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. 2025 Jul 24;10(30):33607-33618.
doi: 10.1021/acsomega.5c04052. eCollection 2025 Aug 5.

Multifunctionalized Conductive Polymers for Self-Healing Silicon Anodes in Li-Ion Batteries

Neslihan Yuca  1   2 , Omer Suat Taskin  1   3 , Emre Guney  1 , Javier García-Alonso  4 , David Maestre  4 , Bianchi Méndez  4
Affiliations

Multifunctionalized Conductive Polymers for Self-Healing Silicon Anodes in Li-Ion Batteries

Neslihan Yuca et al. ACS Omega. .

Abstract

Silicon is a very promising material for lithium-ion batteries (LIBs) due to its high theoretical capacity (3579 mAh/g). However, the volumetric expansion (300%) of silicon during lithiation led to pulverization of the electrode and rapid capacity fading. Self-healing (SH) materials are thought of as a solution for the degradation of active materials, enabling higher capacity retention. Here, we synthesized and integrated an autonomous self-healing poly-(aniline-co-3-aminophenylboronic acid)/PVA composite (SHC) as a binder in a Si anode electrode for LIBs. The synthesized SHC was investigated by Fourier transform infrared (FTIR) spectroscopy, thermogravimetric analysis, and elongation and conductivity tests. Si anodes were prepared with SHC and a PVP cobinder. In addition, Si anodes were prepared separately with PVDF and the CMC-SBR binder as control electrodes. The electrodes were electrochemically characterized by electrochemical impedance spectroscopy, cyclic voltammetry, and galvanostatic charge/discharge tests. The conductive SHC binder was successfully integrated into the Si anode, and a capacity of over 1700 mAh/g was obtained after 100 cycles at C/10, and 650 mAh/g was obtained after 200 cycles at C/2.

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Figures

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1
Schematic representation of the self-healing mechanism of the SHC binder.
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(a) Elongation test of poly­(aniline-co-3-aminophenylboronic acid)/PVA and (b) self-healing test of poly­(aniline-co-3-aminophenylboronic acid)/PVA.
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(a) FTIR spectrum of the synthesized PANI-co-PANI (boronic acid)/PVA (SHP); (b) shift of hydroxyl peaks in FTIR spectra after healing of PANI-co-PANI (boronic acid)/PVA; (c) tensile stress–strain curve of PANI-co-PANI­(boronic acid)/PVA, and (d) conductivity measurement of the SH polymer.
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Illustration of the current flow test for cut and healed SHP.
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XPS measurements of the (A) Si-SHC25 electrode, (B) Si-SHC10 electrode, (C) Si-CMC/SBR electrode, and (D) Si-PVDF electrode.
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Comparison of (a) EIS results with the equivalent circuit shown as an inset, (b) capacity–voltage graphs of electrodes at first cycles, (c) C-rate results, and (d) galvanostatic charge/discharge test results.
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(a) Cycling test of Si-SHC25 at different C rates, (b) CV measurements of Si-SHC25, and (c) comparison of EIS results of the cycled and uncycled Si-SHC25 electrodes.
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SEM images of the Si-SHC25 electrode (a) before cycling, (b) after cycling, (c) showing the self-healing bond region marked in (b). (d) EDS mapping of the electrode Si-SHC25 before cycling, and (e) EDS spectra of the Si-SHC25 electrode before and after cycling.
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References

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