TY - JOUR
T1 - Drying-induced atomic structural rearrangements in sodium-based calcium-alumino-silicate-hydrate gel and the mitigating effects of ZrO2 nanoparticles
AU - Yang, Kengran
AU - Özçelik, V. Ongun
AU - Garg, Nishant
AU - Gong, Kai
AU - White, Claire Emily
N1 - Funding Information:
This work was supported by NSF through the MRSEC Center (Grant No. DMR-1420541). KG was supported by NSF, Grant No. CMMI-1362039, and NG and VOO were funded by the Andlinger Center for Energy and the Environment (Princeton University). The authors would like to thank Mr Kevin Beyer and Dr Olaf Borkiewicz for their assistance with the experiment setup at the Advanced Photon Source (APS). Use of the APS at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The calculations presented in this article 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 authors thank Dr Jie Feng for his help in conducting the dynamic light scattering experiment.
Funding Information:
The authors would like to thank Mr Kevin Beyer and Dr Olaf Borkiewicz for their assistance with the experiment setup at the Advanced Photon Source (APS). Use of the APS at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The calculations presented in this article 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 authors thank Dr Jie Feng for his help in conducting the dynamic light scattering experiment.
Funding Information:
This work was supported by NSF through the MRSEC Center (Grant No. DMR-1420541). KG was supported by NSF, Grant No. CMMI-1362039, and NG and VOO were funded by the Andlinger Center for Energy and the Environment (Princeton University).
Publisher Copyright:
© 2018 the Owner Societies.
PY - 2018
Y1 - 2018
N2 - Conventional drying of colloidal materials and gels (including cement) can lead to detrimental effects due to the buildup of internal stresses as water evaporates from the nano/microscopic pores. However, for these gel materials the underlying nanoscopic alterations that are, in part, responsible for macroscopically-measured strain values (especially at low relative humidity) remain a topic of open debate in the literature. In this study, sodium-based calcium-alumino-silicate-hydrate (C-(N)-A-S-H) gel, the major binding phase of silicate-activated blast furnace slag (one type of low-CO2 cement), is investigated from a drying perspective, since it is known to suffer extensively from drying-induced microcracking. By employing in situ synchrotron X-ray total scattering measurements and pair distribution function (PDF) analysis we show that the significant contributing factor to the strain development in this material at extremely low relative humidity (0%) is the local atomic structural rearrangement of the C-(N)-A-S-H gel, including collapse of interlayer spacing and slight disintegration of the gel. Moreover, analysis of the medium range (1.0-2.2 nm) ordering in the PDF data reveals that the PDF-derived strain values are in much closer agreement (same order of magnitude) with the macroscopically measured strain data, compared to previous results based on reciprocal space X-ray diffraction data. From a mitigation standpoint, we show that small amounts of ZrO2 nanoparticles are able to actively reinforce the structure of silicate-activated slag during drying, preventing atomic level strains from developing. Mechanistically, these nanoparticles induce growth of a silica-rich gel during drying, which, via density functional theory calculations, we show is attributed to the high surface reactivity of tetragonal ZrO2.
AB - Conventional drying of colloidal materials and gels (including cement) can lead to detrimental effects due to the buildup of internal stresses as water evaporates from the nano/microscopic pores. However, for these gel materials the underlying nanoscopic alterations that are, in part, responsible for macroscopically-measured strain values (especially at low relative humidity) remain a topic of open debate in the literature. In this study, sodium-based calcium-alumino-silicate-hydrate (C-(N)-A-S-H) gel, the major binding phase of silicate-activated blast furnace slag (one type of low-CO2 cement), is investigated from a drying perspective, since it is known to suffer extensively from drying-induced microcracking. By employing in situ synchrotron X-ray total scattering measurements and pair distribution function (PDF) analysis we show that the significant contributing factor to the strain development in this material at extremely low relative humidity (0%) is the local atomic structural rearrangement of the C-(N)-A-S-H gel, including collapse of interlayer spacing and slight disintegration of the gel. Moreover, analysis of the medium range (1.0-2.2 nm) ordering in the PDF data reveals that the PDF-derived strain values are in much closer agreement (same order of magnitude) with the macroscopically measured strain data, compared to previous results based on reciprocal space X-ray diffraction data. From a mitigation standpoint, we show that small amounts of ZrO2 nanoparticles are able to actively reinforce the structure of silicate-activated slag during drying, preventing atomic level strains from developing. Mechanistically, these nanoparticles induce growth of a silica-rich gel during drying, which, via density functional theory calculations, we show is attributed to the high surface reactivity of tetragonal ZrO2.
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U2 - 10.1039/c7cp07876e
DO - 10.1039/c7cp07876e
M3 - Article
C2 - 29557431
AN - SCOPUS:85044756287
SN - 1463-9076
VL - 20
SP - 8593
EP - 8606
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 13
ER -