Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)

This article also appears in: Doug Stephan 70th Birthday.

Detalles Bibliográficos
Autores: Moreno, Juan J., Pita-Milleiro, Alejandra, Luque-Gómez, Ana, Espada, María F., López-Serrano, Joaquín, Campos, Jesús
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/340575
Acceso en línea:http://hdl.handle.net/10261/340575
https://api.elsevier.com/content/abstract/scopus_id/85147557964
Access Level:acceso abierto
Palabra clave:Iridium
Bimetallic
Bulky phosphine
Cooperative
Frustrated Lewis pair
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spelling Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)Moreno, Juan J.Pita-Milleiro, AlejandraLuque-Gómez, AnaEspada, María F.López-Serrano, JoaquínCampos, JesúsIridiumBimetallicBulky phosphineCooperativeFrustrated Lewis pairThis article also appears in: Doug Stephan 70th Birthday.The incorporation of transition metals into frustrated Lewis pairs (FLPs) offers multiple opportunities for bond activation and catalysis. In this work, we explore the combination of the Lewis acidic Ir(III) cation [(η5-C5Me5)IrCl(PMe2ArDipp2)]+ (ArDipp2=C6H3−2,6-(C6H3−2,6-iPr2)2) with the Lewis basic Pt(0) compound Pt(PtBu3)2. The bulkiness of the phosphine ligands prevents the formation of a bimetallic adduct. We have explored the cooperative cleavage of dihydrogen to gauge bimetallic FLP reactivity. As anticipated, compounds [(η5-C5Me5)Ir(Cl)(H)(PMe2ArDipp2)] and [PtH(PtBu3)2]+ are rapidly formed, which suggests an actual FLP mechanism operating. However, our in-depth experimental/computational study evidences that the whole process is considerably more complicated. Instead of a genuine FLP-type activation, we favor a synergistic route that entails a number of equilibrium processes and the Brønsted catalyzed hydrogenation of the Pt(0) precursor.This work has been supported by the European Research Council (ERC Starting Grant, CoopCat, 756575). We also thank Grant PID2019-110856GA−I00 funded by MCIN/AEI/10.13039/501100011033, Junta de Andalucía (P18-FR-4688) and US/JUNTA/FEDER, UE (US-1380849). J.J.M. thanks Junta de Andalucía for the postdoctoral program “Personal Investigador Doctor” (ref. DOC_00153). The project that gave rise to these results received the support of a fellowship from ”laCaixa” Foundation (ID 100010434).Peer reviewedJohn Wiley & SonsEuropean Research CouncilMinisterio de Ciencia e Innovación (España)Agencia Estatal de Investigación (España)European CommissionJunta de AndalucíaFundación la CaixaConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202320232023info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/340575https://api.elsevier.com/content/abstract/scopus_id/85147557964reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/H2020/756575info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-110856GA-I00Moreno, Juan J.; Pita-Milleiro, Alejandra; Luque-Gómez, Ana; Espada, María F.; López-Serrano, Joaquín; Campos, Jesús; 2023; Supporting Information. Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0) [Dataset]; John Wiley & Sons; https://doi.org/10.1002/zaac.202300003https://doi.org/10.1002/zaac.202300003Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3405752026-05-22T06:33:51Z
dc.title.none.fl_str_mv Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
title Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
spellingShingle Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
Moreno, Juan J.
Iridium
Bimetallic
Bulky phosphine
Cooperative
Frustrated Lewis pair
title_short Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
title_full Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
title_fullStr Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
title_full_unstemmed Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
title_sort Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0)
dc.creator.none.fl_str_mv Moreno, Juan J.
Pita-Milleiro, Alejandra
Luque-Gómez, Ana
Espada, María F.
López-Serrano, Joaquín
Campos, Jesús
author Moreno, Juan J.
author_facet Moreno, Juan J.
Pita-Milleiro, Alejandra
Luque-Gómez, Ana
Espada, María F.
López-Serrano, Joaquín
Campos, Jesús
author_role author
author2 Pita-Milleiro, Alejandra
Luque-Gómez, Ana
Espada, María F.
López-Serrano, Joaquín
Campos, Jesús
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv European Research Council
Ministerio de Ciencia e Innovación (España)
Agencia Estatal de Investigación (España)
European Commission
Junta de Andalucía
Fundación la Caixa
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Iridium
Bimetallic
Bulky phosphine
Cooperative
Frustrated Lewis pair
topic Iridium
Bimetallic
Bulky phosphine
Cooperative
Frustrated Lewis pair
description This article also appears in: Doug Stephan 70th Birthday.
publishDate 2023
dc.date.none.fl_str_mv 2023
2023
2023
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/340575
https://api.elsevier.com/content/abstract/scopus_id/85147557964
url http://hdl.handle.net/10261/340575
https://api.elsevier.com/content/abstract/scopus_id/85147557964
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/H2020/756575
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-110856GA-I00
Moreno, Juan J.; Pita-Milleiro, Alejandra; Luque-Gómez, Ana; Espada, María F.; López-Serrano, Joaquín; Campos, Jesús; 2023; Supporting Information. Mechanism of Dihydrogen Splitting by An Apparent Bimetallic Frustrated Lewis Pair based on Ir(III)/Pt(0) [Dataset]; John Wiley & Sons; https://doi.org/10.1002/zaac.202300003
https://doi.org/10.1002/zaac.202300003
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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repository.mail.fl_str_mv
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