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Skorodumova, Natalia V.
Alternative names
Publications (10 of 102) Show all publications
Pasti, I. A., Fako, E., Dobrota, A. S., Lopez, N., Skorodumova, N. V. & Mentus, S. V. (2019). Atomically Thin Metal Films on Foreign Substrates: From Lattice Mismatch to Electrocatalytic Activity. ACS Catalysis, 9(4), 3467-3481
Open this publication in new window or tab >>Atomically Thin Metal Films on Foreign Substrates: From Lattice Mismatch to Electrocatalytic Activity
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2019 (English)In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 9, no 4, p. 3467-3481Article in journal (Refereed) Published
Abstract [en]

Electrocatalytic properties of materials are governed by the electronic structure, stability, and reactivity of the surface layer which is exposed to the electrolyte. Over the years, different strategies have been developed to tailor electrocatalyst surfaces but also to reduce the cost of these materials, which is the bottleneck for any practical application. When a very thin metallic layer, intended to serve as an electrocatalyst, is placed over a substrate, its configuration is influenced by the structure of the substrate due to lattice mismatch, while the electronic structure is affected due to the strain and the electronic effects of the support. This results in altered bonding within the electrocatalyst layer and the modification of its electronic properties when compared to the pure phase. In this contribution, we address the possibilities of theoretical prediction of surface properties of atomically thin electrocatalyst films formed over different substrates, focusing on the metal side of the electrified interface. While all these properties can be calculated quite easily using modern computational techniques (but used with care), most often based on density functional theory, we also address an attractive, fast screening possibility to estimate the properties of monometallic and multimetallic overlayers using small sets of calculations on model systems. We discuss how lattice mismatch between a substrate and an overlayer can be used to predict the properties of electrocatalytic films, limitations of such approach, and a possibility of deploying of large databases which enable rapid prescreening of different support/overlayer systems for various electrocatalytic applications.

Keywords
thin film, lattice mismatch, strain, metal films, alloy films
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-382649 (URN)10.1021/acscatal.8b04236 (DOI)000464075700074 ()
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation , 17:503
Available from: 2019-04-29 Created: 2019-04-29 Last updated: 2019-04-29Bibliographically approved
Žguns, P. A., Ruban, A. V. & Skorodumova, N. V. (2019). Influence of composition and oxygen-vacancy ordering on lattice parameter and elastic moduli of Ce1-xGdxO2-x/2: A theoretical study. Scripta Materialia, 158, 126-130
Open this publication in new window or tab >>Influence of composition and oxygen-vacancy ordering on lattice parameter and elastic moduli of Ce1-xGdxO2-x/2: A theoretical study
2019 (English)In: Scripta Materialia, ISSN 1359-6462, E-ISSN 1872-8456, Vol. 158, p. 126-130Article in journal (Refereed) Published
Abstract [en]

We study the behaviour of the lattice parameter and elastic moduli of Ce1-xGdxO2-x/2 for the random (fluoritelike) and C-type ordered oxygen-vacancy configurations [Zguns et al., PCCP 20 (2018) 11805-11818]. For the fluorite phase, elastic moduli decrease linearly with Gd concentration. For the C-type phase, the bulk, shear and Young moduli are found to be systematically larger and the lattice parameter smaller than those for disordered fluorite phase. Essentially the linear behaviour of the bulk modulus and lattice parameter depending on the degree of the C-type order is found. Our findings explain the experimentally observed elastic moduli of Ce1-xGdxO2-x/2. 

KeyWords Plus:GD-DOPED CERIA; X-RAY-DIFFRACTION; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; OXIDE FUEL-CELLS; CEO2-GD2O3 SYSTEM; RAMAN-SPECTROSCOPY; MONTE-CARLO; IONIC-CONDUCTIVITY

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Structure-property relation, Gd-doped ceria, Ordering, Elastic moduli, DFT
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-359573 (URN)10.1016/j.scriptamat.2018.08.034 (DOI)000447094500027 ()
Funder
Swedish Research Council, VR 348-2012-6196Swedish Research Council, 201505538EU, European Research CouncilVINNOVA
Available from: 2018-09-03 Created: 2018-09-03 Last updated: 2018-12-05Bibliographically approved
Bondarenko, N. G., Eriksson, O., Skorodumova, N. V. & Pereiro, M. (2019). Multi-polaron solutions, nonlocal effects and internal modes in a nonlinear chain. Journal of physics: Condensed matter, 31(41), Article ID 415401.
Open this publication in new window or tab >>Multi-polaron solutions, nonlocal effects and internal modes in a nonlinear chain
2019 (English)In: Journal of physics: Condensed matter, ISSN 0953-8984, Vol. 31, no 41, article id 415401Article in journal (Refereed) Published
Abstract [en]

Multipolaron solutions were studied in the framework of the Holstein one-dimensional molecular crystal model. The study was performed in the continuous limit where the crystal model maps into the nonlinear Schrödinger equation for which a new periodic dnoidal solution was found for the multipolaron system. In addition, the stability of the multi-polaron solutions was examined, and it was found that  cnoidal and dnoidal solutions stabilize in different ranges of the parameter space. Moreover, the model was studied under the influence of nonlocal effects and the polaronic dynamics was described in terms of internal solitonic modes.

