Tailoring the efficiency of porphyrin molecular frameworks for the electroactivation of molecular N 2 .

Autor: Romero-Angel M; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es., Amrine R; Institute of Electrochemistry, University of Alicante Apdo. 99 E-03080 Alicante Spain jose.solla@ua.es., Ávila-Bolívar B; Institute of Electrochemistry, University of Alicante Apdo. 99 E-03080 Alicante Spain jose.solla@ua.es., Almora-Barrios N; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es., Ganivet CR; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es., Padial NM; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es., Montiel V; Institute of Electrochemistry, University of Alicante Apdo. 99 E-03080 Alicante Spain jose.solla@ua.es., Solla-Gullón J; Institute of Electrochemistry, University of Alicante Apdo. 99 E-03080 Alicante Spain jose.solla@ua.es., Tatay S; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es., Martí-Gastaldo C; Instituto de Ciencia Molecular, Universidad de València c/Catedrático José Beltrán, 2 46980 Paterna Spain sergio.tatay@uv.es carlos.marti@uv.es.
Jazyk: angličtina
Zdroj: Journal of materials chemistry. A [J Mater Chem A Mater] 2024 Mar 25; Vol. 12 (18), pp. 10956-10964. Date of Electronic Publication: 2024 Mar 25 (Print Publication: 2024).
DOI: 10.1039/d3ta07004b
Abstrakt: 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 Ni 2+ 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.
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE