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A ReaxFF Reactive Force-field for Proton Transfer Reactions in Bulk Water and its Applications to Heterogeneous Catalysis

van Duin, Adri C. T. and Zou, Chenyu and Joshi, Kaushik and Bryantsev, Vyascheslav and Goddard, William A. (2013) A ReaxFF Reactive Force-field for Proton Transfer Reactions in Bulk Water and its Applications to Heterogeneous Catalysis. In: Computational Catalysis. RSC Catalysis Series. No.14. Royal Society of Chemistry , Cambridge, pp. 223-243. ISBN 978-1-84973-451-6. https://resolver.caltech.edu/CaltechAUTHORS:20151119-123721297

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Abstract

We have developed a ReaxFF reactive force-field description for bulk water and for proton transfer in the aqueous phase. This ReaxFF potential was parameterized exclusively against quantumchemical (QM) data, describing a broad range of intra- and intermolecular water interactions, including H–H, HO–OH and O=O bond dissociation energies, charge distributions, angle bending energies, binding energies for [H_2O]2–35-clusters, H-transfer reactions pathways in H_3O^+/H_2O, [H_2O]n and HO−/H_2O-clusters and ice densities and cohesive energies. We find good agreement between ReaxFF and QM for all these cases. We found that this QM-based ReaxFF potential gives a good description of bulk water phases and proton migration, reproducing experimental density, radial distribution and diffusion data, while it overestimates proton diffusion in the OH−/water system. We anticipate that this ReaxFF water description, in combination with ongoing ReaxFF-work on amines, carboxylic acids, phosphates and inorganic materials, should be highly suitable for simulating biochemical reactions involving enzymes and DNA. Furthermore, this potential can be used to simulate water reactions and proton diffusion on metal and metal oxide surfaces, opening up applications to catalysis, crystal growth and crack propagation studies. We have provided a specific example of this force field to heterogeneous catalysis, showing an oxygen/hydrogen recombination reaction in an iron nanoparticle.


Item Type:Book Section
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1039/9781849734905-00223DOIArticle
http://pubs.rsc.org/en/Content/Chapter/9781849734905-00223/978-1-84973-490-5PublisherArticle
ORCID:
AuthorORCID
van Duin, Adri C. T.0000-0002-3478-4945
Goddard, William A.0000-0003-0097-5716
Additional Information:© 2014 The Royal Society of Chemistry.
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1046
Series Name:RSC Catalysis Series
Issue or Number:14
Record Number:CaltechAUTHORS:20151119-123721297
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20151119-123721297
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:62239
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:19 Nov 2015 20:48
Last Modified:21 Feb 2020 17:34

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