New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis

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This research was supported by the Center for Catalytic Hydrocarbon Functionalization, Number DE-SC0001298 (D.L.H. and R.H.C.), and Argonne-Northwestern Solar Energy Research (ANSER), Number DE-SC0001059 (J.M.T., R.-B.S., K.L.M. and G.W.B.); both agencies are Energy Frontier Research Centers funded...

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Autores: Huang, DL, Beltran-Suito, R, Thomsen, JM, Hashmi, SM, Materna, KL, Sheehan, SW, Mercado, BQ, Brudvig, GW, Crabtree, RH
Formato: artículo
Fecha de Publicación:2016
Institución:Consejo Nacional de Ciencia Tecnología e Innovación
Repositorio:CONCYTEC-Institucional
Lenguaje:inglés
OAI Identifier:oai:repositorio.concytec.gob.pe:20.500.12390/1080
Enlace del recurso:https://hdl.handle.net/20.500.12390/1080
https://doi.org/10.1021/acs.inorgchem.5b02809
Nivel de acceso:acceso abierto
Materia:water oxidation catalyst
atom-efficient precursor
oxidation catalysis
https://purl.org/pe-repo/ocde/ford#1.04.00
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oai_identifier_str oai:repositorio.concytec.gob.pe:20.500.12390/1080
network_acronym_str CONC
network_name_str CONCYTEC-Institucional
repository_id_str 4689
dc.title.none.fl_str_mv New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
title New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
spellingShingle New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
Huang, DL
water oxidation catalyst
atom-efficient precursor
atom-efficient precursor
oxidation catalysis
https://purl.org/pe-repo/ocde/ford#1.04.00
title_short New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
title_full New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
title_fullStr New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
title_full_unstemmed New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
title_sort New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
author Huang, DL
author_facet Huang, DL
Beltran-Suito, R
Thomsen, JM
Hashmi, SM
Materna, KL
Sheehan, SW
Mercado, BQ
Brudvig, GW
Crabtree, RH
author_role author
author2 Beltran-Suito, R
Thomsen, JM
Hashmi, SM
Materna, KL
Sheehan, SW
Mercado, BQ
Brudvig, GW
Crabtree, RH
author2_role author
author
author
author
author
author
author
author
dc.contributor.author.fl_str_mv Huang, DL
Beltran-Suito, R
Thomsen, JM
Hashmi, SM
Materna, KL
Sheehan, SW
Mercado, BQ
Brudvig, GW
Crabtree, RH
dc.subject.none.fl_str_mv water oxidation catalyst
topic water oxidation catalyst
atom-efficient precursor
atom-efficient precursor
oxidation catalysis
https://purl.org/pe-repo/ocde/ford#1.04.00
dc.subject.es_PE.fl_str_mv atom-efficient precursor
atom-efficient precursor
oxidation catalysis
dc.subject.ocde.none.fl_str_mv https://purl.org/pe-repo/ocde/ford#1.04.00
description This research was supported by the Center for Catalytic Hydrocarbon Functionalization, Number DE-SC0001298 (D.L.H. and R.H.C.), and Argonne-Northwestern Solar Energy Research (ANSER), Number DE-SC0001059 (J.M.T., R.-B.S., K.L.M. and G.W.B.); both agencies are Energy Frontier Research Centers funded by the U.S. Department of Energy. D.L.H acknowledges support by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1122492 and the Yale Dox Summer Research Fellowship. R.-B.S. R. B.-S. acknowledges support from the Consejo Nacional de Ciencia, Tecnologia e Innovacio ́ ́n Tecnologica (CONCYTEC), and the Ponti ́ ficia Universidad Catolica del Peru ́ ́(PUCP). DLS measurements were conducted in the Yale Facility for Light Scattering. We thank Liam Sharninghausen for assistance with crystallography and Dr. Eric Paulson for assistance with DOSY NMR spectroscopy.
publishDate 2016
dc.date.accessioned.none.fl_str_mv 2024-05-30T23:13:38Z
dc.date.available.none.fl_str_mv 2024-05-30T23:13:38Z
dc.date.issued.fl_str_mv 2016
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.uri.none.fl_str_mv https://hdl.handle.net/20.500.12390/1080
dc.identifier.doi.none.fl_str_mv https://doi.org/10.1021/acs.inorgchem.5b02809
dc.identifier.isi.none.fl_str_mv 371753500053
url https://hdl.handle.net/20.500.12390/1080
https://doi.org/10.1021/acs.inorgchem.5b02809
identifier_str_mv 371753500053
dc.language.iso.none.fl_str_mv eng
language eng
dc.relation.ispartof.none.fl_str_mv Inorganic Chemistry
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv ACS Publications
publisher.none.fl_str_mv ACS Publications
dc.source.none.fl_str_mv reponame:CONCYTEC-Institucional
instname:Consejo Nacional de Ciencia Tecnología e Innovación
instacron:CONCYTEC
instname_str Consejo Nacional de Ciencia Tecnología e Innovación
instacron_str CONCYTEC
institution CONCYTEC
reponame_str CONCYTEC-Institucional
collection CONCYTEC-Institucional
repository.name.fl_str_mv Repositorio Institucional CONCYTEC
repository.mail.fl_str_mv repositorio@concytec.gob.pe
_version_ 1839175822820245504
spelling Publicationrp03077600rp03078600rp03076600rp03073600rp03075600rp03079600rp03080600rp03074600rp03081600Huang, DLBeltran-Suito, RThomsen, JMHashmi, SMMaterna, KLSheehan, SWMercado, BQBrudvig, GWCrabtree, RH2024-05-30T23:13:38Z2024-05-30T23:13:38Z2016https://hdl.handle.net/20.500.12390/1080https://doi.org/10.1021/acs.inorgchem.5b02809371753500053This research was supported by the Center for Catalytic Hydrocarbon Functionalization, Number DE-SC0001298 (D.L.H. and R.H.C.), and Argonne-Northwestern Solar Energy Research (ANSER), Number DE-SC0001059 (J.M.T., R.-B.S., K.L.M. and G.W.B.); both agencies are Energy Frontier Research Centers funded by the U.S. Department of Energy. D.L.H acknowledges support by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1122492 and the Yale Dox Summer Research Fellowship. R.-B.S. R. B.-S. acknowledges support from the Consejo Nacional de Ciencia, Tecnologia e Innovacio ́ ́n Tecnologica (CONCYTEC), and the Ponti ́ ficia Universidad Catolica del Peru ́ ́(PUCP). DLS measurements were conducted in the Yale Facility for Light Scattering. We thank Liam Sharninghausen for assistance with crystallography and Dr. Eric Paulson for assistance with DOSY NMR spectroscopy.This paper introduces IrI(CO)2(pyalc) (pyalc = (2-pyridyl)-2-propanoate) as an atom-efficient precursor for Ir-based homogeneous oxidation catalysis. This compound was chosen to simplify analysis of the water oxidation catalyst species formed by the previously reported Cp*IrIII(pyalc)OH water oxidation precatalyst. