Tailoring the efficiency of porphyrin molecular frameworks for the electroactivation of molecular N2
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Title: | Tailoring the efficiency of porphyrin molecular frameworks for the electroactivation of molecular N2 |
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Authors: | Romero-Angel, María | Amrine, Roumayssa | Avila-Bolivar, Beatriz | Almora-Barrios, Neyvis | Ganivet, Carolina R. | Padial, Natalia M. | Montiel, Vicente | Solla-Gullón, José | Tatay, Sergio | Martí-Gastaldo, Carlos |
Research Group/s: | Electroquímica Aplicada y Electrocatálisis |
Center, Department or Service: | Universidad de Alicante. Departamento de Química Física | Universidad de Alicante. Instituto Universitario de Electroquímica |
Keywords: | Metal–organic frameworks | Molecular N2 | Electroactivation | Porphyrin |
Issue Date: | 25-Mar-2024 |
Publisher: | Royal Society of Chemistry |
Citation: | Journal of Materials Chemistry A. 2024, 12: 10956-10964. https://doi.org/10.1039/D3TA07004B |
Abstract: | The combination of compositional versatility and topological diversity for the integration of electroactive species into high-porosity molecular architectures is perhaps one of the main appeals of metal–organic frameworks (MOFs) in the field of electrocatalysis. This premise has attracted much interest in recent years, and the results generated have also revealed one of the main limitations of molecular materials in this context: low stability under electrocatalytic conditions. Using zirconium MOFs as a starting point, in this work, we use this stability as a variable to discriminate between the most suitable electrocatalytic reaction and specific topologies within this family. Our results revealed that the PCN-224 family is particularly suitable for the electroreduction of molecular nitrogen for the formation of ammonia with faradaic efficiencies above 30% in the presence of Ni2+ sites, an activity that improves most of the catalysts described. We also introduce the fluorination of porphyrin at the meso position as a good alternative to improve both the activity and stability of this material under electrocatalytic conditions. |
Sponsor: | This work was supported by the H2020 Program (ERC-2021-COG-101043428), the Generalitat Valenciana (PROMETEU/2021/054, IDIFEDER/2021/075, MFA/2022/026 and SEJIGENT/2021/059), the Spanish Government (RTI2018-098568-A-I00, CEX2019-000919-M, PID2020-118117RB-I00, EUR2021-121999 & CNS2022-135677), and VLC-Biomed AP2022-5. M. R. A. acknowledges the Spanish Government for a predoctoral grant (PRE-C-2018-0109) and S. T. for a RyC contract (RYC-2016-19817). N. M. P. thanks the La Caixa Foundation for a Postdoctoral Junior Leader–Retaining Fellowship (ID 100010434, fellowship code LCF/BQ/PR20/11770014). We also thank the University of Valencia for research facilities (NANBIOSIS). R. A. acknowledges the Ministry of Higher Education and Scientific Research of the People's Democratic Republic of Algeria for the financial support to carry out her PhD study at the University of Alicante, Spain. |
URI: | http://hdl.handle.net/10045/142151 |
ISSN: | 2050-7488 (Print) | 2050-7496 (Online) |
DOI: | 10.1039/D3TA07004B |
Language: | eng |
Type: | info:eu-repo/semantics/article |
Rights: | This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. |
Peer Review: | si |
Publisher version: | https://doi.org/10.1039/D3TA07004B |
Appears in Collections: | Research funded by the EU INV - LEQA - Artículos de Revistas |
Files in This Item:
File | Description | Size | Format | |
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Romero-Angel_etal_2024_JMaterChemA.pdf | 1,02 MB | Adobe PDF | Open Preview | |
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