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Correlation between the Dynamics of Nanoconfined Water and the Local Chemical Environment in Calcium Silicate Hydrate Nanominerals
Author(s) -
Musumeci Valentina,
Goracci Guido,
Sanz Camacho Paula,
Dolado Jorge S.,
Aymonier Cyril
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202100098
Subject(s) - chemistry , hydrate , solvation , silicate , molecular dynamics , rotational dynamics , calcium silicate hydrate , supercritical fluid , calcium silicate , hydrogen bond , relaxation (psychology) , molecule , calcium , chemical engineering , chemical physics , crystallography , computational chemistry , organic chemistry , materials science , cement , psychology , social psychology , engineering , metallurgy
Calcium silicate hydrates are members of a large family of minerals with layered structures containing pendant CaOH and SiOH groups that interact with confined water molecules. To rationalize the impact of the local chemical environment on the dynamics of water, SiOH‐ and CaOH‐rich model nanocrystals were synthesized by using the continuous supercritical hydrothermal method and then systematically studied by a combination of spectroscopic techniques. In our comprehensive analysis, the ultrafast relaxation dynamics of hanging hydroxy groups can be univocally assigned to CaOH or SiOH environments, and the local chemical environment largely affects the H‐bond network of the solvation water. Interestingly, the ordered “ice‐like” solvation water found in the SiOH‐rich environments is converted to a disordered “liquid‐like” distribution in the CaOH‐rich environment. This refined picture of the dynamics of confined water and hydroxy groups in calcium silicate hydrates can also be applied to other water‐containing materials, with a significant impact in many fields of materials science.