Pustovgar Elizaveta, Sangodkar Rahul P, Andreev Andrey S, Palacios Marta, Chmelka Bradley F, Flatt Robert J, d'Espinose de Lacaillerie Jean-Baptiste
Institute for Building Materials, Department of Civil, Environmental and Geomatic Engineering, ETH Zürich 8093, Switzerland.
Department of Chemical Engineering, University of California, Santa Barbara, California 93106, USA.
Nat Commun. 2016 Mar 24;7:10952. doi: 10.1038/ncomms10952.
Silicate hydration is prevalent in natural and technological processes, such as, mineral weathering, glass alteration, zeolite syntheses and cement hydration. Tricalcium silicate (Ca3SiO5), the main constituent of Portland cement, is amongst the most reactive silicates in water. Despite its widespread industrial use, the reaction of Ca3SiO5 with water to form calcium-silicate-hydrates (C-S-H) still hosts many open questions. Here, we show that solid-state nuclear magnetic resonance measurements of (29)Si-enriched triclinic Ca3SiO5 enable the quantitative monitoring of the hydration process in terms of transient local molecular composition, extent of silicate hydration and polymerization. This provides insights on the relative influence of surface hydroxylation and hydrate precipitation on the hydration rate. When the rate drops, the amount of hydroxylated Ca3SiO5 decreases, thus demonstrating the partial passivation of the surface during the deceleration stage. Moreover, the relative quantities of monomers, dimers, pentamers and octamers in the C-S-H structure are measured.
硅酸盐水化在自然和技术过程中普遍存在,例如矿物风化、玻璃蚀变、沸石合成和水泥水化。硅酸三钙(Ca3SiO5)是波特兰水泥的主要成分,是水中反应活性最高的硅酸盐之一。尽管其在工业上广泛应用,但Ca3SiO5与水反应形成硅酸钙水合物(C-S-H)仍存在许多悬而未决的问题。在此,我们表明,对富含(29)Si的三斜晶Ca3SiO5进行固态核磁共振测量,能够根据瞬态局部分子组成、硅酸盐水化程度和聚合作用对水化过程进行定量监测。这为表面羟基化和水合物沉淀对水化速率的相对影响提供了见解。当速率下降时,羟基化Ca3SiO5的量减少,从而证明在减速阶段表面发生了部分钝化。此外,还测量了C-S-H结构中单体、二聚体、五聚体和八聚体的相对含量。