Growing interest in CO2 injection during mixing stems from its coupled impacts on early-age properties and CO2 uptake. Here we elucidate the rheological response by quantifying how interparticle interactions govern this effect. We combined rheological measurements with zeta potential analysis, atomic force microscopy (AFM) pull-off force mapping, inductively coupled plasma optical emission spectrometry (ICP-OES) and pH characterization of pore solution, thermogravimetric analysis (TGA), transmission electron microscopy (TEM), low-field proton nuclear magnetic resonance (1H NMR), and interparticle-force simulations using Hamaker 2.2. Results show that CO2 injection decreases particle zeta potential by 22.5 %–64.7 % via carbonate precipitation and ionic enrichment, weakening electrostatic repulsion while strengthening van der Waals attraction and promoting carbonate bridging. Consequently, a rigid flocculated network forms, raising yield stress (∼41.3 % under pure CO2 injection) and apparent viscosity. Under shear, the reduced energy barrier facilitates bond rupture and agglomerate breakdown, resulting in lower plastic viscosity. In parallel, early hydration is retarded, slowing structural build-up, illustrating 37.5 % reduction in storage modulus. These findings establish a mechanistic link between early-age carbonation, interparticle forces, and macroscopic rheology, and provide guidance for optimizing CO2 injection to balance flowability and CO2 uptake in low-carbon cementitious materials.
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