DFT Study on the Hydrogenation of CO2 to Methanol on Ho-Doped Cu(211) Surface

Date

2020-10-01

Author

Tezsevin, Ilker
Senkan, Selim
Önal, Işık
Duzenli, Derya

Metadata

Show full item record

This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

Item Usage Stats

228
views

0
downloads

The catalytic conversion of carbon dioxide (CO2) into methanol, a valuable chemical product, has been investigated theoretically on a novel holmium (Ho)-doped Cu(211) surface by density functional theory (DFT) calculations. The possible key intermediates formed during the hydrogenation of CO2 and as well as their further hydrogenated species during the production of methanol are examined thermodynamically and kinetically by computational means. It is found that the adhesion of a Ho atom on the Cu(211) surface enhances the interaction of reactants, especially CO2 molecules, with the surface. This enhancement in the interaction energy, in turn, increases the catalytic activity of the Cu(211) surface. Unlike other Cu surfaces, the Ho-doped Cu(211) surface activates CO2 better than H-2 molecules. The reaction mechanism proceeds through the formation of formate (HCOO), dioxymehylene (H2COO), dissociation of H2COOH into H2CO and OH, and finally the hydrogenation of H2CO to H3COH. The addition of a Ho atom stabilizes the H2COO intermediate rather than the HCOOH intermediate. Among the various intermediates, the last hydrogenation step has the highest activation barrier (1.02 eV), which is followed by the formation of HCOO (0.96 eV) and H2COO (0.95 eV) surface species.

URI

https://hdl.handle.net/11511/69641

Journal

JOURNAL OF PHYSICAL CHEMISTRY C

DOI

https://doi.org/10.1021/acs.jpcc.0c04170

Collections

Graduate School of Natural and Applied Sciences, Article

Suggestions

OpenMETU
Core

DFT investigation of high temperature water gas shift reaction on chromium-iron mixed oxide catalyst Yalcin, Ozgen; Önal, Işık (2014-11-20) As part of high temperature water gas shift reaction mechanism, CO adsorption and H2O adsorption on Fe3O4 (111) and chromium atom substituted Fe3O4 (111) slab surfaces are investigated by means of periodic DFT approach using VASP. Fe3O4 bulk structure has been computed including the Hubbard (U) parameter. One oxygen site (Ooct1) is studied as a probable site among the six Fe3O4 (111) terminations. Cr atom substitution on this surface is also examined. Cr atoms prefer being on the surface rather than in the ...
Quantum chemical simulation of nitric oxide reduction by ammonia (scr reaction) on v2o5 / tio2 catalyst surface Soyer, Sezen; Önal, Işıl; Department of Chemical Engineering (2005) The reaction mechanism for the selective catalytic reduction (SCR) of nitric oxide by ammonia on (010) V2O5 surface represented by a V2O9H8 cluster was simulated by density functional theory (DFT) calculations. The computations indicated that SCR reaction consisted of three main parts. In the first part ammonia activation on Brønsted acidic V-OH site as NH4+ species by a nonactivated process takes place. The second part includes the interaction of NO with pre-adsorbed NH4 + species to eventually form nitros...
Steady-state parallel plate apparatus for measurement of diffusion coefficient in supercritical carbon dioxide Tuan, DQ; Yener, Meryem Esra; Zollweg, JA; Harriott, P; Rizvi, SSH (1999-02-01) A new, steady-state experimental system for measurement of the Fickian diffusion coefficients for solutes in supercritical carbon dioxide (SC-CO2) was designed and evaluated. Mass transfer between a Liquid solute and SC-CO2 was carried out in a parallel plate geometry where a porous metal sheet, immersed in the liquid phase, stabilized the interface. The SC-CO2 flowed over the porous metal sheet containing the liquid phase which was presaturated with CO2. The use of the porous metal sheet and a thin mobile ...
DSC STUDIES ON MELT CRYSTALLIZED, DRAWN AND FUMING NITRIC-ACID OXIDIZED POLYETHYLENE Akar, Ahmet; Zaim, Ömer; Tinçer, Teoman; Aydoğan, A. Cevdet (Wiley, 1989-4) Melting, recrystallisation and remelting of undrawn and drawn linear polyethylene with different molecular weight were studied by differential scanning calorimetry before and after oxidation with nitric acid.
Multiphoton core ionization dynamics of polyatomic molecules Toffolı, Danıele; Decleva, Piero (IOP Publishing, 2013-07-28) The two-photon core ionization dynamics of gas-phase methane, carbon monoxide and nitrogen have been studied with a recent implementation of the lowest order perturbation theory in the framework of density functional theory and a multicentric basis set expansion of bound and scattering states. Ionization cross sections and angular asymmetry parameters have been calculated for the case of a single radiation beam and for both linear and circular light polarizations in the fixed nuclei approximation. Expected ...

Citation Formats

I. Tezsevin, S. Senkan, I. Önal, and D. Duzenli, “DFT Study on the Hydrogenation of CO2 to Methanol on Ho-Doped Cu(211) Surface,” JOURNAL OF PHYSICAL CHEMISTRY C, pp. 22426–22434, 2020, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/69641.