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Development of a ReaxFF Reactive Force Field for Ettringite and Study of its Mechanical Failure Modes from Reactive Dynamics Simulations

Liu, Lianchi and Jaramillo-Botero, Andres and Goddard, William A., III and Sun, Huai (2012) Development of a ReaxFF Reactive Force Field for Ettringite and Study of its Mechanical Failure Modes from Reactive Dynamics Simulations. Journal of Physical Chemistry A, 116 (15). pp. 3918-3925. ISSN 1089-5639. doi:10.1021/jp210135j.

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Ettringite is a hexacalcium aluminate trisulfate hydrate mineral that forms during Portland cement hydration. Its presence plays an important role in controlling the setting rate of the highly reactive aluminate phases in cement paste and has also been associated with severe cracking in cured hardened cement. To understand how it forms and how its properties influence those of hardened cement and concrete, we have developed a first-principles-based ReaxFF reactive force field for Ca/Al/H/O/S. Here, we report on the development of this ReaxFF force field and on its validation and application using reactive molecular dynamics (RMD) simulations to characterize and understand the elastic, plastic, and failure response of ettringite at the atomic scale. The ReaxFF force field was validated by comparing the lattice parameters, pairwise distribution functions, and elastic constants of an ettringite crystal model obtained from RMD simulations with those from experiments. The predicted results are in close agreement with published experimental data. To characterize the atomistic failure modes of ettringite, we performed stress–strain simulations to find that Ca–O bonds are responsible for failure of the calcium sulfate and tricalcium aluminate (C3A) column in ettringite during uniaxial compression and tension and that hydrogen bond re-formation during compression induces an increase in plastic strain beyond the material’s stress–strain proportionality limit. These results provide essential insight into understanding the mechanistic role of this mineral in cement and concrete degradation, and the ReaxFF potential developed in this work serves as a fundamental tool to further study the kinetics of hydration in cement and concrete.

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Jaramillo-Botero, Andres0000-0003-2844-0756
Goddard, William A., III0000-0003-0097-5716
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Additional Information:© 2012 American Chemical Society. Received: October 21, 2011; Revised: February 27, 2012; Published: March 13, 2012. The authors would like to thank Adri van Duin for providing the Al/O ReaxFF parameters and Hegoi Manzano for providing the corresponding Ca/O parameters. L.L. performed the work associated with his contributions in this paper during a visiting appointment at the Materials and Process Simulation Center in Caltech. This material is based on work supported by the Department of Transportation, Federal Highway Administration (FHWA), under Award Number BAA No. DTFH61-09-R- 00017. Special thanks to Dr. Kunik Lee from FHWA for his support of this program.
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Department of Transportation, Federal Highway Administration (FHWA)BAA No. DTFH61-09-R-00017
Issue or Number:15
Record Number:CaltechAUTHORS:20120516-143235565
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Official Citation:Development of a ReaxFF Reactive Force Field for Ettringite and Study of its Mechanical Failure Modes from Reactive Dynamics Simulations Lianchi Liu, Andres Jaramillo-Botero, William A. Goddard, III, and Huai Sun The Journal of Physical Chemistry A2012116 (15), 3918-3925
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:31509
Deposited By: Andres Jaramillo
Deposited On:22 May 2012 22:15
Last Modified:09 Nov 2021 19:54

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