Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin
- Autores
- Chandra, Shubhadeep; Hazari, Arijit Singha; Song, Qian; Hunger, David; Neuman, Nicolás Ignacio; van Slageren, Joris; Klemm, Elias; Sarkar, Biprajit
- Año de publicación
- 2023
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- A bimetallic triply fused copper(II) porphyrin complex (1) was prepared, comprising two monomeric porphyrin units linked through β–β, meso–meso, β′–β′ triple covalent linkages and exhibiting remarkable catalytic activity for the electrochemical hydrogen evolution reaction in comparison to the analogous monomeric copper(II) porphyrin complex (2). Electrochemical investigations in the presence of a proton source (trifluoroacetic acid) confirmed that the catalytic activity of the fused metalloporphyrin occurred at a significantly lower overpotential (≈320 mV) compared to the non-fused monomer. Controlled potential electrolysis combined with kinetic analysis of catalysts 1 and 2 confirmed production of hydrogen, with 96 and 71 % faradaic efficiencies and turnover numbers of 102 and 18, respectively, with an observed rate constant of around 107 s−1 for the dicopper complex. The results thus firmly establish triply fused porphyrin ligands as outstanding candidates for generating highly stable and efficient molecular electrocatalysts in combination with earth-abundant 3d transition metals.
Fil: Chandra, Shubhadeep. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Hazari, Arijit Singha. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Song, Qian. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Hunger, David. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Neuman, Nicolás Ignacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
Fil: van Slageren, Joris. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Klemm, Elias. Staatliches Museum fur Naturkunde Stuttgart; Alemania
Fil: Sarkar, Biprajit. Staatliches Museum fur Naturkunde Stuttgart; Alemania - Materia
-
COPPER
ELECTROCATALYSIS
FUSED PORPHYRIN
PROTON REDUCTION
TURNOVER NUMBER - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/225718
Ver los metadatos del registro completo
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CONICET Digital (CONICET) |
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Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused PorphyrinChandra, ShubhadeepHazari, Arijit SinghaSong, QianHunger, DavidNeuman, Nicolás Ignaciovan Slageren, JorisKlemm, EliasSarkar, BiprajitCOPPERELECTROCATALYSISFUSED PORPHYRINPROTON REDUCTIONTURNOVER NUMBERhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A bimetallic triply fused copper(II) porphyrin complex (1) was prepared, comprising two monomeric porphyrin units linked through β–β, meso–meso, β′–β′ triple covalent linkages and exhibiting remarkable catalytic activity for the electrochemical hydrogen evolution reaction in comparison to the analogous monomeric copper(II) porphyrin complex (2). Electrochemical investigations in the presence of a proton source (trifluoroacetic acid) confirmed that the catalytic activity of the fused metalloporphyrin occurred at a significantly lower overpotential (≈320 mV) compared to the non-fused monomer. Controlled potential electrolysis combined with kinetic analysis of catalysts 1 and 2 confirmed production of hydrogen, with 96 and 71 % faradaic efficiencies and turnover numbers of 102 and 18, respectively, with an observed rate constant of around 107 s−1 for the dicopper complex. The results thus firmly establish triply fused porphyrin ligands as outstanding candidates for generating highly stable and efficient molecular electrocatalysts in combination with earth-abundant 3d transition metals.Fil: Chandra, Shubhadeep. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Hazari, Arijit Singha. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Song, Qian. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Hunger, David. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Neuman, Nicolás Ignacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; ArgentinaFil: van Slageren, Joris. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Klemm, Elias. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaFil: Sarkar, Biprajit. Staatliches Museum fur Naturkunde Stuttgart; AlemaniaWiley VCH Verlag2023-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/225718Chandra, Shubhadeep; Hazari, Arijit Singha; Song, Qian; Hunger, David; Neuman, Nicolás Ignacio; et al.; Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin; Wiley VCH Verlag; Chemsuschem; 16; 1; 1-2023; 1-121864-5631CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1002/cssc.202201146info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:25:05Zoai:ri.conicet.gov.ar:11336/225718instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 10:25:05.604CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
title |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
spellingShingle |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin Chandra, Shubhadeep COPPER ELECTROCATALYSIS FUSED PORPHYRIN PROTON REDUCTION TURNOVER NUMBER |
title_short |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
title_full |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
title_fullStr |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
title_full_unstemmed |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
title_sort |
Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin |
