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A DFT study of the oxygen reduction reaction mechanism on be doped graphene

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Abstract

Graphene despite its high surface area has very limited activity towards the oxygen reduction reaction (ORR), demonstrating selectivity towards the unfavorable two-electron mechanism. We have employed the spin polarized density functional theory method to investigate the oxygen reduction reaction activity of the heteroatom p-type beryllium (Be) doped graphene in gas and aqueous media. The preferred doping sites, active sites and reaction mechanisms available on the doped graphene surfaces were investigated with increasing Be concentrations of 0.03 ML, 0.06 ML and 0.09 ML. Our results reveal that oxygen is physisorbed on bare graphene, however, Be at the lattice sites provides site for oxygen adsorption and ORR. Generally, Be concentration increase in a single honey-comb of graphene from 1 to 2, increasing oxygen activation and dissociation on graphene, compared to their isolated defective counterparts. Considering the conjugated Be defective surfaces, oxygen binds dissociatively on the doped surfaces preferentially in the order 0.06 ML > 0.09 ML > 0.03 ML. Whereby strong binding at the 0.06 ML doped surface corresponds to least charge loss to oxygen. Surfaces with the least affinity for O*, OH* and H2O*, and can transfer the most charges to O2 leading to dissociation (as seen on the 0.03 ML surface), shows the highest reaction activity towards the ORR. From these results surfaces that bind O2 weakly and dissociatively could hold promise for the ORR reaction. Single atom catalyst of Be, based on graphene is promising for the ORR.

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Quantum Espresso is an opensource code available at https://www.quantum-espresso.org/

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Acknowledgements

CRK is grateful for the grants from The World Academy of Sciences (TWAS) and Swedish International Development Cooperation Agency (SIDA). CRK and RT acknowledge the UK’s Royal Society and Leverhulme Trust for a research grant under the Royal Society-Leverhulme Africa Postdoctoral Fellowship Award Scheme. Authors acknowledge the Center for High Performance Computing (CHPC), South Africa for additional computing resources.

Funding

CRK is grateful for funding from The World Academy of Sciences (Grant 18–032 RG/CHE/AF/AC_I). CRK and RT acknowledges the UK Royal Society and Leverhulme Trust for a research grant under the Royal Society-Leverhulme Africa Postdoctoral Fellowship Award Scheme (grant LAF\R1\180013).

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Data were collected by Mr. KL and Mr. DK. Manuscript was drafted by Dr. CRK and revised by Dr. EM and Dr. AA. Research concept was developed and supervised by Prof. RT and Prof. EA.

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Correspondence to Caroline R. Kwawu.

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Kwawu, C.R., Aniagyei, A., Konadu, D. et al. A DFT study of the oxygen reduction reaction mechanism on be doped graphene. Chem. Pap. 76, 4471–4480 (2022). https://doi.org/10.1007/s11696-022-02201-4

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  • DOI: https://doi.org/10.1007/s11696-022-02201-4

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