Kinetic Evolution Of The Internal Flocculation-linkage Network Within Cementitious Materials Subjected To Coupled Hydration-carbonation Mechanisms

Author

• Hengrui Liu
• Kaiyin Zhao
• Shipeng Zhang
• Shuangshuang Liu
• Hanghua Zhang
• Guangqi Xiong
• Zhenlin Li
• Qi Deng
• Hongyan Ma, Missouri University of Science and TechnologyFollow
• Kamal Khayat, Missouri University of Science and TechnologyFollow
• Chi Sun Poon

Abstract

This study systematically investigates the dynamic evolution of the microstructure and the flocculation-linkage network in cementitious materials under the competitive hydration and carbonation. Findings reveal that the governing mechanism of CO₂ on paste rheological behavior stems from the coupled effects of multiple factors: the physical packing of solid products (hydration products and nano-CaCO₃), the alteration of pore solution chemistry, and the dynamic partitioning of physically and chemically bound water. To elucidate the microstructural origins of rheological transitions of CO₂-mixed paste deeply, this research establish the concept of the "Flocculation-particle-linkage Unit (FPL unit)" based on Improved Particle Linkage(IPL) theory and flocculation concept. Analysis demonstrates that the time-dependent characteristics of physicochemical linkages within the FPL unit dominate the macroscopic evolution of the CO₂-mixed paste network. Notably, the reinforcing effect of linkage strength on the overall network is significantly enhanced during the acceleration period. In-depth characterization further divides the spatiotemporal evolution of the network linkage number into three characteristic stages: (i) the initial skeleton formation stage (0–1 h), where J1 and J2 linkage clusters dominate the construction of the initial topological framework; (ii) the network strengthening stage (1–3 h), characterized by a rapid surge in linkage density; and (iii) the solid matrix transformation stage (3–4 h), wherein the flocculated framework irreversibly transforms into a hardened matrix. Finally, this study establishes a quantitative correlation model between the compositional features of FPL units and macroscopic rheological parameters, precisely identifying the key micro-phase parameters that drive rheological transitions of CO₂-mixed paste.

Recommended Citation

H. Liu and K. Zhao and S. Zhang and S. Liu and H. Zhang and G. Xiong and Z. Li and Q. Deng and H. Ma and K. Khayat and C. S. Poon, "Kinetic Evolution Of The Internal Flocculation-linkage Network Within Cementitious Materials Subjected To Coupled Hydration-carbonation Mechanisms," Cement and Concrete Composites, vol. 173, article no. 106761, Elsevier, Oct 2026.

The definitive version is available at https://doi.org/10.1016/j.cemconcomp.2026.106761

Department(s)

Civil, Architectural and Environmental Engineering

Publication Status

Full Text Access

Keywords and Phrases

Carbon dioxide; Flocculation structure; FPL unit; Particle linkage; Rheological behavior

International Standard Serial Number (ISSN)

0958-9465

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2026 Elsevier, All rights reserved.

Publication Date

01 Oct 2026