National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-340881 (URN)10.1088/1361-648X/ab306e (DOI)000476531900001 ()31317871 (PubMedID)
Funder
Swedish Research Council, 2014-5993Swedish Foundation for Strategic Research Swedish Energy AgencyKnut and Alice Wallenberg FoundationeSSENCE - An eScience Collaboration
Available from: 2018-02-05 Created: 2018-02-05 Last updated: 2019-08-27Bibliographically approved
Diklic, N. P., Dobrota, A. S., Pasti, I. A., Mentus, S. V., Johansson, B. & Skorodumova, N. V. (2019). Sodium storage via single epoxy group on graphene: The role of surface doping. Electrochimica Acta, 297, 523-528
Open this publication in new window or tab >>Sodium storage via single epoxy group on graphene: The role of surface doping
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2019 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 297, p. 523-528Article in journal (Refereed) Published
Abstract [en]

Due to its unique physical and chemical properties, graphene is being considered as a promising material for energy conversion and storage applications. Introduction of functional groups and dopants on/in graphene is a useful strategy for tuning its properties. In order to fully exploit its potential, atomic-level understanding of its interaction with species of importance for such applications is required. We present a DFT study of the interaction of sodium atoms with epoxy-graphene and analyze how this interaction is affected upon doping with boron and nitrogen. We demonstrate how the dopants, combined with oxygen-containing groups alter the reactivity of graphene towards Na. Dopants act as attractors of epoxy groups, enhancing the sodium adsorption on doped oxygen-functionalized graphene when compared to the case of non-doped epoxy-graphene. Furthermore, by considering thermodynamics of the Na interaction with doped epoxy-graphene it has been concluded that such materials are good candidates for Na storage applications. Therefore, we suggest that controlled oxidation of doped carbon materials could lead to the development of advanced anode materials for rechargeable Na-ion batteries.

Keywords
Graphene, Graphene doping, Graphene oxidation, Sodium storage, Battery
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-375795 (URN)10.1016/j.electacta.2018.11.108 (DOI)000455642500058 ()
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation , 17:503Swedish National Infrastructure for Computing (SNIC)
Available from: 2019-02-15 Created: 2019-02-15 Last updated: 2019-02-15Bibliographically approved
Alekseev, A. Y., Chernykh, A. G., Filonov, A. B., Migas, D. B. & Skorodumova, N. V. (2019). Stability of 2D Alkaline-Earth Metal Silicides, Germanides and Stannides. International Journal of Nanoscience, 18(3-4), Article ID 1940013.
Open this publication in new window or tab >>Stability of 2D Alkaline-Earth Metal Silicides, Germanides and Stannides
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2019 (English)In: International Journal of Nanoscience, ISSN 0219-581X, Vol. 18, no 3-4, article id 1940013Article in journal (Refereed) Published
Abstract [en]

By means of ab initio calculations, we have estimated stability of 2D Me2X (Me = Mg, Ca, Sr, Ba and X = Si, Ge, Sn) in the T and Td phases, which are similar to the ones of 2D transition metal chalcogenides, in addition to their phonon spectra. The T phase is found to be more stable for 2D Ca2X, Sr2X and Ba2X, whereas the Td phase is predicted to be the ground state for 2D Mg2X. We have also discussed that imaginary frequencies in the calculated phonon spectra of 2D Me2X, which appeared in the vicinity of the Gamma point, were not necessarily associated with the dynamic instability.

