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We study the conductive heat transport through calcium silicate hydrate (C-S-H) and organically cross-linked C-S-H via experiments, micromechanical homogenization theory, and molecular simulations. We find that C-S-H's intrinsic thermal conductivity falls below its amorphous limit when cross-linked with short-chain organosilanes. The observed reduction correlates with the alkyl chain length of the bis-organosilane molecule. To understand the underlying fundamental molecular processes accountable for such a reduction, we construct realistic molecular structures of cross-linked C-S-H and validate them against the spectroscopic and pycnometery measurements. The atomistic simulations indicate that the reduction in the contribution of propagons (propagating heat carriers) and diffusons (diffusive heat carriers) to heat transport, and the amplification of locons (localized vibrational modes), are the main driving factors allowing to limit the heat conduction in C-S-H. Presented findings offer new potential directions to nanoengineering novel admixtures for cement composites and resilient lightweight cementitious mesostructures for thermally efficient building envelopes.more » « lessFree, publicly-accessible full text available December 1, 2024
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El Awad, Santiago ; Stefaniuk, Damian ; Krakowiak, Konrad J. ( , Mechanics of Materials)null (Ed.)