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
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/225718
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/225718
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling 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 Técnicas2025-10-22T11:57:46Zoai: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:34982025-10-22 11:57:46.99CONICET 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
_version_ 1846782289823924224
score 12.982451

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