Multiscale Modelling of In Situ Oil Sands Upgrading with Molybdenum Carbide Nanoparticles

  • Xingchen Liu
  • Baojing Zhou
  • Farouq Ahmed
  • Alexander Tkalych
  • Akira Miyamoto
  • Dennis R. Salahub
Chapter
Part of the Challenges and Advances in Computational Chemistry and Physics book series (COCH, volume 21)

Abstract

This chapter presents multi-scale models of the reactions that occur in the in situ oil sands upgrading process. Its focus is on the various modelling tools and their applications to the benzene hydrogenation reactions catalyzed by molybdenum carbide nanoparticles. As the reaction mechanism of benzene hydrogenation on molybdenum carbide is not clear, we start with density functional theory (DFT) studies to elucidate the reaction mechanism, using both periodic and cluster models. Benzene hydrogenation on molybdenum carbide follows the Langmuir-Hinshelwood mechanism, with the six-member ring tilting up gradually. A tight-binding quantum chemical molecular dynamics (TB-QCMD) method is used to track the physical motion of the atoms in the reaction processes of C6H6 on a Mo-terminated α-Mo2C (0001) surface. The approximate DFT method, density functional tight-binding (DFTB), was parameterized to allow the quantum mechanical treatment of nanoscale systems. With the nudged elastic band method, the potential energy profiles of benzene hydrogenation on molybdenum carbide nanoparticles have been obtained. Finally a force field was brought in to describe the solvent environment in the system, leading to a multiscale quantum mechanical/molecular mechanical (QM/MM) model. This study suggests that entropy and the environment play important roles in heterogeneous reactions catalyzed by molybdenum carbide nanoparticles.

List of Acronyms (alphabetical order)

ADFT

Auxiliary density functional theory

DFT

Density functional theory

DFTB

Density functional tight-binding

HDN

Hydrodenitrogenation

HDS

Hydrodesulphurization

HRTEM

High-resolution transmission electron microscopy

KS

Kohn-Sham

L-H

Langmuir-Hinshelwood

LCGTO

Linear combination of Gaussian type orbitals

MCNPs

Molybdenum carbide nanoparticles

MD

Molecular dynamics

MEP

Minimum energy path

PAH

Polyaromatic hydrocarbons

PAW

Projector augmented wave

PMF

Potential of mean force

QM/MM

Quantum mechanics/molecular mechanics

SAGD

Steam-assisted gravity drainage

SCC

Self-consistent-charge

TB

Tight-binding

TB-QC

Tight-binding quantum chemistry

TB-QCMD

Tight-binding quantum chemical molecular dynamics

TPR-MS

Temperature-programmed reaction-mass spectrometry

TS

Transition state

UD

Ultra-dispersed

WHAM

Weighted-histogram analysis method

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Copyright information

© Springer International Publishing Switzerland 2015

Authors and Affiliations

  • Xingchen Liu
    • 1
  • Baojing Zhou
    • 2
  • Farouq Ahmed
    • 3
  • Alexander Tkalych
    • 4
  • Akira Miyamoto
    • 5
  • Dennis R. Salahub
    • 1
  1. 1.Department of Chemistry, Institute for Quantum Science and Technology, and Centre for Molecular SimulationUniversity of CalgaryCalgaryCanada
  2. 2.Department of Chemistry, School of Chemical EngineeringNanjing University of Science and TechnologyNanjingChina
  3. 3.Chemical and Petroleum Engineering Department, Schulich School of EngineeringUniversity of CalgaryCalgaryCanada
  4. 4.Department of ChemistryPrinceton UniversityPrincetonUSA
  5. 5.New Industry Creation Hatchery CenterTohoku UniversityAobaJapan

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