dc.creator.none.fl_str_mv |
Chandra, Shubhadeep Hazari, Arijit Singha Song, Qian Hunger, David Neuman, Nicolás Ignacio van Slageren, Joris Klemm, Elias Sarkar, Biprajit |
author |
Chandra, Shubhadeep |
author_facet |
Chandra, Shubhadeep Hazari, Arijit Singha Song, Qian Hunger, David Neuman, Nicolás Ignacio van Slageren, Joris Klemm, Elias Sarkar, Biprajit |
author_role |
author |
author2 |
Hazari, Arijit Singha Song, Qian Hunger, David Neuman, Nicolás Ignacio van Slageren, Joris Klemm, Elias Sarkar, Biprajit |
author2_role |
author author author author author author author |
dc.subject.none.fl_str_mv |
COPPER ELECTROCATALYSIS FUSED PORPHYRIN PROTON REDUCTION TURNOVER NUMBER |
topic |
COPPER ELECTROCATALYSIS FUSED PORPHYRIN PROTON REDUCTION TURNOVER NUMBER |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
A bimetallic triply fused copper(II) porphyrin complex (1) was prepared, comprising two monomeric porphyrin units linked through β–β, meso–meso, β′–β′ triple covalent linkages and exhibiting remarkable catalytic activity for the electrochemical hydrogen evolution reaction in comparison to the analogous monomeric copper(II) porphyrin complex (2). Electrochemical investigations in the presence of a proton source (trifluoroacetic acid) confirmed that the catalytic activity of the fused metalloporphyrin occurred at a significantly lower overpotential (≈320 mV) compared to the non-fused monomer. Controlled potential electrolysis combined with kinetic analysis of catalysts 1 and 2 confirmed production of hydrogen, with 96 and 71 % faradaic efficiencies and turnover numbers of 102 and 18, respectively, with an observed rate constant of around 107 s−1 for the dicopper complex. The results thus firmly establish triply fused porphyrin ligands as outstanding candidates for generating highly stable and efficient molecular electrocatalysts in combination with earth-abundant 3d transition metals. Fil: Chandra, Shubhadeep. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Hazari, Arijit Singha. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Song, Qian. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Hunger, David. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Neuman, Nicolás Ignacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina Fil: van Slageren, Joris. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Klemm, Elias. Staatliches Museum fur Naturkunde Stuttgart; Alemania Fil: Sarkar, Biprajit. Staatliches Museum fur Naturkunde Stuttgart; Alemania |
description |
A bimetallic triply fused copper(II) porphyrin complex (1) was prepared, comprising two monomeric porphyrin units linked through β–β, meso–meso, β′–β′ triple covalent linkages and exhibiting remarkable catalytic activity for the electrochemical hydrogen evolution reaction in comparison to the analogous monomeric copper(II) porphyrin complex (2). Electrochemical investigations in the presence of a proton source (trifluoroacetic acid) confirmed that the catalytic activity of the fused metalloporphyrin occurred at a significantly lower overpotential (≈320 mV) compared to the non-fused monomer. Controlled potential electrolysis combined with kinetic analysis of catalysts 1 and 2 confirmed production of hydrogen, with 96 and 71 % faradaic efficiencies and turnover numbers of 102 and 18, respectively, with an observed rate constant of around 107 s−1 for the dicopper complex. The results thus firmly establish triply fused porphyrin ligands as outstanding candidates for generating highly stable and efficient molecular electrocatalysts in combination with earth-abundant 3d transition metals. |
publishDate |
2023 |
dc.date.none.fl_str_mv |
2023-01 |
dc.type.none.fl_str_mv |
info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion http://purl.org/coar/resource_type/c_6501 info:ar-repo/semantics/articulo |
format |
article |
status_str |
publishedVersion |
dc.identifier.none.fl_str_mv |
http://hdl.handle.net/11336/225718 Chandra, Shubhadeep; Hazari, Arijit Singha; Song, Qian; Hunger, David; Neuman, Nicolás Ignacio; et al.; Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin; Wiley VCH Verlag; Chemsuschem; 16; 1; 1-2023; 1-12 1864-5631 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/225718 |
identifier_str_mv |
Chandra, Shubhadeep; Hazari, Arijit Singha; Song, Qian; Hunger, David; Neuman, Nicolás Ignacio; et al.; Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin; Wiley VCH Verlag; Chemsuschem; 16; 1; 1-2023; 1-12 1864-5631 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/doi/10.1002/cssc.202201146 |
dc.rights.none.fl_str_mv |
info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by/2.5/ar/ |
eu_rights_str_mv |
openAccess |
rights_invalid_str_mv |
https://creativecommons.org/licenses/by/2.5/ar/ |
dc.format.none.fl_str_mv |
application/pdf application/pdf |
dc.publisher.none.fl_str_mv |
Wiley VCH Verlag |
publisher.none.fl_str_mv |
Wiley VCH Verlag |
dc.source.none.fl_str_mv |
reponame:CONICET Digital (CONICET) instname:Consejo Nacional de Investigaciones Científicas y Técnicas |
reponame_str |
CONICET Digital (CONICET) |
collection |
CONICET Digital (CONICET) |
instname_str |
Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.name.fl_str_mv |
CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.mail.fl_str_mv |
dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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1844614248684060672 |
score |
13.070432 |