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Title: On the nature of structural disorder in calcium silicate hydrates with a calcium/silicon ratio similar to tobermorite

Abstract

Four calcium silicate hydrates (C-S-H) with structural calcium/silicon (Ca/Si) ratios ranging from 0.82 ± 0.02 to 0.87 ± 0.02 were synthesized at room temperature, 50, 80, and 110 °C. Their structure was elucidated by collating information from electron probe micro-analysis, transmission electron microscopy, extended X-ray absorption fine structure spectroscopy, and powder X-ray diffraction (XRD). A modeling approach specific to defective minerals was used because sample turbostratism prevented analysis using usual XRD refinement techniques (e.g. Rietveld analysis). It is shown that C-S-H with Ca/Si ratio of ∼ 0.8 are structurally similar to nano-crystalline turbostratic tobermorite, a naturally occurring mineral. Their structure thus consists of sheets of calcium atoms in 7-fold coordination, covered by ribbons of silicon tetrahedra with a dreierketten (wollastonite-like) organization. In these silicate ribbons, 0.42 Si per bridging tetrahedron are missing. Random stacking faults occur systematically between successive layers (turbostratic stacking). Layer-to-layer distance is equal to 11.34 Å. Crystallites have a mean size of 10 nm in the a–b plane, and a mean number of 2.6–2.9 layers stacked coherently along the c* axis.

Authors:
 [1]; ;  [1];  [2]; ;  [3];  [4];  [5];  [6]
  1. BRGM, 3, Avenue Claude Guillemin, 45060 Orléans Cedex 2 (France)
  2. CRMD, UMR 6619 – CNRS, 1b rue de la férollerie, 45071 Orléans Cedex 2 (France)
  3. Laboratory of Environmental Geology, Research Group of Geoenvironmental/Engineering Division of Solid Waste, Resources and Geoenvironmental/Engineering Graduate School of Engineering, Hokkaido University, Kita 13 Nishi 8, Sapporo 060-8628 (Japan)
  4. Faculty of Integrated Arts and Sciences, The University of Tokushima, 1-1, Minami-Josanjima, Tokushima, 770-8502 (Japan)
  5. ANDRA, Centre de Meuse/Haute Marne, 55290 Bure (France)
  6. ISTerre, Grenoble University, CNRS, F-38041 Grenoble (France)
Publication Date:
OSTI Identifier:
22220811
Resource Type:
Journal Article
Journal Name:
Cement and Concrete Research
Additional Journal Information:
Journal Volume: 52; Other Information: Copyright (c) 2013 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0008-8846
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; ABSORPTION SPECTROSCOPY; CALCIUM; CALCIUM SILICATES; ELECTRON MICROPROBE ANALYSIS; FINE STRUCTURE; HYDRATES; LAYERS; NANOSTRUCTURES; POWDERS; SILICON; SIMULATION; STACKING FAULTS; TRANSMISSION ELECTRON MICROSCOPY; X-RAY DIFFRACTION; X-RAY SPECTROSCOPY

Citation Formats

Grangeon, Sylvain, E-mail: S.Grangeon@brgm.fr, Claret, Francis, Lerouge, Catherine, Warmont, Fabienne, Sato, Tsutomu, Anraku, Sohtaro, Numako, Chiya, Linard, Yannick, and Lanson, Bruno. On the nature of structural disorder in calcium silicate hydrates with a calcium/silicon ratio similar to tobermorite. United States: N. p., 2013. Web. doi:10.1016/J.CEMCONRES.2013.05.007.
Grangeon, Sylvain, E-mail: S.Grangeon@brgm.fr, Claret, Francis, Lerouge, Catherine, Warmont, Fabienne, Sato, Tsutomu, Anraku, Sohtaro, Numako, Chiya, Linard, Yannick, & Lanson, Bruno. On the nature of structural disorder in calcium silicate hydrates with a calcium/silicon ratio similar to tobermorite. United States. doi:10.1016/J.CEMCONRES.2013.05.007.
Grangeon, Sylvain, E-mail: S.Grangeon@brgm.fr, Claret, Francis, Lerouge, Catherine, Warmont, Fabienne, Sato, Tsutomu, Anraku, Sohtaro, Numako, Chiya, Linard, Yannick, and Lanson, Bruno. Tue . "On the nature of structural disorder in calcium silicate hydrates with a calcium/silicon ratio similar to tobermorite". United States. doi:10.1016/J.CEMCONRES.2013.05.007.
@article{osti_22220811,
title = {On the nature of structural disorder in calcium silicate hydrates with a calcium/silicon ratio similar to tobermorite},
author = {Grangeon, Sylvain, E-mail: S.Grangeon@brgm.fr and Claret, Francis and Lerouge, Catherine and Warmont, Fabienne and Sato, Tsutomu and Anraku, Sohtaro and Numako, Chiya and Linard, Yannick and Lanson, Bruno},
abstractNote = {Four calcium silicate hydrates (C-S-H) with structural calcium/silicon (Ca/Si) ratios ranging from 0.82 ± 0.02 to 0.87 ± 0.02 were synthesized at room temperature, 50, 80, and 110 °C. Their structure was elucidated by collating information from electron probe micro-analysis, transmission electron microscopy, extended X-ray absorption fine structure spectroscopy, and powder X-ray diffraction (XRD). A modeling approach specific to defective minerals was used because sample turbostratism prevented analysis using usual XRD refinement techniques (e.g. Rietveld analysis). It is shown that C-S-H with Ca/Si ratio of ∼ 0.8 are structurally similar to nano-crystalline turbostratic tobermorite, a naturally occurring mineral. Their structure thus consists of sheets of calcium atoms in 7-fold coordination, covered by ribbons of silicon tetrahedra with a dreierketten (wollastonite-like) organization. In these silicate ribbons, 0.42 Si per bridging tetrahedron are missing. Random stacking faults occur systematically between successive layers (turbostratic stacking). Layer-to-layer distance is equal to 11.34 Å. Crystallites have a mean size of 10 nm in the a–b plane, and a mean number of 2.6–2.9 layers stacked coherently along the c* axis.},
doi = {10.1016/J.CEMCONRES.2013.05.007},
journal = {Cement and Concrete Research},
issn = {0008-8846},
number = ,
volume = 52,
place = {United States},
year = {2013},
month = {10}
}