This study investigated the nature of hydration products of white portland cement (WPC) containing 20 mM malic acid or 1 M calcium chloride hydrated for 11 years. The study identiifed the hydration products and characterized the chemical composition, morphology, micro/nano structure of C-S-H and the main binding phase in cementitious materials. Calcium hydroxide (CH), ettringite and C-S-H were identiifed in WPC with 20 mM malic acid paste hydrated for 11 years. WPC with 1 M calcium chloride paste hydrated for 11 years contained the same phases, but with less CH, and the presence of Friedel’s salt (Ca2Al(OH)6Cl·2H2O). There were still small amount of anhydrous cement particles remaining in both pastes after 11 years hydration according to the SEM and29Si MAS NMR results. The hydration products of paste containing malic acid had a lower porosity than those prepared with calcium chloride upon visual inspection under SEM. The morphology of the outer product (Op) C-S-H was coarse ifbrillar and the inner product (Ip) C-S-H had a very ifne microstructure in both pastes under TEM. Both Ip and Op C-S-H formed in paste containing malic acid had lower Ca/Si and higher Al/Si than those in paste containing calcium chloride. C-S-H in paste containing calcium chloride had longer MCL and less percentage of bridging tetrahedra occupied by aluminum in silicon/aluminum chains due to relatively lessQ1 and moreQ2. A new type of silicon tetrahedra,Q2B, was introduced during deconvolution of29Si MAS NMR results. Ip and Op C-S-H in both pastes had aluminum substituted tobermorite-type and jennite-type structure, and all the charges caused by aluminum substituting silicon bridging tetrahedra were balanced by Ca2+.
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