3D crystalline phase and pore structure evolution upon CO2 exposure in sodium sulfate-activated cement pastes

Zengliang Yue; Zixian Su; Partha P. Paul; Alastair T.M. Marsh; Alice Macente; Marco Di Michiel; John L. Provis; Philip J. Withers; Susan A. Bernal

doi:10.1016/j.cemconres.2024.107716

3D crystalline phase and pore structure evolution upon CO₂ exposure in sodium sulfate-activated cement pastes

Zengliang Yue, Zixian Su, Partha P. Paul, Alastair T.M. Marsh, Alice Macente, Marco Di Michiel, John L. Provis, Philip J. Withers, Susan A. Bernal

Research output: Contribution to journal › Article › peer-review

3 Citations (SciVal)

Abstract

The effects of CO₂ exposure on sodium sulfate-activated blast furnace slag cement paste have been characterised by X-ray (attenuation) computed tomography revealing changes in micron-scale pore structure, and X-ray diffraction computed tomography (XRD-CT) elucidating changes in the spatial distribution of crystalline and semi-crystalline phases. Accelerated carbonation reduced ettringite volumes and induced formation of hydrotalcite, demonstrating the critical role of Mg-Al-SO₄-layered double hydroxide phases in the CO₂ uptake of these cements. These changes yield a refinement of small pores and increase the overall porosity, reaching values comparable to those of blended Portland cements. Formation factor values were determined considering the pore solution electrical resistivity, calculated from thermodynamic modelling, and the porosity. A correlation between simulated tortuosity and porosity is proposed to estimate the diffusion tortuosity and formation factor of sodium sulfate-activated slag pastes. This approach represents a significant step forward for assessing carbonation resistance and CO₂ uptake capacity of cementitious pastes.

Original language	English
Article number	107716
Journal	Cement and Concrete Research
Volume	187
Early online date	11 Nov 2024
DOIs	https://doi.org/10.1016/j.cemconres.2024.107716
Publication status	Published - 1 Jan 2025

Data Availability Statement

The data associated with this paper are openly available at https://doi.esrf.fr/10.15151/ESRF-ES-895887564

Funding

This research was sponsored by the Engineering and Physical Sciences Research Council (EPSRC) Early Career Fellowship EP/R001642/1. Z. Yue is grateful to the University of Leeds for his PhD studentship. The authors acknowledge Beamline ID15A at The European Synchrotron (ESRF) for the experiments (MA-5424, https://doi.esrf.fr/10.15151/ESRF-ES-895887564). PJW and PPP are grateful for the support for the Henry Royce Institute for Advanced Materials, established through EPSRC Grants EP/R00661X/1, EP/P025498/1 and EP/P025021/1 and an EPSRC centre-to-centre collaboration with the ESRF through grants EP/W003333/1 and EP/T02593X/1 as well as access to the NXCT funded through EP/X034941/1 and EP/T02593X/1. The participation of JLP in this work was supported by in part by EPSRC under grant EP/T008407/1.

Keywords

Alkali-activated cements
Carbon capture
Pore network
Sodium sulfate
X-ray computed tomography
X-ray diffraction computed tomography

ASJC Scopus subject areas

Building and Construction
General Materials Science

Access to Document

10.1016/j.cemconres.2024.107716Licence: CC BY

Cite this

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title = "3D crystalline phase and pore structure evolution upon CO2 exposure in sodium sulfate-activated cement pastes",

abstract = "The effects of CO2 exposure on sodium sulfate-activated blast furnace slag cement paste have been characterised by X-ray (attenuation) computed tomography revealing changes in micron-scale pore structure, and X-ray diffraction computed tomography (XRD-CT) elucidating changes in the spatial distribution of crystalline and semi-crystalline phases. Accelerated carbonation reduced ettringite volumes and induced formation of hydrotalcite, demonstrating the critical role of Mg-Al-SO4-layered double hydroxide phases in the CO2 uptake of these cements. These changes yield a refinement of small pores and increase the overall porosity, reaching values comparable to those of blended Portland cements. Formation factor values were determined considering the pore solution electrical resistivity, calculated from thermodynamic modelling, and the porosity. A correlation between simulated tortuosity and porosity is proposed to estimate the diffusion tortuosity and formation factor of sodium sulfate-activated slag pastes. This approach represents a significant step forward for assessing carbonation resistance and CO2 uptake capacity of cementitious pastes.",

keywords = "Alkali-activated cements, Carbon capture, Pore network, Sodium sulfate, X-ray computed tomography, X-ray diffraction computed tomography",

author = "Zengliang Yue and Zixian Su and Paul, {Partha P.} and Marsh, {Alastair T.M.} and Alice Macente and {Di Michiel}, Marco and Provis, {John L.} and Withers, {Philip J.} and Bernal, {Susan A.}",

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AU - Yue, Zengliang

AU - Su, Zixian

AU - Paul, Partha P.

AU - Marsh, Alastair T.M.

AU - Macente, Alice

AU - Di Michiel, Marco

AU - Provis, John L.

AU - Withers, Philip J.

AU - Bernal, Susan A.

PY - 2025/1/1

Y1 - 2025/1/1

N2 - The effects of CO2 exposure on sodium sulfate-activated blast furnace slag cement paste have been characterised by X-ray (attenuation) computed tomography revealing changes in micron-scale pore structure, and X-ray diffraction computed tomography (XRD-CT) elucidating changes in the spatial distribution of crystalline and semi-crystalline phases. Accelerated carbonation reduced ettringite volumes and induced formation of hydrotalcite, demonstrating the critical role of Mg-Al-SO4-layered double hydroxide phases in the CO2 uptake of these cements. These changes yield a refinement of small pores and increase the overall porosity, reaching values comparable to those of blended Portland cements. Formation factor values were determined considering the pore solution electrical resistivity, calculated from thermodynamic modelling, and the porosity. A correlation between simulated tortuosity and porosity is proposed to estimate the diffusion tortuosity and formation factor of sodium sulfate-activated slag pastes. This approach represents a significant step forward for assessing carbonation resistance and CO2 uptake capacity of cementitious pastes.

AB - The effects of CO2 exposure on sodium sulfate-activated blast furnace slag cement paste have been characterised by X-ray (attenuation) computed tomography revealing changes in micron-scale pore structure, and X-ray diffraction computed tomography (XRD-CT) elucidating changes in the spatial distribution of crystalline and semi-crystalline phases. Accelerated carbonation reduced ettringite volumes and induced formation of hydrotalcite, demonstrating the critical role of Mg-Al-SO4-layered double hydroxide phases in the CO2 uptake of these cements. These changes yield a refinement of small pores and increase the overall porosity, reaching values comparable to those of blended Portland cements. Formation factor values were determined considering the pore solution electrical resistivity, calculated from thermodynamic modelling, and the porosity. A correlation between simulated tortuosity and porosity is proposed to estimate the diffusion tortuosity and formation factor of sodium sulfate-activated slag pastes. This approach represents a significant step forward for assessing carbonation resistance and CO2 uptake capacity of cementitious pastes.

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KW - Sodium sulfate

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KW - X-ray diffraction computed tomography

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