Calcium silicate hydrate (C(-A)-S-H) and its aluminosilicate counterpart (C-A-S-H) constitute the principal binding phases in Portland cement and blended systems, governing mechanical strength and durability. This paper presents a summary of the work related to dehydration of C(-A)-S-H and rehydration of dehydrated C(-A)-S-H. Their thermal dehydration, a key process for cement recycling, induces profound multi-scale transformations: at the atomic level, it alters calcium and aluminum coordination environments and disrupts chemical bonding; at the chain-structure level, it causes depolymerization of the silicate/aluminosilicate networks; and at the microstructural level, it leads to changes in nanoscale particle morphology, aggregation state, and pore structure, creating a metastable, defect-rich, high-energy state distinct from the original C(-A)-S-H. The subsequent rehydration of this dehydrated C(-A)-S-H, which is not a simple reversal but a distinct dissolution–precipitation process, enables microstructural reconstruction and restored reactivity upon contact with water. This rehydration capacity is fundamentally exploited in thermally activated recycled cement—a novel binder concept that leverages dehydration-induced metastability for renewed strength development. Understanding these interconnected processes, influenced by factors like temperature, humidity, rate, and aluminum content, is critical for advancing sustainable cement technology, enabling the design of high-performance recycled cement and concrete, and facilitating the recycling of cementitious materials.
Wang et al. (Sat,) studied this question.