The oxidation mechanism investigation of benzene catalyzed by palladium nanoparticle: A ReaxFF molecular dynamics

Wei, Mingrui; Wu, Sheng; Mao, Qian; Wang, Yun; Guo, Guanlun; Zhang, Dongju

doi:10.1016/j.fuel.2020.117989

Cited by 20 publications

(6 citation statements)

References 45 publications

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“…Similar energy trends of C–OH, O–H, and various C–H bonds in phenolic pyrolysis were obtained between ReaxFF and CCSD(T) in a systematic comparison of DFT, the self-consistent charge density-functional tight-binding (SCC-DFTB), and ReaxFF carried out by Qi et al Some reaction enthalpy comparisons for benzene oxidation between ReaxFF and G3 suggest their agreement . The key intermediates and initiation reactions of H abstraction and pyrolysis obtained from ReaxFF MD simulations of toluene oxidation were confirmed by comparison of the reaction enthalpy between ReaxFF, DFT, and the literature by Cheng et al In addition, the well matched heats of formation for the alkoxy benzyl radical between ReaxFF prediction and literature values with a maximal deviation of ∼8.7 kcal were reported.…”

Section: Theory and Methodology Progress Of Reaxff MD Simulationssupporting

confidence: 69%

ReaxFF Molecular Dynamics Simulations of Thermal Reactivity of Various Fuels in Pyrolysis and Combustion

Ren

et al. 2021

Energy Fuels

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The methodology development and applications of ReaxFF molecular dynamics (ReaxFF MD) in unraveling the complex reactions and kinetics for pyrolysis and oxidation of organic systems are reviewed. Particular attention is given to the large-scale ReaxFF MD simulation method of ∼10,000 atoms and practical simulation strategies to overcome the temporal−spatial limits as much as possible. High-performance computing codes running on CPU cluster/supercomputers and on GPU were overviewed. GPU-enabled code like GMD-Reax is revolutionizing large-scale ReaxFF MD simulations to run mainly on a single GPU. A step-forward for reaction analysis was achieved in the code of VARxMD to reveal detailed reactions based on the identification of bond types and unique species that allows for categorization of reaction species and pathways through structure searching of reaction sites and reactants/products. Efforts for extracting rate constants and kinetics modeling from unperturbed kinetics of ReaxFF MD simulations are reviewed, and challenges remain. The important factors of model scale effects, elevated simulation temperature, and possible validation of ReaxFF MD reaction simulation results theoretically and experimentally are illustrated and discussed. The novel hybrid simulation strategies proposed recently that may expand applications of ReaxFF MD to connect with realistic scenarios of engine combustion and relevant chemical effects on aerospace vehicle materials are briefed. The simulation practices of large-scale ReaxFF MD in understanding the similarities and differences of reactivity and reaction mechanisms in pyrolysis of liquid hydrocarbon fuels, solid fuels (coal, biomass, polymer), and energetic materials of CL-20 and its cocrystals are briefly described, which indicates that large-scale ReaxFF MD simulations are a feasible and straight means to capture the dynamics of an almost entire reaction process and to evaluate reactivity of organic systems computationally. There is still a great deal of work to be done to push the boundaries of ReaxFF MD simulations forward. With the constant improvement of the ReaxFF force field and reaction analysis capability, ReaxFF MD playing a key role in understanding reaction mechanisms and its potential in kinetics modeling of pyrolysis and oxidation of various fuels can be expected.