Place, publisher, year, edition, pages
World Scientific, 2019
Keywords
2D crystal, silicide, germanide, stannide, stability, total energy, phonon dispersion
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-390595 (URN)10.1142/S0219581X19400131 (DOI)000472775200014 ()
Funder
EU, Horizon 2020Swedish Research Council, 2014-5993
Available from: 2019-08-13 Created: 2019-08-13 Last updated: 2019-08-13Bibliographically approved
Karacic, D., Korac, S., Dobrota, A. S., Pasti, I. A., Skorodumova, N. V. & Gutic, S. J. (2019). When supporting electrolyte matters: Tuning capacitive response of graphene oxide via electrochemical reduction in alkali and alkaline earth metal chlorides. Electrochimica Acta, 297, 112-117
Open this publication in new window or tab >>When supporting electrolyte matters: Tuning capacitive response of graphene oxide via electrochemical reduction in alkali and alkaline earth metal chlorides
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2019 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 297, p. 112-117Article in journal (Refereed) Published
Abstract [en]

The ability to tune charge storage properties of graphene oxide (GO) is of utmost importance for energy conversion applications. Here we show that the electrochemical reduction of GO is highly sensitive to the cations present in the solution. GO is reduced at more negative potential in alkali metal chloride solutions than in alkaline earth metal chlorides. During the reduction, the capacitance of GO increases from 10 to 70 times. The maximum capacitances of reduced GO are between 65 and 130 F g-1, depending on the electrolyte and the presence of conductive additive. We propose that different interactions of cations with oxygen functional groups of GO during the reduction are responsible for the observed effect. This hypothesis has been confirmed by Density Functional Theory calculations of alkali and alkaline earth metals interactions with epoxy-functionalized graphene sheet.

Keywords
Graphene oxide, Capacitance, Electrochemical reduction, Capacitance tuning
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-375794 (URN)10.1016/j.electacta.2018.11.173 (DOI)000455642500014 ()
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation , 17:503Swedish National Infrastructure for Computing (SNIC)
Available from: 2019-02-15 Created: 2019-02-15 Last updated: 2019-02-15Bibliographically approved
Gavrilov, N., Momcilovic, M., Dobrota, A. S., Stankovic, D. M., Jokic, B., Babic, B., . . . Pasti, I. A. (2018). A study of ordered mesoporous carbon doped with Co and Ni as a catalyst of oxygen reduction reaction in both alkaline and acidic media. Surface & Coatings Technology, 349, 511-521
Open this publication in new window or tab >>A study of ordered mesoporous carbon doped with Co and Ni as a catalyst of oxygen reduction reaction in both alkaline and acidic media
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2018 (English)In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 349, p. 511-521Article in journal (Refereed) Published
Abstract [en]

The incorporation of trace amounts (< 0.2%) of Co and Ni noticeably enhanced the catalytic activity of nitrogen free ordered mesoporous carbon (OMC) towards oxygen reduction reaction (ORR). (Co,Ni)-doped OMCs were characterized by N-2-adsorption measurements, X-ray powder diffraction, field emission scanning electron microscopy and Raman spectroscopy methods, and their ORR activity was estimated by voltammetry on rotating disk electrode in acidic and alkaline media. (Co,Ni)-doped OMCs show modest activities in acidic media, while the catalytic activity in alkaline media is rather high. The measured activities are compared to the Pt-based and Pt-free ORR catalysts reported in the literature. The number of electrons consumed per O-2 in metal-doped OMCs was found to vary between 2 and 4, which is advantageous in comparison to metal-free OMC. Also, the mass activities of metal-doped OMCs were found to be up to 2.5 times higher compared to that of metal-free OMC. We suggest that the ORR activity is governed by a balance between (i) textural properties, which determine the electrochemically accessible surface of the catalyst and which are influenced by the addition of a metal precursor, and (ii) novel active sites formed upon the introduction of metals into the carbon structure. In particular, our Density Functional Theory calculations suggest that Co and Ni atoms embedded into the single vacancies of graphene can activate the O-2 molecule and contribute to the decomposition of peroxide.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE SA, 2018
Keywords
Electrocatalysts, Oxygen reduction reaction, Ordered mesoporous carbon, Cobalt, Nickel, Metal dopants
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-362097 (URN)10.1016/j.surfcoat.2018.06.008 (DOI)000441492600054 ()
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation
Available from: 2018-10-05 Created: 2018-10-05 Last updated: 2018-10-05Bibliographically approved
Nowakowska, S., Mazzola, F., Alberti, M. N., Song, F., Voigt, T., Nowakowski, J., . . . Jung, T. A. (2018). Adsorbate-Induced Modification of the Confining Barriers in a Quantum Box Array. ACS Nano, 12(1), 768-778
Open this publication in new window or tab >>Adsorbate-Induced Modification of the Confining Barriers in a Quantum Box Array
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2018 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, no 1, p. 768-778Article in journal (Refereed) Published
Abstract [en]

Quantum devices depend on addressable elements, which can be modified separately and in their mutual interaction. Self-assembly at surfaces, for example, formation of a porous (metal-) organic network, provides an ideal way to manufacture arrays of identical quantum boxes, arising in this case from the confinement of the electronic (Shockley) surface state within the pores. We show that the electronic quantum box state as well as the interbox coupling can be modified locally to a varying extent by a selective choice of adsorbates, here C60, interacting with the barrier. In view of the wealth of differently acting adsorbates, this approach allows for engineering quantum states in on-surface network architectures.

