Development and Validation of ReaxFF Reactive Force Field for Hydrocarbon Chemistry Catalyzed by Nickel
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.
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.Attached Files
Supplemental Material - jp9035056_si_001.txt
Supplemental Material - jp9035056_si_002.pdf
Supplemental Material - jp9035056_si_003.pdf
Supplemental Material - jp9035056_si_004.txt
Supplemental Material - jp9035056_si_005.zip
Supplemental Material - jp9035056_si_006.zip
Supplemental Material - jp9035056_si_007.zip
Supplemental Material - jp9035056_si_008.zip
Supplemental Material - jp9035056_si_009.zip
Supplemental Material - jp9035056_si_010.zip
Supplemental Material - jp9035056_si_011.zip
Files
Name | Size | Download all |
---|---|---|
md5:e2267d60d38d063d3a79f51f85d73375
|
7.0 MB | Preview Download |
md5:b4364dae9c2c41c71ab2674573b67494
|
7.0 MB | Preview Download |
md5:6f39a2015ebaf8e53dbca01ce9dc1df3
|
7.7 MB | Preview Download |
md5:4032aaec2a9e3f8abff10af85c97f255
|
432.6 kB | Preview Download |
md5:388110ce8d72f2bc6261e9e40987dd2c
|
7.0 MB | Preview Download |
md5:ea2dabc078cd9ed551cd8ee1fb2c6bfb
|
83.9 kB | Preview Download |
md5:7a24c190c025c74ed907d3cdc75e4a11
|
6.0 kB | Preview Download |
md5:4692ccbeaaea907e2176ef696a4d2a8d
|
7.0 MB | Preview Download |
md5:74ade74ad4095bd2128f61706f31620c
|
7.7 MB | Preview Download |
md5:1a82bdee31736a2f4e683e52e5ffa383
|
1.5 kB | Preview Download |
md5:97ee195db0aa9885a70f4f8c19543f87
|
34.2 kB | Preview Download |
Additional details
- Eprint ID
- 17896
- Resolver ID
- CaltechAUTHORS:20100408-095811343
- Intel
- Created
-
2010-04-08Created from EPrint's datestamp field
- Updated
-
2021-11-08Created from EPrint's last_modified field