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Title: In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration

Abstract

The understanding and control of early hydration of tricalcium silicate (C3S) is of great importance to cement science and concrete technology. However, traditional characterization methods are incapable of providing morphological and spectroscopic information about in situ hydration at the nanoscale. Using soft X-ray spectromicroscopy, we report the changes in morphology and molecular structure of C3S at an early stage of hydration. In situ C3S hydration in a wet cell, beginning with induction (~1 h) and acceleration (~4 h) periods of up to ~8 h, was studied and compared with ex situ measurements in the deceleration period after 15 h of curing. Analysis of the near-edge X-ray absorption fine structure showed that the Ca binding energy and energy splitting of C3S changed rapidly in the early age of hydration and exhibited values similar to calcium silicate hydrate (C–S–H). The formation of C–S–H nanoseeds in the C3S solution and the development of a fibrillar C–S–H morphology on the C3S surface were visualized. Following this, silicate polymerization accompanied by C–S–H precipitation produced chemical shifts in the peaks of the main Si K edge and in multiple scattering. However, the silicate polymerization process did not significantly affect the Ca binding energy of C–S–H.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6]
  1. Hanyang Univ., Seoul (Korea)
  2. Tokyo Univ. of Science, Chiba (Japan)
  3. Univ. Autonoma de Chiapas, Chiapas (Mexico)
  4. National Univ. of Singapore (Singapore)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1413704
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1996-1944
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; hydration; tricalcium silicate; C–S–H; kinetics; spectromicroscopy

Citation Formats

Bae, Sungchul, Kanematsu, Manabu, Hernandez-Cruz, Daniel, Moon, Juhyuk, Kilcoyne, David, and Monteiro, Paulo J. M. In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration. United States: N. p., 2016. Web. doi:10.3390/ma9120976.
Bae, Sungchul, Kanematsu, Manabu, Hernandez-Cruz, Daniel, Moon, Juhyuk, Kilcoyne, David, & Monteiro, Paulo J. M. In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration. United States. https://doi.org/10.3390/ma9120976
Bae, Sungchul, Kanematsu, Manabu, Hernandez-Cruz, Daniel, Moon, Juhyuk, Kilcoyne, David, and Monteiro, Paulo J. M. Thu . "In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration". United States. https://doi.org/10.3390/ma9120976. https://www.osti.gov/servlets/purl/1413704.
@article{osti_1413704,
title = {In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration},
author = {Bae, Sungchul and Kanematsu, Manabu and Hernandez-Cruz, Daniel and Moon, Juhyuk and Kilcoyne, David and Monteiro, Paulo J. M.},
abstractNote = {The understanding and control of early hydration of tricalcium silicate (C3S) is of great importance to cement science and concrete technology. However, traditional characterization methods are incapable of providing morphological and spectroscopic information about in situ hydration at the nanoscale. Using soft X-ray spectromicroscopy, we report the changes in morphology and molecular structure of C3S at an early stage of hydration. In situ C3S hydration in a wet cell, beginning with induction (~1 h) and acceleration (~4 h) periods of up to ~8 h, was studied and compared with ex situ measurements in the deceleration period after 15 h of curing. Analysis of the near-edge X-ray absorption fine structure showed that the Ca binding energy and energy splitting of C3S changed rapidly in the early age of hydration and exhibited values similar to calcium silicate hydrate (C–S–H). The formation of C–S–H nanoseeds in the C3S solution and the development of a fibrillar C–S–H morphology on the C3S surface were visualized. Following this, silicate polymerization accompanied by C–S–H precipitation produced chemical shifts in the peaks of the main Si K edge and in multiple scattering. However, the silicate polymerization process did not significantly affect the Ca binding energy of C–S–H.},
doi = {10.3390/ma9120976},
journal = {Materials},
number = 12,
volume = 9,
place = {United States},
year = {Thu Dec 01 00:00:00 EST 2016},
month = {Thu Dec 01 00:00:00 EST 2016}
}

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Advances in understanding hydration of Portland cement
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A new view on the kinetics of tricalcium silicate hydration
journal, August 2016


Influence of Nucleation Seeding on the Hydration Mechanisms of Tricalcium Silicate and Cement
journal, February 2009

  • Thomas, Jeffrey J.; Jennings, Hamlin M.; Chen, Jeffrey J.
  • The Journal of Physical Chemistry C, Vol. 113, Issue 11
  • DOI: 10.1021/jp809811w

Soft X-ray induced modifications of PVA-based microbubbles in aqueous environment: a microspectroscopy study
journal, January 2009

  • Tzvetkov, George; Fernandes, Paulo; Wenzel, Stephan
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 7
  • DOI: 10.1039/b814946a

Hydration of tricalcium silicate in the presence of synthetic calcium–silicate–hydrate
journal, January 2009

  • Alizadeh, Rouhollah; Raki, Laila; Makar, Jon M.
  • Journal of Materials Chemistry, Vol. 19, Issue 42
  • DOI: 10.1039/b910216g

A Reaction Zone Hypothesis for the Effects of Particle Size and Water-to-Cement Ratio on the Early Hydration Kinetics of C 3 S
journal, December 2013

  • Masoero, Enrico; Thomas, Jeffrey J.; Jennings, Hamlin M.
  • Journal of the American Ceramic Society, Vol. 97, Issue 3
  • DOI: 10.1111/jace.12713

The Effect of Magnesium and Zinc Ions on the Hydration Kinetics of C 3 S
journal, August 2014

  • Bazzoni, Amélie; Ma, Suhua; Wang, Qianqian
  • Journal of the American Ceramic Society, Vol. 97, Issue 11
  • DOI: 10.1111/jace.13156

Soft X‐ray Spectromicroscopic Investigation of Synthetic C‐S‐H and C 3 S Hydration Products
journal, June 2015

  • Bae, Sungchul; Taylor, Rae; Hernández‐Cruz, Daniel
  • Journal of the American Ceramic Society, Vol. 98, Issue 9
  • DOI: 10.1111/jace.13709

Quantitative in situ X-ray diffraction analysis of early hydration of Portland cement at defined temperatures
journal, June 2009

  • Hesse, C.; Goetz-Neunhoeffer, F.; Neubauer, J.
  • Powder Diffraction, Vol. 24, Issue 2
  • DOI: 10.1154/1.3120603

Ca X-ray absorption spectroscopy of C—S—H and some model compounds
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Scanning Transmission X-Ray Microscopic Study of Carbonated Calcium Silicate Hydrate
journal, January 2010

  • Ha, J.; Chae, S.; Chou, K. W.
  • Transportation Research Record: Journal of the Transportation Research Board, Vol. 2142, Issue 1
  • DOI: 10.3141/2142-12

Works referencing / citing this record: