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Title: Effects of Incorporating High-Volume Fly Ash into Tricalcium Silicate on the Degree of Silicate Polymerization and Aluminum Substitution for Silicon in Calcium Silicate Hydrate

Abstract

This study assesses the quantitative effects of incorporating high-volume fly ash (HVFA) into tricalcium silicate (C3S) paste on the hydration, degree of silicate polymerization, and Al substitution for Si in calcium silicate hydrate (C–S–H). Thermogravimetric analysis and isothermal conduction calorimetry showed that, although the induction period of C3S hydration was significantly extended, the degree of hydration of C3S after the deceleration period increased due to HVFA incorporation. Synchrotron-sourced soft X-ray spectromicroscopy further showed that most of the C3S in the C3S-HVFA paste was fully hydrated after 28 days of hydration, while that in the pure C3S paste was not. The chemical shifts of the Si K edge peaks in the near-edge X-ray fine structure of C–S–H in the C3S-HVFA paste directly indicate that Al substitutes for Si in C–S–H and that the additional silicate provided by the HVFA induces an enhanced degree of silicate polymerization. This new spectromicroscopic approach, supplemented with 27Al and 29Si magic-angle spinning nuclear magnetic resonance spectroscopy and transmission electron microscopy, turned out to be a powerful characterization tool for studying a local atomic binding structure of C–S–H in C3S-HVFA system and presented results consistent with previous literature.

Authors:
 [1];  [2];  [3];  [4];  [2]
  1. Hanyang Univ., Seoul (Korea)
  2. Univ. of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. National Univ. of Singapore (Singapore)
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:
1413716
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Materials
Additional Journal Information:
Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 1996-1944
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; calcium silicate hydrate; tricalcium silicate; fly ash; hydration products; X-ray microscopy

Citation Formats

Bae, Sungchul, Taylor, Rae, Kilcoyne, David, Moon, Juhyuk, and Monteiro, Paulo J. M. Effects of Incorporating High-Volume Fly Ash into Tricalcium Silicate on the Degree of Silicate Polymerization and Aluminum Substitution for Silicon in Calcium Silicate Hydrate. United States: N. p., 2017. Web. doi:10.3390/ma10020131.
Bae, Sungchul, Taylor, Rae, Kilcoyne, David, Moon, Juhyuk, & Monteiro, Paulo J. M. Effects of Incorporating High-Volume Fly Ash into Tricalcium Silicate on the Degree of Silicate Polymerization and Aluminum Substitution for Silicon in Calcium Silicate Hydrate. United States. https://doi.org/10.3390/ma10020131
Bae, Sungchul, Taylor, Rae, Kilcoyne, David, Moon, Juhyuk, and Monteiro, Paulo J. M. Sat . "Effects of Incorporating High-Volume Fly Ash into Tricalcium Silicate on the Degree of Silicate Polymerization and Aluminum Substitution for Silicon in Calcium Silicate Hydrate". United States. https://doi.org/10.3390/ma10020131. https://www.osti.gov/servlets/purl/1413716.
@article{osti_1413716,
title = {Effects of Incorporating High-Volume Fly Ash into Tricalcium Silicate on the Degree of Silicate Polymerization and Aluminum Substitution for Silicon in Calcium Silicate Hydrate},
author = {Bae, Sungchul and Taylor, Rae and Kilcoyne, David and Moon, Juhyuk and Monteiro, Paulo J. M.},
abstractNote = {This study assesses the quantitative effects of incorporating high-volume fly ash (HVFA) into tricalcium silicate (C3S) paste on the hydration, degree of silicate polymerization, and Al substitution for Si in calcium silicate hydrate (C–S–H). Thermogravimetric analysis and isothermal conduction calorimetry showed that, although the induction period of C3S hydration was significantly extended, the degree of hydration of C3S after the deceleration period increased due to HVFA incorporation. Synchrotron-sourced soft X-ray spectromicroscopy further showed that most of the C3S in the C3S-HVFA paste was fully hydrated after 28 days of hydration, while that in the pure C3S paste was not. The chemical shifts of the Si K edge peaks in the near-edge X-ray fine structure of C–S–H in the C3S-HVFA paste directly indicate that Al substitutes for Si in C–S–H and that the additional silicate provided by the HVFA induces an enhanced degree of silicate polymerization. This new spectromicroscopic approach, supplemented with 27Al and 29Si magic-angle spinning nuclear magnetic resonance spectroscopy and transmission electron microscopy, turned out to be a powerful characterization tool for studying a local atomic binding structure of C–S–H in C3S-HVFA system and presented results consistent with previous literature.},
doi = {10.3390/ma10020131},
journal = {Materials},
number = 2,
volume = 10,
place = {United States},
year = {Sat Feb 04 00:00:00 EST 2017},
month = {Sat Feb 04 00:00:00 EST 2017}
}

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Cited by: 15 works
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journal, September 2011


The contribution of class-F fly ash to the strength of cementitious mixtures
journal, June 2005


A new aluminium-hydrate species in hydrated Portland cements characterized by 27Al and 29Si MAS NMR spectroscopy
journal, January 2006


Composition, morphology and nanostructure of C–S–H in white Portland cement pastes hydrated at 55 °C
journal, December 2007


Supplementary cementitious materials
journal, December 2011


Hydration of C3S thin films
journal, April 2012


Hydration of Portland cement with high replacement by siliceous fly ash
journal, October 2012


Hydration of water- and alkali-activated white Portland cement pastes and blends with low-calcium pulverized fuel ash
journal, May 2016


Characterization of calcium aluminate phases in cements by aluminum-27 MAS NMR spectroscopy
journal, March 1993

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27 Al and 29 Si Solid-State NMR Characterization of Calcium-Aluminosilicate-Hydrate
journal, January 2012

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Aluminum Incorporation to Dreierketten Silicate Chains
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Aluminum Incorporation in Calcium Silicate Hydrates (C−S−H) Depending on Their Ca/Si Ratio
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Soft X‐ray Spectromicroscopic Investigation of Synthetic C‐S‐H and C 3 S Hydration Products
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  • Bae, Sungchul; Taylor, Rae; Hernández‐Cruz, Daniel
  • Journal of the American Ceramic Society, Vol. 98, Issue 9
  • DOI: 10.1111/jace.13709

In Situ Soft X-ray Spectromicroscopy of Early Tricalcium Silicate Hydration
journal, December 2016

  • Bae, Sungchul; Kanematsu, Manabu; Hernández-Cruz, Daniel
  • Materials, Vol. 9, Issue 12
  • DOI: 10.3390/ma9120976

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  • Jee, Hyeonseok; Park, Jaeyeon; Zalnezhad, Erfan
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  • Du, Sen; Wu, Junliang; AlShareedah, Othman
  • Nanomaterials, Vol. 9, Issue 9
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  • Zhao, Zhiguang; Wei, Jiangxiong; Li, Fangxian
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  • Bae, Sungchul; Hikaru, Fumino; Kanematsu, Manabu
  • Materials, Vol. 11, Issue 1
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Characterization of Titanium Nanotube Reinforced Cementitious Composites: Mechanical Properties, Microstructure, and Hydration
journal, May 2019

  • Jee, Hyeonseok; Park, Jaeyeon; Zalnezhad, Erfan
  • Materials, Vol. 12, Issue 10
  • DOI: 10.3390/ma12101617

Nanotechnology in Cement-Based Materials: A Review of Durability, Modeling, and Advanced Characterization
journal, August 2019

  • Du, Sen; Wu, Junliang; AlShareedah, Othman
  • Nanomaterials, Vol. 9, Issue 9
  • DOI: 10.3390/nano9091213