Nanocrystalline
calcium silicate hydrate (C–S–H)
is the binding phase of many low-CO2 cements. Understanding
its structure–mechanical properties relationship is critical
in designing sustainable concrete. For the first time, a similar basal
spacing (only 0.17 Å variation) of C–S–Hs at Ca/Si
ratios of 0.8–1.5 is prepared via coprecipitation. The C–S–H
nanostructure is determined using X-ray absorption spectroscopy, and
the intrinsic nanomechanical properties of C–S–H at
various Ca/Si are measured using high-pressure X-ray diffraction.
For the first time, the influence of basal spacing on the nanomechanical
properties is eliminated. At similar basal spacing, the ab-planar incompressibility remains independent of Ca/Si and silicate
chain length, while the c-axis incompressibility
is governed by the interlayer density (i.e., interlayer Ca content).
The bulk modulus of C–S–H is governed by the interlayer
densitymore interlayer Ca yields higher bulk modulus at comparable
basal spacings. Our results show that coprecipitated C–S–Hs
at higher Ca/Si have higher mechanical properties. The results have
implications in designing green cement/concrete using bottom-up approaches
by providing property inputs for multiscale simulation and references
for validating computational methods/parameters.