Keywords
quantum box, electronic coupling, on-surface self-assembled network, surface state, adsorption
National Category
Condensed Matter Physics Nano Technology
Identifiers
urn:nbn:se:uu:diva-346371 (URN)10.1021/acsnano.7b07989 (DOI)000423495200082 ()29272579 (PubMedID)
Funder
Swedish Research Council, 348-2012-6196; 2014-5993EU, European Research Council, ERC-2012-StG 307760-SURF-PROKnut and Alice Wallenberg FoundationEuropean Social Fund (ESF)
Available from: 2018-03-23 Created: 2018-03-23 Last updated: 2018-03-23Bibliographically approved
Pasti, I. A., Jovanovic, A., Dobrota, A. S., Mentus, S. V., Johansson, B. & Skorodumova, N. V. (2018). Atomic adsorption on graphene with a single vacancy: systematic DFT study through the periodic table of elements. Physical Chemistry, Chemical Physics - PCCP, 20(2), 858-865
Open this publication in new window or tab >>Atomic adsorption on graphene with a single vacancy: systematic DFT study through the periodic table of elements
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 2, p. 858-865Article in journal (Refereed) Published
Abstract [en]

Vacancies in graphene present sites of altered chemical reactivity and open possibilities to tune graphene properties by defect engineering. The understanding of chemical reactivity of such defects is essential for successful implementation of carbon materials in advanced technologies. We report the results of a systematic DFT study of atomic adsorption on graphene with a single vacancy for the elements of rows 1-6 of the periodic table of elements (PTE), excluding lanthanides. The calculations have been performed using the PBE, long-range dispersion interaction-corrected PBE (PBE+D2 and PBE+D3) and non-local vdW-DF2 functionals. We find that most elements strongly bind to the vacancy, except for the elements of groups 11 and 12, and noble gases, for which the contribution of dispersion interaction to bonding is most significant. The strength of the interaction with the vacancy correlates with the cohesive energy of the elements in their stable phases: the higher the cohesive energy is, the stronger bonding to the vacancy can be expected. As most atoms can be trapped at the SV site we have calculated the potentials of dissolution and found that in most cases the metals adsorbed at the vacancy are more "noble" than they are in their corresponding stable phases.

National Category
Chemical Sciences Physical Sciences
Identifiers
urn:nbn:se:uu:diva-341487 (URN)10.1039/c7cp07542a (DOI)000419219700015 ()29238768 (PubMedID)
Available from: 2018-02-28 Created: 2018-02-28 Last updated: 2018-02-28Bibliographically approved
Pasti, I. A., Jovanovic, A., Dobrota, A. S., Mentus, S. V., Johansson, B. & Skorodumova, N. V. (2018). Atomic adsorption on pristine graphene along the Periodic Table of Elements - From PBE to non-local functionals. Applied Surface Science, 436, 433-440
Open this publication in new window or tab >>Atomic adsorption on pristine graphene along the Periodic Table of Elements - From PBE to non-local functionals
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2018 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 436, p. 433-440Article in journal (Refereed) Published
Abstract [en]

The understanding of atomic adsorption on graphene is of high importance for many advanced technologies. Here we present a complete database of the atomic adsorption energies for the elements of the Periodic Table up to the atomic number 86 (excluding lanthanides) on pristine graphene. The energies have been calculated using the projector augmented wave (PAW) method with PBE, long-range dispersion interaction corrected PBE (PBE+D2, PBE+D3) as well as non-local vdW-DF2 approach. The inclusion of dispersion interactions leads to an exothermic adsorption for all the investigated elements. Dispersion interactions are found to be of particular importance for the adsorption of low atomic weight earth alkaline metals, coinage and s-metals (11th and 12th groups), high atomic weight p-elements and noble gases. We discuss the observed adsorption trends along the groups and rows of the Periodic Table as well some computational aspects of modelling atomic adsorption on graphene.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE BV, 2018
Keywords
Graphene, Adsorption, Atomic adsorption, Periodic Table of Elements, Dispersion interactions
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-350485 (URN)10.1016/j.apsusc.2017.12.046 (DOI)000425723100050 ()
Funder
Swedish Research Council, 348-2012-6196]Swedish Research Council, 2014-5993]Carl Tryggers foundation
Available from: 2018-05-17 Created: 2018-05-17 Last updated: 2018-05-17Bibliographically approved
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