TY - JOUR
T1 - Predicting CaO-(MgO)-Al2O3-SiO2 glass reactivity in alkaline environments from force field molecular dynamics simulations
AU - Gong, Kai
AU - White, Claire E.
N1 - Funding Information:
This material is based on work supported by ARPA-E under Grant No. DE-AR0001145 and the National Science Foundation under Grant No. 1362039 . K.G. was partially supported by a Charlotte Elizabeth Proctor Fellowship from the Princeton Graduate School. The MD simulations were performed on computational resources supported by the Princeton Institute for Computational Science and Engineering (PICSciE) and the Office of Information Technology's High Performance Computing Center and Visualization Laboratory at Princeton University. The 11-ID-B beam line is located 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 NPDF instrument is located at Los Alamos Neutron Science Center, previously funded by DOE Office of Basic Energy Sciences. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. The upgrade of NPDF was funded by the NSF through grant DMR 00-76488 .
Funding Information:
This material is based on work supported by ARPA-E under Grant No. DE-AR0001145 and the National Science Foundation under Grant No. 1362039. K.G. was partially supported by a Charlotte Elizabeth Proctor Fellowship from the Princeton Graduate School. The MD simulations were performed on computational resources supported by the Princeton Institute for Computational Science and Engineering (PICSciE) and the Office of Information Technology's High Performance Computing Center and Visualization Laboratory at Princeton University. The 11-ID-B beam line is located 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 NPDF instrument is located at Los Alamos Neutron Science Center, previously funded by DOE Office of Basic Energy Sciences. Los Alamos National Laboratory is operated by Los Alamos National Security LLC under DOE Contract DE-AC52-06NA25396. The upgrade of NPDF was funded by the NSF through grant DMR 00-76488.
Publisher Copyright:
© 2021 Elsevier Ltd
PY - 2021/12
Y1 - 2021/12
N2 - In this investigation, force field-based molecular dynamics (MD) simulations have been employed to generate detailed structural representations for a range of amorphous quaternary CaO-MgO-Al2O3-SiO2 (CMAS) and ternary CaO-Al2O3-SiO2 (CAS) glasses. Comparison of the simulation results with select experimental X-ray and neutron total scattering and literature data reveals that the MD-generated structures have captured the key structural features of these CMAS and CAS glasses. Based on the MD-generated structural representations, we have developed two structural descriptors, specifically (i) average metal oxide dissociation energy (AMODE) and (ii) average self-diffusion coefficient (ASDC) of all the atoms at melting. Both structural descriptors are seen to more accurately predict the relative glass reactivity than the commonly used degree of depolymerization parameter, especially for the eight synthetic CAS glasses that span a wide compositional range. Hence these descriptors hold great promise for predicting CMAS and CAS glass reactivity in alkaline environments from compositional information.
AB - In this investigation, force field-based molecular dynamics (MD) simulations have been employed to generate detailed structural representations for a range of amorphous quaternary CaO-MgO-Al2O3-SiO2 (CMAS) and ternary CaO-Al2O3-SiO2 (CAS) glasses. Comparison of the simulation results with select experimental X-ray and neutron total scattering and literature data reveals that the MD-generated structures have captured the key structural features of these CMAS and CAS glasses. Based on the MD-generated structural representations, we have developed two structural descriptors, specifically (i) average metal oxide dissociation energy (AMODE) and (ii) average self-diffusion coefficient (ASDC) of all the atoms at melting. Both structural descriptors are seen to more accurately predict the relative glass reactivity than the commonly used degree of depolymerization parameter, especially for the eight synthetic CAS glasses that span a wide compositional range. Hence these descriptors hold great promise for predicting CMAS and CAS glass reactivity in alkaline environments from compositional information.
KW - Amorphous aluminosilicate
KW - Glass reactivity
KW - Molecular dynamics simulations
KW - Structural descriptors
KW - X-ray and neutron scattering
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U2 - 10.1016/j.cemconres.2021.106588
DO - 10.1016/j.cemconres.2021.106588
M3 - Article
AN - SCOPUS:85115056282
SN - 0008-8846
VL - 150
JO - Cement and Concrete Research
JF - Cement and Concrete Research
M1 - 106588
ER -