Details

Autor(en) / Beteiligte

• Novčić, Katarina A.
• Dobrota, Ana S.
• Petković, Milena
• Johansson, Börje
• Skorodumova, Natalia V.
• Mentus, Slavko V.
• Pašti, Igor A.

Titel

Theoretical analysis of doped graphene as cathode catalyst in Li-O2 and Na-O2 batteries – the impact of the computational scheme

Ist Teil von

• Electrochimica acta, 2020-09, Vol.354, p.136735, Article 136735

Ort / Verlag

Oxford: Elsevier Ltd

Erscheinungsjahr

2020

Quelle

Elsevier ScienceDirect Journals

Beschreibungen/Notizen

• •Modelling of oxygen reduction in Li-O2 and Na-O2 cells is analysed.•Graphene-based materials are considered as cathode catalysts.•Modelling approach is revisited by combining different levels of theory.•General guidelines for identification of new catalysts are provided. Understanding the reactions in M-O2 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-O2 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-O2 and Na-O2 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-O2 cells in terms of the optimization of the interactions of catalyst surface with reaction intermediates. [Display omitted]