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Theoretical analysis of doped graphene as cathode catalyst in Li-O2 and Na-O2 batteries: the impact of the computational scheme
Univ Belgrade, Fac Phys Chem, Studentski Trg 12-16, Belgrade 11158, Serbia..
Univ Belgrade, Fac Phys Chem, Studentski Trg 12-16, Belgrade 11158, Serbia..
Univ Belgrade, Fac Phys Chem, Studentski Trg 12-16, Belgrade 11158, Serbia..
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. KTH Royal Inst Technol, Sch Ind Engn & Management, Dept Mat Sci & Engn, Brinellvagen 23, S-10044 Stockholm, Sweden.;Humboldt Univ, Phys Dept, Zum Grossen Windkanal 6, D-12489 Berlin, Germany..
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2020 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 354, article id 136735Article in journal (Refereed) Published
Abstract [en]

Understanding the reactions in M-O-2 cells (M = Li or Na) is of great importance for further advancement of this promising technology. Computational modelling can be helpful along this way, but an adequate approach is needed to model such complex systems. We propose a new scheme for modelling processes in M-O-2 cells, where reference energies are obtained from high-level theory, CCSD(T), while the interactions of reaction intermediates with catalyst surfaces are extracted from computationally less expensive DFT. The approach is demonstrated for the case of graphene-based surfaces as model catalysts in Li-O-2 and Na-O-2 cells using the minimum viable mechanism. B-doped graphene was identified as the best catalyst amongst considered surfaces, while pristine graphene performs poorly. Moreover, we show that the inclusion of dispersion corrections for DFT has a significant impact on calculated discharge and charge potentials and suggests that long-range dispersion interactions should always be considered when graphene-based materials are modelled as electrocatalysts. Finally, we offer general guidelines for designing new ORR catalysts for M-O-2 cells in terms of the optimization of the interactions of catalyst surface with reaction intermediates.

Place, publisher, year, edition, pages
Elsevier BV , 2020. Vol. 354, article id 136735
Keywords [en]
Graphene, Doped graphene, Metal-air batteries, Oxygen reduction reaction, Modelling
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Other Chemistry Topics
Identifiers
URN: urn:nbn:se:uu:diva-423076DOI: 10.1016/j.electacta.2020.136735ISI: 000569141000014OAI: oai:DiVA.org:uu-423076DiVA, id: diva2:1478023
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation , 18:177Available from: 2020-10-21 Created: 2020-10-21 Last updated: 2020-10-21Bibliographically approved

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Johansson, BörjeSkorodumova, Natalia V.

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