<p>In-situ growth of polymer has shown great promise in smart rheology control of cement-based materials, a critical demand for ‘construction-of-the-future’ applications. However, its mechanistic role in governing time-evolving rheology of cement paste remains unclear. Here, we show this role by investigating in-situ polymerization in cement pastes under varying initiator concentrations, revealing how polymer chain growth modulates rheological behaviors. Yield stress development is governed by the kinetics of in-situ polymerization and proceeds through two stages: an initial stage dominated by the increasing polymer concentration from polymerization, and a subsequent stage driven by polymer chain growth. Unexpectedly, longer polymer chains do not always enhance interparticle forces through bridging effect. Once chain length exceeds a critical threshold (~750 kDa), polymers adopt more contracted conformations, leading to self-shielding of potential adsorption sites for bridging contacts and increased particle separation distances, thereby diminishing attractive interparticle interactions. This result highlights a delicate balance between bridging-induced attraction and steric-induced repulsion in determining rheology of cement paste.</p>

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In-situ growth of polymer drives time-evolving rheology of cement paste

  • Zhaoyang Sun,
  • Zixuan Yang,
  • Bin Xu,
  • Binmeng Chen

摘要

In-situ growth of polymer has shown great promise in smart rheology control of cement-based materials, a critical demand for ‘construction-of-the-future’ applications. However, its mechanistic role in governing time-evolving rheology of cement paste remains unclear. Here, we show this role by investigating in-situ polymerization in cement pastes under varying initiator concentrations, revealing how polymer chain growth modulates rheological behaviors. Yield stress development is governed by the kinetics of in-situ polymerization and proceeds through two stages: an initial stage dominated by the increasing polymer concentration from polymerization, and a subsequent stage driven by polymer chain growth. Unexpectedly, longer polymer chains do not always enhance interparticle forces through bridging effect. Once chain length exceeds a critical threshold (~750 kDa), polymers adopt more contracted conformations, leading to self-shielding of potential adsorption sites for bridging contacts and increased particle separation distances, thereby diminishing attractive interparticle interactions. This result highlights a delicate balance between bridging-induced attraction and steric-induced repulsion in determining rheology of cement paste.