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Development and Validation of ReaxFF Reactive Force Field for Hydrocarbon Chemistry Catalyzed by Nickel

Mueller, Jonathan E. and van Duin, Adri C. T. and Goddard, William A., III (2010) Development and Validation of ReaxFF Reactive Force Field for Hydrocarbon Chemistry Catalyzed by Nickel. Journal of Physical Chemistry C, 114 (11). pp. 4939-4949. ISSN 1932-7447. https://resolver.caltech.edu/CaltechAUTHORS:20100408-095811343

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Abstract

To enable the study of hydrocarbon reactions catalyzed by nickel surfaces and particles using reactive molecular dynamics on thousands of atoms as a function of temperature and pressure, we have developed the ReaxFF reactive force field to describe adsorption, decomposition, reformation and desorption of hydrocarbons as they interact with the nickel surface. The ReaxFF parameters were determined by fitting to the geometries and energy surfaces from quantum mechanics (QM) calculations for a large number of reaction pathways for hydrocarbon molecules chemisorbed onto nickel (111), (100) and (110) surfaces, supplemented with QM equations of state for nickel and nickel carbides. We demonstrate the validity and accuracy of ReaxFF by applying it to study the reaction dynamics of hydrocarbons as catalyzed by nickel particles and surfaces. For the dissociation of methyl on the (111), (100), and stepped (111) surfaces of nickel, we observe the formation of chemisorbed CH plus subsurface carbide. We observe that the (111) surface is the least reactive, the (100) surface has the fastest reaction rates, and the stepped (111) surface has an intermediate reaction rate. The importance of surface defects in accelerating reaction rates is highlighted by these results.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp9035056DOIArticle
ORCID:
AuthorORCID
Mueller, Jonathan E.0000-0001-8811-8799
van Duin, Adri C. T.0000-0002-3478-4945
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2010 American Chemical Society. Published In Issue: March 25, 2010; article ASAP: February 26, 2010; received: April 16, 2009; revised: January 22, 2010. This research was supported partly by Intel Components Research and by Intel Corporate Research.
Funders:
Funding AgencyGrant Number
IntelUNSPECIFIED
Issue or Number:11
Record Number:CaltechAUTHORS:20100408-095811343
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20100408-095811343
Official Citation:Development and Validation of ReaxFF Reactive Force Field for Hydrocarbon Chemistry Catalyzed by Nickel Jonathan E. Mueller, Adri C. T. van Duin, William A. Goddard III The Journal of Physical Chemistry C 2010 114 (11), 4939-4949
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:17896
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:08 Apr 2010 20:18
Last Modified:17 Nov 2020 00:55

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