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Peer-reviewedCC BY-NC-ND 4.0Journal of Power Sources

Influence of aqueously synthesized polyacrylic acid binder content on the processing and cycling of Si–Gr anodes

Abstract

Polyacrylic acid (PAA) is an emerging binder for silicon–graphite (Si–Gr) composite anodes due to its strong affinity for the native SiOx layer that covers Si particles and its ability to act as an artificial solid–electrolyte interphase (SEI). Here, PAA with a high molecular weight (Mw = 845 kg mol−1) is synthesized using a green, aqueous route. The effect of varying PAA content (from ⁓3 to 15 wt%) on electrode processing, physical properties, and cycling stability is systematically investigated. Increasing PAA concentration improves slurry stability and dispersion, widening the electrode processability window. X-ray photoelectron spectroscopy (XPS) confirms that PAA preferentially localizes on the silicon surface, with evidence of agglomeration at higher concentrations. An optimal PAA content of 10.6 wt% delivers the highest reversible specific capacity and good cycling stability (1270 mAh gelectrode−1 at the 50th cycle in half cell and 860 mAh gelectrode−1 in full cell). Lower PAA content results in deficient binder networks and increased irreversible capacity, while excessive binder content leads to binder agglomeration and increased resistivity. Post-mortem solid-state NMR analysis further supports the role of PAA as an artificial SEI, mitigating uncontrolled electrolyte decomposition and lithium loss.

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BibTeX
@article{herkendaal2026influence,
  title = {{Influence of aqueously synthesized polyacrylic acid binder content on the processing and cycling of Si–Gr anodes}},
  author = {Natalie Herkendaal and Nicolas Dupré and Jean-Marc Suau and Thomas Devic and Bernard Lestriez and Lionel Roué},
  journal = {Journal of Power Sources},
  year = {2026},
  month = oct,
  doi = {10.1016/j.jpowsour.2026.240358},
  url = {https://hal.science/hal-05685988v2},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - JOUR
TI  - Influence of aqueously synthesized polyacrylic acid binder content on the processing and cycling of Si–Gr anodes
AU  - Natalie Herkendaal
AU  - Nicolas Dupré
AU  - Jean-Marc Suau
AU  - Thomas Devic
AU  - Bernard Lestriez
AU  - Lionel Roué
PY  - 2026
DA  - 2026/10/08
JO  - Journal of Power Sources
DO  - 10.1016/j.jpowsour.2026.240358
UR  - https://hal.science/hal-05685988v2
AB  - Polyacrylic acid (PAA) is an emerging binder for silicon–graphite (Si–Gr) composite anodes due to its strong affinity for the native SiOx layer that covers Si particles and its ability to act as an artificial solid–electrolyte interphase (SEI). Here, PAA with a high molecular weight (Mw = 845 kg mol−1) is synthesized using a green, aqueous route. The effect of varying PAA content (from ⁓3 to 15 wt%) on electrode processing, physical properties, and cycling stability is systematically investigated. Increasing PAA concentration improves slurry stability and dispersion, widening the electrode processability window. X-ray photoelectron spectroscopy (XPS) confirms that PAA preferentially localizes on the silicon surface, with evidence of agglomeration at higher concentrations. An optimal PAA content of 10.6 wt% delivers the highest reversible specific capacity and good cycling stability (1270 mAh gelectrode−1 at the 50th cycle in half cell and 860 mAh gelectrode−1 in full cell). Lower PAA content results in deficient binder networks and increased irreversible capacity, while excessive binder content leads to binder agglomeration and increased resistivity. Post-mortem solid-state NMR analysis further supports the role of PAA as an artificial SEI, mitigating uncontrolled electrolyte decomposition and lithium loss.
SN  - 0378-7753
SN  - 1873-2755
ER  -