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Peer-reviewedCC BY 4.0Advanced Science

Self‐Assembly of Organic–Inorganic Copolymers Toward Bio‐Inspired Cementitious Composites

  • Zonglin Xie1,2
  • Suning Li1,2
  • Fuwen Zhong1,2
  • Gongkun Xiang1,2
  • Mustapha Jamaa Garba1,2
  • Yi Tian1,2
  • Jun Wu3
  • Zhiwu Yu1,2
  • Qiang Yuan1,2
  1. 1School of Civil Engineering Central South University Changsha China
  2. 2National Engineering Research Center for High‐Speed Railway Construction Technology Changsha China
  3. 3China Railway Group Limited Beijing China
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Abstract

Refined by millions of years of rigorous evolution, highly mineralized biological materials have perfected organic–inorganic self‐assembly to break the traditional trade‐off between strength and damage tolerance. Their rigid‐flexible precursor architectures motivate an organic–inorganic copolymerization strategy for the bottom‐up design of cementitious materials, the most pervasive and resource‐intensive engineered products. Herein, as the primary binding phase in cement, calcium silicate hydrate (CSH) is copolymerized with thioctic acid (TA) into a hybrid precursor through a thermodynamically spontaneous process driven by Lewis acid‐base coordination (Ca2+‐COO−). Hot pressing promotes the synergistic evolution of amorphous CSH into a denser and structurally reorganized framework together with TA crosslinking, resulting in a self‐organized organic–inorganic nanocomposite that resembles the disordered collagen‐mineral architecture in trabecular bone. Notably, the poly(CSH‐TA) composite features a microphase‐homogeneous architecture that delivers an exceptional compressive strength of over 300 MPa at 10% strain. Even more impressively, we demonstrated the intrinsic physical reprocessibility of cementitious materials, allowing retention of over 80% of strength and energy absorption capacity through five consecutive powder‐to‐bulk cycles. The organic–inorganic copolymerization route opens a bioinspired pathway for next‐generation cementitious materials toward achieving multifunctional performance breakthroughs.

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Cite

BibTeXRIS
BibTeX
@article{xie2026selfassembly,
  title = {{Self‐Assembly of Organic–Inorganic Copolymers Toward Bio‐Inspired Cementitious Composites}},
  author = {Zonglin Xie and Suning Li and Fuwen Zhong and Gongkun Xiang and Mustapha Jamaa Garba and Yi Tian and Jun Wu and Zhiwu Yu and Qiang Yuan},
  journal = {Advanced Science},
  year = {2026},
  month = aug,
  doi = {10.1002/advs.77041},
  url = {https://doi.org/10.1002/advs.77041},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Self‐Assembly of Organic–Inorganic Copolymers Toward Bio‐Inspired Cementitious Composites
AU  - Zonglin Xie
AU  - Suning Li
AU  - Fuwen Zhong
AU  - Gongkun Xiang
AU  - Mustapha Jamaa Garba
AU  - Yi Tian
AU  - Jun Wu
AU  - Zhiwu Yu
AU  - Qiang Yuan
PY  - 2026
DA  - 2026/08/07
JO  - Advanced Science
DO  - 10.1002/advs.77041
UR  - https://doi.org/10.1002/advs.77041
AB  - Refined by millions of years of rigorous evolution, highly mineralized biological materials have perfected organic–inorganic self‐assembly to break the traditional trade‐off between strength and damage tolerance. Their rigid‐flexible precursor architectures motivate an organic–inorganic copolymerization strategy for the bottom‐up design of cementitious materials, the most pervasive and resource‐intensive engineered products. Herein, as the primary binding phase in cement, calcium silicate hydrate (CSH) is copolymerized with thioctic acid (TA) into a hybrid precursor through a thermodynamically spontaneous process driven by Lewis acid‐base coordination (Ca2+‐COO−). Hot pressing promotes the synergistic evolution of amorphous CSH into a denser and structurally reorganized framework together with TA crosslinking, resulting in a self‐organized organic–inorganic nanocomposite that resembles the disordered collagen‐mineral architecture in trabecular bone. Notably, the poly(CSH‐TA) composite features a microphase‐homogeneous architecture that delivers an exceptional compressive strength of over 300 MPa at 10% strain. Even more impressively, we demonstrated the intrinsic physical reprocessibility of cementitious materials, allowing retention of over 80% of strength and energy absorption capacity through five consecutive powder‐to‐bulk cycles. The organic–inorganic copolymerization route opens a bioinspired pathway for next‐generation cementitious materials toward achieving multifunctional performance breakthroughs.
SN  - 2198-3844
ER  -