The
incorporation of carbon-fixing materials such as photosynthetic
algae in concrete formulations offers a promising strategy toward
mitigating the concerningly high carbon footprint of cement. Prior
literature suggests that the introduction of up to 0.5 wt % chlorella
biological matter (biomatter) in ordinary Portland cement induces
a retardation of the composite cement’s strength evolution
while enabling a long-term compressive strength comparable to pure
cement at a lower carbon footprint. In this work, we provide insights
into the fundamental mechanisms governing this retardation effect
and reveal a concentration threshold above which the presence of biomatter
completely hinders the hydration reactions. We incorporate Chlorella or Spirulina, two algal species
with different morphology and composition, in ordinary Portland cement
at concentrations ranging between 0.5 and 15 wt % and study the evolution
of mechanical properties of the resulting biocomposites over a period
of 91 days. The compressive strength in both sets of biocomposites
exhibits a concentration-dependent long-term drastic reduction, which
plateaus at 5 wt % biomatter content. At and above 5 wt %, all biocomposites
show a strength reduction of more than 80% after 91 days of curing
compared to pure cement, indicating a permanent hindrance effect on
hardening. Characterization of the hydration kinetics and the cured
materials shows that both algal biomatters hinder the hydration reactions
of calcium silicates, preventing the formation of calcium hydroxide
and calcium silicate hydrate, while the secondary reactions of tricalcium
aluminate that form ettringite are not affected. We propose that the
alkaline conditions during cement hydration lead to the formation
of charged glucose-based carbohydrates, which subsequently create
a hydrogen bonding network that ultimately encapsulates calcium silicates.
This encapsulation prevents the formation of primary hydrate products
and thus blocks the hardening of cement. Furthermore, we observe new
hydration products with composition and micromorphology deviating
from the expected hardened cement compounds. Our analysis provides
fundamental insights into the mechanisms that govern the introduction
of two carbon-negative algal species as fillers in cement, which are
crucial for enabling strategies to overcome the detrimental effects
that those fillers have on the mechanical properties of cement.