Stability of SrCO3 within composite Portland-slag cement blends

Sam A. Walling; Laura J. Gardner; Dale P. Prentice; Malin C. Dixon Wilkins; Adham A. Hammad; Wooyong Um; Claire L. Corkhill; Neil C. Hyatt

doi:10.1016/j.cemconcomp.2022.104823

Stability of SrCO₃ within composite Portland-slag cement blends

Sam A. Walling, Laura J. Gardner, Dale P. Prentice, Malin C. Dixon Wilkins, Adham A. Hammad, Wooyong Um, Claire L. Corkhill^*, Neil C. Hyatt

^*Corresponding author for this work

School of Earth Sciences

Research output: Contribution to journal › Article (Academic Journal) › peer-review

6 Citations (Scopus)

Abstract

The stability and reactivity of SrCO₃ within a blended Portland-slag cement at both 20 °C and 60 °C (to simulate an indicative waste form for disposal) was determined via XRD, TG-MS, SEM-EDX and thermodynamic modelling. Sr¹⁴CO₃ is a potential long-term sink for trapping radioactive ¹⁴C, produced through the nuclear fuel cycle, therefore understanding its stability in potential cementitious waste forms is of interest and importance. Incorporation of 30 wt% SrCO₃ in blended Portland-slag cement caused minor reactions to occur, resulting in increased formation of carbonated AFm phases, along with stabilisation of ettringite at 20 °C, precluded at 60 °C due to the reduced stability to ettringite at this temperature. Thermodynamic modelling predicted only minor SrCO₃ reactivity up to 360 days, with carbonate remaining stable over this timeframe, validated by our experimental results. Thus, thermodynamic simulations predict that SrCO₃ is an effective immobilisation matrix for ¹⁴C, within a blended Portland-slag cement waste form, suitable for long-term geological disposal.

Original language	English
Article number	104823
Number of pages	12
Journal	Cement and Concrete Composites
Volume	135
Early online date	9 Nov 2022
DOIs	https://doi.org/10.1016/j.cemconcomp.2022.104823
Publication status	Published - Jan 2023

Bibliographical note

Publisher Copyright:
© 2022 The Authors

Keywords

Carbonate
Immobilisation
Nuclear
Reaction
Strontium
Thermodynamics

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title = "Stability of SrCO3 within composite Portland-slag cement blends",

abstract = "The stability and reactivity of SrCO3 within a blended Portland-slag cement at both 20 °C and 60 °C (to simulate an indicative waste form for disposal) was determined via XRD, TG-MS, SEM-EDX and thermodynamic modelling. Sr14CO3 is a potential long-term sink for trapping radioactive 14C, produced through the nuclear fuel cycle, therefore understanding its stability in potential cementitious waste forms is of interest and importance. Incorporation of 30 wt% SrCO3 in blended Portland-slag cement caused minor reactions to occur, resulting in increased formation of carbonated AFm phases, along with stabilisation of ettringite at 20 °C, precluded at 60 °C due to the reduced stability to ettringite at this temperature. Thermodynamic modelling predicted only minor SrCO3 reactivity up to 360 days, with carbonate remaining stable over this timeframe, validated by our experimental results. Thus, thermodynamic simulations predict that SrCO3 is an effective immobilisation matrix for 14C, within a blended Portland-slag cement waste form, suitable for long-term geological disposal.",

keywords = "Carbonate, Immobilisation, Nuclear, Reaction, Strontium, Thermodynamics",

author = "Walling, {Sam A.} and Gardner, {Laura J.} and Prentice, {Dale P.} and {Dixon Wilkins}, {Malin C.} and Hammad, {Adham A.} and Wooyong Um and Corkhill, {Claire L.} and Hyatt, {Neil C.}",

note = "Publisher Copyright: {\textcopyright} 2022 The Authors",

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doi = "10.1016/j.cemconcomp.2022.104823",

language = "English",

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AU - Walling, Sam A.

AU - Gardner, Laura J.

AU - Prentice, Dale P.

AU - Dixon Wilkins, Malin C.

AU - Hammad, Adham A.

AU - Um, Wooyong

AU - Corkhill, Claire L.

AU - Hyatt, Neil C.

PY - 2023/1

Y1 - 2023/1

N2 - The stability and reactivity of SrCO3 within a blended Portland-slag cement at both 20 °C and 60 °C (to simulate an indicative waste form for disposal) was determined via XRD, TG-MS, SEM-EDX and thermodynamic modelling. Sr14CO3 is a potential long-term sink for trapping radioactive 14C, produced through the nuclear fuel cycle, therefore understanding its stability in potential cementitious waste forms is of interest and importance. Incorporation of 30 wt% SrCO3 in blended Portland-slag cement caused minor reactions to occur, resulting in increased formation of carbonated AFm phases, along with stabilisation of ettringite at 20 °C, precluded at 60 °C due to the reduced stability to ettringite at this temperature. Thermodynamic modelling predicted only minor SrCO3 reactivity up to 360 days, with carbonate remaining stable over this timeframe, validated by our experimental results. Thus, thermodynamic simulations predict that SrCO3 is an effective immobilisation matrix for 14C, within a blended Portland-slag cement waste form, suitable for long-term geological disposal.

AB - The stability and reactivity of SrCO3 within a blended Portland-slag cement at both 20 °C and 60 °C (to simulate an indicative waste form for disposal) was determined via XRD, TG-MS, SEM-EDX and thermodynamic modelling. Sr14CO3 is a potential long-term sink for trapping radioactive 14C, produced through the nuclear fuel cycle, therefore understanding its stability in potential cementitious waste forms is of interest and importance. Incorporation of 30 wt% SrCO3 in blended Portland-slag cement caused minor reactions to occur, resulting in increased formation of carbonated AFm phases, along with stabilisation of ettringite at 20 °C, precluded at 60 °C due to the reduced stability to ettringite at this temperature. Thermodynamic modelling predicted only minor SrCO3 reactivity up to 360 days, with carbonate remaining stable over this timeframe, validated by our experimental results. Thus, thermodynamic simulations predict that SrCO3 is an effective immobilisation matrix for 14C, within a blended Portland-slag cement waste form, suitable for long-term geological disposal.

KW - Carbonate

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KW - Nuclear

KW - Reaction

KW - Strontium

KW - Thermodynamics

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