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The Dynamic Nature of Graphene Active Sites in the H2O Gasification process: A ReaxFF and DFT Study

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Abstract

Context

A steam-rich environment is a more promising application scenario for future coal-fired processes, while active sites are the key factor that determines the reactivity of carbonaceous fuels. The steam gasification process of carbon surfaces with different numbers of active sites (0, 12, 24, 36) was simulated using reactive molecular dynamics in the present study. The temperature for the decomposition of H2O and the gasification of carbon is determined using temperature-increasing simulation. The decomposition of H2O was influenced by two driving forces, thermodynamics and active sites on the carbon surface, which dominated the different reaction stages, leading to the observed segmentation phenomenon of the H2 production rate. The existence and number of initial active sites have a positive correlation with both two stages of the reaction, greatly reducing the activation energy. Residual OH groups play an important role in the gasification of carbon surfaces. The supply of OH groups through the cleavage of OH bonds in H2O is the rate-limiting step in the carbon gasification reaction. The adsorption preference at carbon defect sites was calculated using density functional theory. Two stable configurations (ether & semiquinone groups) can be formed with O atoms adsorbed on the carbon surface according to the number of active sites. This study will provide further insights into the tuning of active sites for advanced carbonaceous fuels or materials.

Methods

The large-scale atomic/molecule massively parallel simulator (LAMMPS) code combined with the reaction force-field method was used to carry out the ReaxFF molecular dynamics simulation, where the ReaxFF potentials were taken from Castro-Marcano, Weismiller and William. The initial configuration was built using Packmol, and the visualization of the calculation results was realized through Visual Molecular Dynamics (VMD). The timestep was set to 0.1 fs to detect the oxidation process with high precision. PWscf code in QUANTUM ESPRESSO (QE) package, was used to evaluate the relative stability of different possible intermediate configurations and the thermodynamic stability of gasification reactions. The projector augmented wave (PAW) and the generalized gradient approximation of Perdew-Burke-Ernzerhof (PBE-GGA) were adopted. Kinetic energy cutoffs of 50 Ry and 600 Ry, and a uniform mesh of 4 × 4 × 1 k-points were used.

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Acknowledgements

This work was supported by the Young Elite Scientist Sponsorship Program by CAST (Grant numbers [YESS20210090]), the National Natural Science Foundation of China (Grant numbers [51974019]), Beijing Natural Science Foundation (Grant numbers [J210017]), China Baowu Low Carbon Metallurgy Innovation Foudation (Grant numbers [BWLCF202119]), and the National Key Research and Development Program of China (Grant numbers [2017YFB0304300] and [2017YFB0304303]). Computations were completed on the Niagara supercomputer at the SciNet HPC Consortium in the Compute/Calcul Canada national computing platform. SciNet is funded by the Canada Foundation for Innovation under the auspices of Compute Canada, the Government of Ontario, Ontario Research Fund - Research Excellence, and the University of Toronto. The authors acknowledge Prof. Mansoor Barati of the University of Toronto for the technical support.

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Authors and Affiliations

  1. School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083, P.R. China

    Zeng Liang, Kejiang Li, Yushan Bu & Jianliang Zhang

  2. School of Physical Science and Information Technology, Liaocheng University, Liaocheng, 252000, China

    Feng Guo

  3. Modern Technology and Education Centre, North China University of Science and Technology, Tangshan, Tangshan, 063009, PR China

    Hang Zhang

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Zeng Liang: Data curation, Formal analysis, Writing original draft. Kejiang Li: Conceptualization, Discussion, Review & editing. Supervision. Feng Guo: Discussion. Hang Zhang: Software. Yushan Bu: Software, Visualization. Jianliang Zhang: Investigation, Supervision, Funding acquisition.

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Table S1. Fig. S1. Structural evolution of carbon surface cracking starting at 4450K. Fig. S2. Generation data for additional molecules (OH, H) as a function of time for (a) Pr; (b)12AS; (c) 24AS; (d) 36AS surfaces. Fig. S3. The (a) area; (b) perimeter; of the surface defect (light blue area) in Fig.6. Fig. S4. reaction intermediates of C-H2O system. Fig. S5. the energy difference between the 6AS-3O system with ether groups and the 6AS-3O system with semiquinone groups (Edifference = E6AS-semiquinone - E6AS-ether), which was eventually stabilized at 4.77 eV

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Liang, Z., Li, K., Guo, F. et al. The Dynamic Nature of Graphene Active Sites in the H2O Gasification process: A ReaxFF and DFT Study. J Mol Model 29, 116 (2023). https://doi.org/10.1007/s00894-023-05527-2

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