Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution

Abstract Non-precious electrocatalysts as the alternative to Pt have become a hot research area in the last decade due to the suitable catalytic activity in Oxygen reduction reaction (ORR) in electrochemical systems. In this work, the density functional theory calculations were investigated to explo...

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Main Authors: Tahereh Jangjooye Shaldehi, Soosan Rowshanzamir
Format: Article
Language:English
Published: Nature Portfolio 2024-06-01
Series:Scientific Reports
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Online Access:https://doi.org/10.1038/s41598-024-61223-y
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author Tahereh Jangjooye Shaldehi
Soosan Rowshanzamir
author_facet Tahereh Jangjooye Shaldehi
Soosan Rowshanzamir
author_sort Tahereh Jangjooye Shaldehi
collection DOAJ
description Abstract Non-precious electrocatalysts as the alternative to Pt have become a hot research area in the last decade due to the suitable catalytic activity in Oxygen reduction reaction (ORR) in electrochemical systems. In this work, the density functional theory calculations were investigated to explore the activity of Fe, Cu, and Fe-Cu atoms supported by N-doped graphene as the ORR electrocatalyst for Oxygen-depolarized cathodes (ODCs). To this end, the ORR mechanism was surveyed in detail in the gas and solvent phases. The results show that the solvent phase leads to a higher overpotential and thermodynamic limiting potential. According to the density of states curves, there are strong interactions between metal atom and substrate that can effectively tune the electronics of catalysts. Bader's analysis confirms that, in addition to the single metal atoms, nitrogen atoms have also played a critical role in charge transfer between substrates and oxygen molecules in ORR. It is also predicted that Fe-Cu@NC SAC exhibits the highest catalytic activity which is consistent with thermodynamic limiting potential and theoretical overpotential of  − 0.26 and  0.66 (V vs. SHE), respectively, indicating that this type of catalyst may be a suitable candidate instead of precious metals in oxygen-depolarized cathodes in electrochemical devices.
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spelling doaj-art-431b0005e29a4401899ff81b763ac26d2024-12-22T12:25:33ZengNature PortfolioScientific Reports2045-23222024-06-011411910.1038/s41598-024-61223-yTheoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solutionTahereh Jangjooye Shaldehi0Soosan Rowshanzamir1Hydrogen & Fuel Cell Research Laboratory, School of Chemical, Petroleum and Gas Engineering, Iran University of Science and TechnologyHydrogen & Fuel Cell Research Laboratory, School of Chemical, Petroleum and Gas Engineering, Iran University of Science and TechnologyAbstract Non-precious electrocatalysts as the alternative to Pt have become a hot research area in the last decade due to the suitable catalytic activity in Oxygen reduction reaction (ORR) in electrochemical systems. In this work, the density functional theory calculations were investigated to explore the activity of Fe, Cu, and Fe-Cu atoms supported by N-doped graphene as the ORR electrocatalyst for Oxygen-depolarized cathodes (ODCs). To this end, the ORR mechanism was surveyed in detail in the gas and solvent phases. The results show that the solvent phase leads to a higher overpotential and thermodynamic limiting potential. According to the density of states curves, there are strong interactions between metal atom and substrate that can effectively tune the electronics of catalysts. Bader's analysis confirms that, in addition to the single metal atoms, nitrogen atoms have also played a critical role in charge transfer between substrates and oxygen molecules in ORR. It is also predicted that Fe-Cu@NC SAC exhibits the highest catalytic activity which is consistent with thermodynamic limiting potential and theoretical overpotential of  − 0.26 and  0.66 (V vs. SHE), respectively, indicating that this type of catalyst may be a suitable candidate instead of precious metals in oxygen-depolarized cathodes in electrochemical devices.https://doi.org/10.1038/s41598-024-61223-yDensity functional theoryOxygen reduction reactionDual atom electrocatalystAlkaline solution
spellingShingle Tahereh Jangjooye Shaldehi
Soosan Rowshanzamir
Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
Scientific Reports
Density functional theory
Oxygen reduction reaction
Dual atom electrocatalyst
Alkaline solution
title Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
title_full Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
title_fullStr Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
title_full_unstemmed Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
title_short Theoretical investigation of electrocatalytic activity of Pt-free dual atom-doped graphene for O2 reduction in an alkaline solution
title_sort theoretical investigation of electrocatalytic activity of pt free dual atom doped graphene for o2 reduction in an alkaline solution
topic Density functional theory
Oxygen reduction reaction
Dual atom electrocatalyst
Alkaline solution
url https://doi.org/10.1038/s41598-024-61223-y
work_keys_str_mv AT taherehjangjooyeshaldehi theoreticalinvestigationofelectrocatalyticactivityofptfreedualatomdopedgrapheneforo2reductioninanalkalinesolution
AT soosanrowshanzamir theoreticalinvestigationofelectrocatalyticactivityofptfreedualatomdopedgrapheneforo2reductioninanalkalinesolution