A first principles study of CO<sub>2</sub> adsorption on α-SiO<sub>2</sub>(001) surfaces

Malyi, Oleksandr I.; Thiyam, Priyadarshini; Boström, Mathias; Persson, Clas

doi:10.1039/c5cp02279g

Cited by 17 publications

(29 citation statements)

References 70 publications

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“…It worth nothing that formation of CO 3 -like complexes is common for oxide surfaces. [69][70][71][72][73][74][75] In the most stable conformation, the C atom is chemically bonded to the surface oxygen O S with the short bond of 1.33 Å, which is shorter than a typical length of single C-O bond (about 1.43 Å) 76 ,b).…”

Section: Resultsmentioning

confidence: 99%

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Band gap modulation of SrTiO₃ upon CO₂ adsorption

Sopiha

Malyi

Persson

et al. 2017

Phys. Chem. Chem. Phys.

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CO 2 chemisorption on SrTiO 3 (001) surfaces is studied using ab initio calculations in order to establish new chemical sensing mechanisms. We find that CO 2 adsorption opens the material band gap, however, while the adsorption on the TiO 2 -terminated surface neutralizes surface states at the valence band (VB) maximum, CO 2 on the SrO-terminated surfaces suppresses the conduction band (CB) minimum. For the TiO 2 -terminated surface, the effect is explained by the passivation of dangling bonds, whereas for the SrO-terminated surface, the suppression is caused by the surface relaxation. Modulation of the VB states implies a more direct change in charge distribution, and thus the induced change in band gap is more prominent at the TiO 2 termination. Further, we show that both CO 2 adsorption energy and surface band gap are strongly dependent on CO 2 coverage, suggesting that the observed effect can be utilized for sensing application in a wide range of CO 2 concentrations.

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Section: Resultsmentioning

confidence: 99%

“…1f. [69][70][71][72][73][74][75] In the most stable conformation, the C atom is chemically bonded to the surface oxygen O S with the short bond of The formed chemical bonding between CO 2 and SrTiO 3 (001) surfaces has a significant impact on their electronic structures (see Fig. 3).…”

Section: Methodsmentioning

confidence: 99%

Band gap modulation of SrTiO₃ upon CO₂ adsorption

Sopiha

Malyi

Persson

et al. 2017

Phys. Chem. Chem. Phys.

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“…CO2 chemisorption on the γ-Al2O3 (110) surface is generally quite similar to adsorption on many other oxides, with adsorption energies in the range of −0.5 to −2.5 eV, formation of a surface carbonate with Lewis basic surface oxygens, strongly bent bi-or tridentate adsorption configurations, and negative charge transfer to the molecule. [15][16][17][18][19][20][21][22][23] The fairly strong adsorption of CO2 on the alumina support might also increase the retention time of the molecule near the surface, giving it more time to reach an active catalyst site, although it could also increase the competition between metal and support sites.…”

Section: Transition Metal Atom Adsorption On the Al2o3 Supportmentioning

confidence: 99%

Effect of plasma-induced surface charging on catalytic processes: application to CO₂activation

Bal

Huygh

Bogaerts

et al. 2018

Plasma Sources Sci. Technol.

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Understanding the nature and effect of the multitude of plasma-surface interactions in plasma catalysis is a crucial requirement for further process development and improvement. A particularly intriguing and rather unique property of a plasma-catalytic setup is the ability of the plasma to modify the electronic structure, and hence chemical properties, of the catalyst through charging, i.e., the absorption of excess electrons. In this work, we develop a quantum chemical model based on density functional theory (DFT) to study excess negative surface charges in a heterogeneous catalyst exposed to a plasma. This method is specifically applied to investigate plasma-catalytic CO2 activation on supported M/Al2O3 (M = Ti, Ni, Cu) single atom catalysts. We find that (1) the presence of a negative surface charge dramatically improves the reductive power of the catalyst, strongly promoting the splitting of CO2 to CO and oxygen, and (2) the relative activity of the investigated transition metals is also changed upon charging, suggesting that controlled surface charging is a powerful additional parameter to tune catalyst activity and selectivity. These results strongly point to plasma-induced surface charging of the catalyst as an important factor contributing to the plasma-catalyst synergistic effects frequently reported for plasma catalysis.

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“…OptB86-vdW was mostly used to treat van der Waals type of systems, achieving quite good success. [32][33][34] The adsorption calculations are conducted on 6-layer slabs of Al(111) with a 12Å vacuum gap. A (3 Â 3) mesh is used for the adsorption calculation of a single H 2 O molecule on O preadsorbed surface and a (4 Â 4) supercell is used to coadsorption.…”

Section: Computational Detailsmentioning

confidence: 99%