TY - JOUR
T1 - Time-dependent phase quantification and local structure analysis of hydroxide-activated slag via X-ray total scattering and molecular modeling
AU - Gong, Kai
AU - White, Claire E.
N1 - Funding Information:
This work was supported by the National Science Foundation under Grant No. 1362039 and ARPA-E under Grant No. DE-AR0001145 . KG was partially supported by a Charlotte Elizabeth Procter Fellowship from Princeton University. The authors would like to acknowledge the use of the 11-ID-B beamline at the Advanced Photon Source, an Office of Science User Facility operated for the U.S. DOE Office of Science by Argonne National Laboratory, under U.S. DOE Contract No. DE-AC02-06CH11357. The authors would like to thank the beamline staff Mr. Kevin Beyer and Dr. Olaf Borkiewicz, and colleagues Dr. Kengran Yang and Dr. Arne Peys for their assistance during the synchrotron experiment. The authors also acknowledge the use of computational resources supported by Princeton Institute for Computational Science and Engineering (PICSciE) and the High Performance Computing Research Center at Princeton University.
Publisher Copyright:
© 2021 Elsevier Ltd
PY - 2022/1
Y1 - 2022/1
N2 - Here, an approach to quantify the amorphous-to-disordered/crystalline transformation occurring in NaOH-activated ground granulated blast-furnace slag (GGBS) is outlined that combines atomistic modeling with in situ pair distribution function (PDF) analysis. Firstly, by using force-field molecular dynamics (MD) simulations, a detailed structural representation is generated for the amorphous GGBS that is in agreement with experimental X-ray scattering data. Use of this structural representation along with literature-derived structures for the reaction products allows for real space X-ray PDF refinement of the alkaline activation of GGBS, resulting in the quantification of all phases and the degree of reaction (DOR) as a function of reaction time. All phases and the DOR are seen to approximately follow a logarithmic-type time-dependent behavior up to 5 months, while at the early age (up to 11 h), the DOR is accurately captured by a modified pseudo-single step first-order reaction model. Lastly, the evolution of DOR is found to agree with several other complementary in situ data containing quantitative reaction information, including isothermal conduction calorimetry, Fourier transform infrared spectroscopy, and quasi-elastic neutron scattering.
AB - Here, an approach to quantify the amorphous-to-disordered/crystalline transformation occurring in NaOH-activated ground granulated blast-furnace slag (GGBS) is outlined that combines atomistic modeling with in situ pair distribution function (PDF) analysis. Firstly, by using force-field molecular dynamics (MD) simulations, a detailed structural representation is generated for the amorphous GGBS that is in agreement with experimental X-ray scattering data. Use of this structural representation along with literature-derived structures for the reaction products allows for real space X-ray PDF refinement of the alkaline activation of GGBS, resulting in the quantification of all phases and the degree of reaction (DOR) as a function of reaction time. All phases and the DOR are seen to approximately follow a logarithmic-type time-dependent behavior up to 5 months, while at the early age (up to 11 h), the DOR is accurately captured by a modified pseudo-single step first-order reaction model. Lastly, the evolution of DOR is found to agree with several other complementary in situ data containing quantitative reaction information, including isothermal conduction calorimetry, Fourier transform infrared spectroscopy, and quasi-elastic neutron scattering.
KW - Alkali-activated materials
KW - Blast-furnace slag
KW - In situ pair distribution function analysis
KW - Molecular dynamics simulations
KW - Phase quantification
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U2 - 10.1016/j.cemconres.2021.106642
DO - 10.1016/j.cemconres.2021.106642
M3 - Article
AN - SCOPUS:85117798216
SN - 0008-8846
VL - 151
JO - Cement and Concrete Research
JF - Cement and Concrete Research
M1 - 106642
ER -