Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction
Current selective modification methods, coupled with functionalization through organic or inorganic molecules, are crucial for designing and constructing custom-made molecular materials that act as electroactive interfaces. A versatile method for derivatizing surfaces is through an aryl diazonium sa...
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MDPI AG
2021-03-01
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author | Camila F. Olguín Nicolás Agurto Carlos P. Silva Carolina P. Candia Mireya Santander-Nelli Juan Oyarzo Alejandra Gómez Juan F. Silva Jorge Pavez |
author_facet | Camila F. Olguín Nicolás Agurto Carlos P. Silva Carolina P. Candia Mireya Santander-Nelli Juan Oyarzo Alejandra Gómez Juan F. Silva Jorge Pavez |
author_sort | Camila F. Olguín |
collection | DOAJ |
description | Current selective modification methods, coupled with functionalization through organic or inorganic molecules, are crucial for designing and constructing custom-made molecular materials that act as electroactive interfaces. A versatile method for derivatizing surfaces is through an aryl diazonium salt reduction reaction (DSRR). A prominent feature of this strategy is that it can be carried out on various materials. Using the DSRR, we modified gold surface electrodes with 4-aminebenzene from 4-nitrobenzenediazonium tetrafluoroborate (NBTF), regulating the deposited mass of the aryl film to achieve covering control on the electrode surface. We got different degrees of covering: monolayer, intermediate, and multilayer. Afterwards, the ArNO<sub>2</sub> end groups were electrochemically reduced to ArNH<sub>2</sub> and functionalized with Fe(II)-Phthalocyanine to study the catalytic performance for the oxygen reduction reaction (ORR). The thickness of the electrode covering determines its response in front of ORR. Interestingly, the experimental results showed that an intermediate covering film presents a better electrocatalytic response for ORR, driving the reaction by a four-electron pathway. |
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series | Molecules |
spelling | doaj.art-f17a1c9272f743f4ac4db5326d80aa922023-11-21T10:33:59ZengMDPI AGMolecules1420-30492021-03-01266163110.3390/molecules26061631Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen ReductionCamila F. Olguín0Nicolás Agurto1Carlos P. Silva2Carolina P. Candia3Mireya Santander-Nelli4Juan Oyarzo5Alejandra Gómez6Juan F. Silva7Jorge Pavez8Universidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileInstituto de Química, Pontificia Universidad Católica de Valparaíso, Valparaíso 2374631, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileUniversidad de Santiago de Chile (USACH), Faculty of Chemistry and Biology, Department of Chemistry of the Materials, Soft Matter Research and Technology Center, SMAT-C. Av. Libertador B. O’Higgins 3363, Box 40, Correo 33, Santiago 9170022, ChileCurrent selective modification methods, coupled with functionalization through organic or inorganic molecules, are crucial for designing and constructing custom-made molecular materials that act as electroactive interfaces. A versatile method for derivatizing surfaces is through an aryl diazonium salt reduction reaction (DSRR). A prominent feature of this strategy is that it can be carried out on various materials. Using the DSRR, we modified gold surface electrodes with 4-aminebenzene from 4-nitrobenzenediazonium tetrafluoroborate (NBTF), regulating the deposited mass of the aryl film to achieve covering control on the electrode surface. We got different degrees of covering: monolayer, intermediate, and multilayer. Afterwards, the ArNO<sub>2</sub> end groups were electrochemically reduced to ArNH<sub>2</sub> and functionalized with Fe(II)-Phthalocyanine to study the catalytic performance for the oxygen reduction reaction (ORR). The thickness of the electrode covering determines its response in front of ORR. Interestingly, the experimental results showed that an intermediate covering film presents a better electrocatalytic response for ORR, driving the reaction by a four-electron pathway.https://www.mdpi.com/1420-3049/26/6/1631grafting covering controlaryl diazonium saltFe(II) Phthalocyanineoxygen reduction reaction |
spellingShingle | Camila F. Olguín Nicolás Agurto Carlos P. Silva Carolina P. Candia Mireya Santander-Nelli Juan Oyarzo Alejandra Gómez Juan F. Silva Jorge Pavez Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction Molecules grafting covering control aryl diazonium salt Fe(II) Phthalocyanine oxygen reduction reaction |
title | Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction |
title_full | Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction |
title_fullStr | Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction |
title_full_unstemmed | Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction |
title_short | Tuning the Covering on Gold Surfaces by Grafting Amino-Aryl Films Functionalized with Fe(II) Phthalocyanine: Performance on the Electrocatalysis of Oxygen Reduction |
title_sort | tuning the covering on gold surfaces by grafting amino aryl films functionalized with fe ii phthalocyanine performance on the electrocatalysis of oxygen reduction |
topic | grafting covering control aryl diazonium salt Fe(II) Phthalocyanine oxygen reduction reaction |
url | https://www.mdpi.com/1420-3049/26/6/1631 |
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