Casar, ZigaMohamed, Aslam KunhiBowen, PaulScrivener, Karen2023-10-092023-10-092023-10-092023-09-0810.1021/acs.jpcc.3c03350https://infoscience.epfl.ch/handle/20.500.14299/201448WOS:001066132500001Deciphering the calcium silicate hydrate (C-S-H) surface is crucial for unraveling the mechanisms of cement hydration and property development. Experimental observations of C-S-H in cement systems suggest a surface termination which is fundamentally different from the silicate-terminated surface assumed in many atomistic level studies. Here, a new multiparameter approach to describing the (001) basal C-S-H surface is developed, which considers how the surface termination affects the overall properties (Ca/Si ratio, mean chain length, relative concentration of silanol and hydroxide groups). Contrary to current beliefs, it is concluded that the (001) C-S-H surface is dominantly calcium terminated. Finally, an adsorption mechanism for calcium and hydroxide ions is proposed, which is in agreement with the surface charge densities observed in previous studies.Chemistry, PhysicalNanoscience & NanotechnologyMaterials Science, MultidisciplinaryChemistryScience & Technology - Other TopicsMaterials Sciencec-s-hmolecular-dynamicscrystal-structuremodeladsorptionzetainterfaceshydroxidemicrostructuresimulationstext::journal::journal article::research article