.; Hong, Y. K.; Lee, S. Y.; Park, J. H. Ultrahigh loading dry-process for solvent-free lithium-ion battery electrode fabrication. Nat. Comm. 2023 , 14 , 1316..

Dai, F.; Cai, M. Best practices in lithium battery cell preparation and evaluation. Commun. Mater. 2022 , 3 , 64..

Xue, Z.; Guan, D.; Zeng, J.; Cao, Y.; Peng, Z.; Hu, G.; Du, K. Research on the assembly process of full coin cells: key factors affecting data reliability. Ionics 2023 , 29 , 5285−5293..

Fulmer, G. R.; Miller, A. J. M.; Sherden, N. H.; Gottlieb, H. E.; Nudelman, A.; Stoltz, B. M.; Bercaw, J. E.; Goldberg, K. I. NMR chemical shifts of trace impurities: common laboratory solvents, organics, and gases in deuterated solvents relevant to the organometallic chemist. Organometallics 2010 , 29 , 2176−2179..

Yan, J.; Zheng, Y.; Zhou, Y.; Liu, Y.; Tan, H.; Fu, Q.; Ding, M. Application of infrared spectroscopy in the multiscale structure characterization of poly(L-lactic acid). Polymer 2023 , 278 , 125985..

Elyashberg, M. Identification and structure elucidation by NMR spectroscopy. TrAC Trend. Anal. Chem. 2015 , 69 , 88−97..

Andoh, C. N.; Attiogbe, F.; Bonsu Ackerson, N. O.; Antwi, M.; Adu-Boahen, K. Fourier transform infrared spectroscopy: an analytical technique for microplastic identification and quantification. Infrared Phys. Techn. 2024 , 136 , 105070..

Fair, R. A.; Xie, R.; Lee, Y.; Colby, R. H.; Gomez, E. D. Molecular weight characterization of conjugated polymers through gel permeation chromatography and static light scattering. ACS Appl. Polym. Mater. 2021 , 3 , 4572−4578..

Hagiwara, H.; Endo, K.; Yukawa, Y. Design of dispersant in cathode of Li-ion batteries for cathode slurry with high solid content and high battery performance. Meet. Abstracts . 2023 , MA2023-01 , 534..

Qian, J.; Wiener, C. G.; Zhu, Y.; Vogt, B. D. Swelling and plasticization of polymeric binders by li-containing carbonate electrolytes using quartz crystal microbalance with dissipation. Polymer 2018 , 143 , 237−244..

Lößlein, S. M.; Merz, R.; Müller, D. W.; Kopnarski, M.; Mücklich, F. An in-depth evaluation of sample and measurement induced influences on static contact angle measurements. Sci. Rep. 2022 , 12 , 19389..

Akbari, R.; Antonini, C. Contact angle measurements: from existing methods to an open-source tool. Adv. Colloid Interfac. 2021 , 294 , 102470..

Deng, L.; Liu, J. K.; Wang, Z.; Lin, J. X.; Liu, Y. X.; Bai, G. Y.; Zheng, K. G.; Zhou, Y.; Sun, S. G.; Li, J. T. A formula to customize cathode binder for lithium ion battery. Adv. Energy Mater . 2024 , 14 , 2401514..

Halalay, I. C.; Lukitsch, M. J.; Balogh, M. P.; Wong, C. A. Nanoindentation testing of separators for lithium-ion batteries. J. Power Sources 2013 , 238 , 469−477..

Shishvan, S. S.; Fleck, N. A.; McMeeking, R. M.; Deshpande, V. S. Cracking and associated volumetric expansion of NMC811 secondary particles. J. Power Sources 2023 , 588 , 233745..

Ma, S.; Jiang, M.; Tao, P.; Song, C.; Wu, J.; Wang, J.; Deng, T.; Shang, W. Temperature effect and thermal impact in lithium-ion batteries: a review. Prog. Nat. Sci-Mater. 2018 , 28 , 653−666..

Drzeżdżon, J.; Jacewicz, D.; Sielicka, A.; Chmurzyński, L. Characterization of polymers based on differential scanning calorimetry based techniques. TrAC Trend. Anal. Chem. 2019 , 110 , 51−56..

Tsao, C. H.; Yang, T. K.; Chen, K. Y.; Fang, C. E.; Ueda, M.; Richter, F. H.; Janek, J.; Chiu, C.; Kuo, P. L. Comparing the ion-conducting polymers with sulfonate and ether moieties as cathode binders for high-power lithium-ion batteries. ACS Appl. Mater. Interfaces 2021 , 13 , 9846−9855..

Wang, S.; Zhang, J.; Gharbi, O.; Vivier, V.; Gao, M.; Orazem, M. E. Electrochemical impedance spectroscopy. Nat. Rev. Method. Prime. 2021 , 1 , 1−21..

Wang, Y.; Dong, N.; Liu, B.; Tian, G.; Qi, S.; Wu, D. Self-adaptive gel poly (imide-siloxane) binder ensuring stable cathode-electrolyte interface for achieving high-performance NCM811 cathode in lithium-ion batteries. Energy Storage Mater. 2023 , 56 , 621−630..

Dees, D. W.; Kawauchi, S.; Abraham, D. P.; Prakash, J. Analysis of the galvanostatic intermittent titration technique (GITT) as applied to a lithium-ion porous electrode. J. Power Sources 2009 , 189 , 263−268..

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