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Section: Theory and Methodology Progress Of Reaxff MD Simulationssupporting

confidence: 69%

ReaxFF Molecular Dynamics Simulations of Thermal Reactivity of Various Fuels in Pyrolysis and Combustion

Ren

et al. 2021

Energy Fuels

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“…3 (a) The oxidation process of C 6 H 6 on Pd nanoparticles and (b) further oxidation of C 6 HO to small molecules. 54 time of HCHO decreased with the increase of H/C ratio at low temperature. However, at high temperature, the H/C ratio has almost no effect on HCHO.…”

Section: Pyrolysis and Combustion Mechanism Of Multicomponents Of Avi...mentioning

confidence: 92%

“…Aromatic hydrocarbons are very common in the alternative model [32][33][34] of aviation kerosene. In order to understand the properties of aromatic hydrocarbons more comprehensively, the process of pyrolysis or combustion of aromatic hydrocarbons has been studied 17,[54][55][56][57][58][59][60][61] under various conditions.…”

Section: Pyrolysis and Combustion Mechanism Of Aromatic Hydrocarbons ...mentioning

confidence: 99%

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Recent ReaxFF MD studies on pyrolysis and combustion mechanisms of aviation/aerospace fuels and energetic additives

Chen

Li²,

Zhang

et al. 2023

Energy Adv.

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“…The MD simulation with the reactive force field (ReaxFF) can be used for larger systems involving chemical reactions. In the past 20 years, the ReaxFF MD simulation has been a useful means of exploring reaction mechanisms and dynamic processes. − Methane oxidation was also investigated both in the gas phase and on the palladium nanoparticles based on the ReaxFF MD technology.…”

Section: Introductionmentioning

confidence: 99%

Dynamic Evolution of Methane Oxidation on Pd-Based Catalysts: A Reactive Force Field Molecular Dynamics Study

Wang

2022

J. Phys. Chem. C

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Studying the dynamic evolution of the reaction process that identifies the key intermediate is important for elaborating the reaction mechanism, but it is still challenging from the point of view of the experiment. Methane oxidation over Pd-based catalysts including Pd (111) with different oxygen coverages and PdO ( 101) is studied by reactive force field molecular dynamic simulations in this work to explore the dynamic character of oxygen species like chemisorbed oxygen and lattice oxygen on the C−H bond activation and the C−O bond formation. The results show that methane oxidation on the Pd (111) surfaces is initiated by the direct dissociation of methane molecules (CH 4 → CH 3 + H) rather than the oxygen-assisted dissociation (CH 4 + O → CH 3 + OH), which is in agreement with the first-principle electronic structure calculation results. A comparison of methane oxidation at different oxygen coverages shows that the catalytic activity increases with the increase of oxygen pressure in general: There is no CO at low oxygen coverage and CO is formed at higher oxygen coverage up to 3/9 ML, but no CO 2 is formed. This is because the C−O bond formation barrier is higher than the H− O bond formation barrier. Therefore, it is in favor of the formation of OH species instead of the CO 2 formation for methane oxidation on metallic Pd. On the PdO (101) surface, we notice that the lattice oxygen species are more active compared to the chemisorbed oxygen species in both the activation of methane and the oxidation of CH x species due to its strong hydrogen affinity and high electron density, leading to high methane oxidation activity and ultimately CO 2 formation. Importantly, a novel path for the CO 2 formation via a dioxymethylene (H 2 COO) intermediate (CH 2 O + O → H 2 COO) or a hydroxymethoxy (H 2 COOH) intermediate (CH 2 O + OH → H 2 COOH) has been identified from our present reactive force field molecular dynamic simulations, which is generally ignored in the static electronic structure scheme like density functional theory. It is hoped that the present results would be a guide for the rational design of the methane oxidation catalysts by controlling the active phase of Pd (or Pt) or provide more essential knowledge for a better understanding of the methane oxidation or methane reformation reaction mechanism.

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The oxidation mechanism investigation of benzene catalyzed by palladium nanoparticle: A ReaxFF molecular dynamics

Cited by 20 publications

References 45 publications

ReaxFF Molecular Dynamics Simulations of Thermal Reactivity of Various Fuels in Pyrolysis and Combustion

ReaxFF Molecular Dynamics Simulations of Thermal Reactivity of Various Fuels in Pyrolysis and Combustion

Recent ReaxFF MD studies on pyrolysis and combustion mechanisms of aviation/aerospace fuels and energetic additives

Dynamic Evolution of Methane Oxidation on Pd-Based Catalysts: A Reactive Force Field Molecular Dynamics Study

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