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A density functional theory study of CO2 hydrogenation on carbon-terminated TaC (111) surface

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Abstract

In this study, the density functional theory implemented in the Vienna ab initio simulation package was used to shed more light on the catalytic Carbon dioxide (CO2) hydrogenation process on the (111) facet of the carbon-terminated tantalum carbide (TaC) surface. The adsorption of several intermediates and their hydrogenation elementary steps on the TaC (111) surface towards the formation and desorption of the main products including carbon monoxide (CO), methane (CH4), and methanol (CH3OH) was investigated. The results indicate that the involved intermediates adsorb strongly to the carbon-terminated TaC (111) surface by releasing large energies. The calculated reaction energies concluded in proposing the preferred mechanisms energetically, where the found pathways are overall endothermic which can be provided by the large exothermic adsorption energies of the intermediates. The favorite routes to the formation of desired compounds including CO, CH4, and CH3OH require overall reaction energies of 1.29, 5.96, and 6.63 eV, where they go through dihydroxycarbene (HOCOH) intermediate created from t-COOH hydrogenation. Along these routes, COH dehydrogenation to CO releases the largest exothermic reaction energy of − 2.30 eV, while hydrogenation of t-HCOH to CH2OH requires the highest endothermic reaction energy of 2.69 eV to proceed. It is concluded that CO and CH4 are the main products of CO2 hydrogenation on carbon terminated TaC (111) surface, in agreement with experimental and theoretical studies.

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The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

S.S.T thanks the Iran National Science Foundation (INSF) Grant No. 97020912 for the financial support of this investigation. The authors are also grateful to the Research Affairs Division of the Amirkabir University of Technology (AUT), Tehran, Iran, for their financial support. This work utilized the ARCHER2 UK National Supercomputing Service (http://archer2.ac.uk) through our participation in the UK's HEC Materials Chemistry Consortium, sponsored by the EPSRC (EP/R029431). Additionally, this work has used the computing resources provided by Cardiff University, HPC Wales, and the Advanced Research Computing at Cardiff (ARCCA) Division.

Funding

Funding was provided by Iran National Science Foundation (Grant Number 97020912).

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Authors and Affiliations

  1. Department of Chemistry, Amirkabir University of Technology (Tehran Polytechnic), No. 350, Hafez Avenue, Tehran, 1591634311, Iran

    Saeedeh Sarabadani Tafreshi & Mostafa Torkashvand

  2. School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK

    Saeedeh Sarabadani Tafreshi & Nora H. de Leeuw

  3. Department of Physics, Iran University of Science and Technology, Narmak, Tehran, 16846-13114, Iran

    Narges Taghizade & S. F. K. S. Panahi

  4. Department of Physics, North Tehran Branch, Islamic Azad University, Tehran, 16511-53311, Iran

    Mahmoodreza Sharifian

  5. Department of Earth Sciences, Utrecht University, 3584 CB, Utrecht, The Netherlands

    Nora H. de Leeuw

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Sarabadani Tafreshi, S., Taghizade, N., Sharifian, M. et al. A density functional theory study of CO2 hydrogenation on carbon-terminated TaC (111) surface. Reac Kinet Mech Cat 136, 1945–1963 (2023). https://doi.org/10.1007/s11144-023-02458-0

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