Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups
The search of active, stable and low costs catalysts for the oxygen reduction reaction (ORR) is crucial for the extensive use of fuel cells and metal–air batteries. The development of metal-free catalysts, instead of platinum-based materials, can dramatically reduce the cost and increase the efficie...
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MDPI AG
2023-07-01
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Series: | Surfaces |
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Online Access: | https://www.mdpi.com/2571-9637/6/3/15 |
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author | Elisa Tosin Teresa Gatti Stefano Agnoli Laura Calvillo Enzo Menna |
author_facet | Elisa Tosin Teresa Gatti Stefano Agnoli Laura Calvillo Enzo Menna |
author_sort | Elisa Tosin |
collection | DOAJ |
description | The search of active, stable and low costs catalysts for the oxygen reduction reaction (ORR) is crucial for the extensive use of fuel cells and metal–air batteries. The development of metal-free catalysts, instead of platinum-based materials, can dramatically reduce the cost and increase the efficiency of these devices. In this work, carbon nanohorns (CNHs) have been covalently functionalized with N-containing heterocycles by the Tour reaction protocol and tested as metal-free ORR catalysts. The insertion of N-functionalities favored the complete reduction of oxygen to hydroxyl ions, while their absence favored the production of hydrogen peroxide. With the aim of determining the N-species responsible for the ORR activity of CNHs, photoemission and electrochemical measurements were combined. Results suggest that protonated N is the main species involved in the ORR process, facilitating the adsorption of oxygen, with their consequent reduction to neutral hydrogenated N species. |
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id | doaj.art-d2e13e109eb444819a486da87a92e3e8 |
institution | Directory Open Access Journal |
issn | 2571-9637 |
language | English |
last_indexed | 2024-03-10T21:59:47Z |
publishDate | 2023-07-01 |
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series | Surfaces |
spelling | doaj.art-d2e13e109eb444819a486da87a92e3e82023-11-19T13:01:00ZengMDPI AGSurfaces2571-96372023-07-016322723810.3390/surfaces6030015Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen GroupsElisa Tosin0Teresa Gatti1Stefano Agnoli2Laura Calvillo3Enzo Menna4Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padova, ItalyDepartment of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padova, ItalyDepartment of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padova, ItalyDepartment of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padova, ItalyDepartment of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padova, ItalyThe search of active, stable and low costs catalysts for the oxygen reduction reaction (ORR) is crucial for the extensive use of fuel cells and metal–air batteries. The development of metal-free catalysts, instead of platinum-based materials, can dramatically reduce the cost and increase the efficiency of these devices. In this work, carbon nanohorns (CNHs) have been covalently functionalized with N-containing heterocycles by the Tour reaction protocol and tested as metal-free ORR catalysts. The insertion of N-functionalities favored the complete reduction of oxygen to hydroxyl ions, while their absence favored the production of hydrogen peroxide. With the aim of determining the N-species responsible for the ORR activity of CNHs, photoemission and electrochemical measurements were combined. Results suggest that protonated N is the main species involved in the ORR process, facilitating the adsorption of oxygen, with their consequent reduction to neutral hydrogenated N species.https://www.mdpi.com/2571-9637/6/3/15carbon nanohornsnitrogen groupsoxygen reduction reactionin line XPS |
spellingShingle | Elisa Tosin Teresa Gatti Stefano Agnoli Laura Calvillo Enzo Menna Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups Surfaces carbon nanohorns nitrogen groups oxygen reduction reaction in line XPS |
title | Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups |
title_full | Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups |
title_fullStr | Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups |
title_full_unstemmed | Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups |
title_short | Nitrogen- and Fluorine-Doped Carbon Nanohorns as Efficient Metal-Free Oxygen Reduction Catalyst: Role of the Nitrogen Groups |
title_sort | nitrogen and fluorine doped carbon nanohorns as efficient metal free oxygen reduction catalyst role of the nitrogen groups |
topic | carbon nanohorns nitrogen groups oxygen reduction reaction in line XPS |
url | https://www.mdpi.com/2571-9637/6/3/15 |
work_keys_str_mv | AT elisatosin nitrogenandfluorinedopedcarbonnanohornsasefficientmetalfreeoxygenreductioncatalystroleofthenitrogengroups AT teresagatti nitrogenandfluorinedopedcarbonnanohornsasefficientmetalfreeoxygenreductioncatalystroleofthenitrogengroups AT stefanoagnoli nitrogenandfluorinedopedcarbonnanohornsasefficientmetalfreeoxygenreductioncatalystroleofthenitrogengroups AT lauracalvillo nitrogenandfluorinedopedcarbonnanohornsasefficientmetalfreeoxygenreductioncatalystroleofthenitrogengroups AT enzomenna nitrogenandfluorinedopedcarbonnanohornsasefficientmetalfreeoxygenreductioncatalystroleofthenitrogengroups |