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<p>Calcium silicate hydrate (C-S-H) and calcium hydroxide (CH, portlandite) are the dominant hydration products of Portland cement. However, the anisotropic layered CH and uncoordinated nucleation of C-S-H and CH severely restrict the macroscopic performance of cementitious materials. Here, we report a hydrogen-bond-regulated proton transfer strategy to mechanochemically synthesize a positively charged, isotropic disordered CH precursor (CHP_H<sup>+</sup>). This precursor serves as a growth-accelerating nucleus to trigger dual heterogeneous nucleation of CH and C-S-H, in situ forming a CH@C-S-H composite. Free energy calculations reveal that hydroxyl vacancies on CH surfaces drive spontaneous water adsorption to generate ≡Ca−OH<sub>2</sub><sup>+</sup> sites, which stabilize silicate clusters and promote composite growth. The resulting cementitious material shows accelerated hydration kinetics, higher hydration heat release, and greatly improved elastic modulus and compressive strength, delivering a 5.4-fold improvement in 12 h strength over the control. This work provides an atomic-scale design principle for advanced cementitious materials by reprogramming the nucleation and growth pathways of hydration products via protonation regulation.</p>

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Protonated portlandite precursor unlocks enhanced nucleation and growth for cement hydration

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月30日

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  • Jingyi Zeng,
  • Qiao Liu,
  • Jin Yang,
  • Zhongyong Zhang,
  • Huangjie Zou,
  • Ying Su,
  • Yingbin Wang,
  • Yubo Li,
  • Neng Li,
  • Xingyang He

摘要

Calcium silicate hydrate (C-S-H) and calcium hydroxide (CH, portlandite) are the dominant hydration products of Portland cement. However, the anisotropic layered CH and uncoordinated nucleation of C-S-H and CH severely restrict the macroscopic performance of cementitious materials. Here, we report a hydrogen-bond-regulated proton transfer strategy to mechanochemically synthesize a positively charged, isotropic disordered CH precursor (CHP_H+). This precursor serves as a growth-accelerating nucleus to trigger dual heterogeneous nucleation of CH and C-S-H, in situ forming a CH@C-S-H composite. Free energy calculations reveal that hydroxyl vacancies on CH surfaces drive spontaneous water adsorption to generate ≡Ca−OH2+ sites, which stabilize silicate clusters and promote composite growth. The resulting cementitious material shows accelerated hydration kinetics, higher hydration heat release, and greatly improved elastic modulus and compressive strength, delivering a 5.4-fold improvement in 12 h strength over the control. This work provides an atomic-scale design principle for advanced cementitious materials by reprogramming the nucleation and growth pathways of hydration products via protonation regulation.