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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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A Cellulose-Derived Polymer Additive for Stabilizing Thick Cathodes in All-Solid-State Batteries.

Tiantian Liu1,2, Rong-Hao Wang1, Shao-Xiong Yang1

  • 1School of Engineering Science, Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, CAS Key Laboratory of Mechanical Behavior and Design of Materials (LMBD), University of Science and Technology of China, Hefei, Anhui, People's Republic of China.

Angewandte Chemie (International Ed. in English)
|July 9, 2026
PubMed
Summary

A new cellulose-derived polymer additive (CA-MDI) enhances solid-solid interfacial contact in all-solid-state batteries (ASSBs). This improves cycling stability and energy density for advanced battery applications.

Keywords:
all solid‐state batteriescellulose‐derivate additiveinterfacial engineeringmultifunctional additivethick cathodes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • All-solid-state batteries (ASSBs) promise superior safety and energy density compared to conventional lithium-ion batteries.
  • Challenges in ASSBs include poor interfacial contact and processing limitations with solid-state electrolytes, hindering high active material loading.
  • Current methods like cold-pressing result in inadequate interfacial contact, limiting battery performance.

Purpose of the Study:

  • To develop a novel polymer additive that improves solid-solid interfacial contact in ASSB composite cathodes.
  • To ensure continuous electron and ion transport across the cathode-electrolyte interface.
  • To enhance the cycling stability and energy density of thick composite cathodes for high-performance ASSBs.

Main Methods:

  • Synthesis of a cellulose-derived polymer additive (CA-MDI) via polymerization of cellulose acetate (CA) and methylene diphenyl diisocyanate (MDI).
  • Incorporation of the CA-MDI additive into composite cathodes using high-nickel (LiNi0.89Co0.055Mn0.055O2) and other cathode materials (LiCoO2, Li-rich layered oxides).
  • Fabrication and electrochemical testing of all-solid-state batteries with CA-MDI modified and additive-free cathodes.

Main Results:

  • ASSBs with CA-MDI modified LiNi0.89Co0.055Mn0.055O2 cathodes achieved a high areal capacity of 6.4 mAh cm-2.
  • The modified cathodes delivered an initial discharge capacity of 136.6 mAh g-1 at 0.3C, retaining 91.1% after 100 cycles.
  • Long-term cycling at 1C showed sustained performance, with 80% capacity retention over 620 cycles for a 1.8 mAh cm-2 areal capacity cell.

Conclusions:

  • The cellulose-derived CA-MDI additive effectively establishes intimate solid-solid interfacial contact and ensures continuous transport in composite cathodes.
  • CA-MDI significantly improves the cycling stability of thick composite cathodes, overcoming limitations of conventional processing methods.
  • This mechanically adaptive polymer additive presents a viable strategy for developing high-energy-density and stable all-solid-state batteries.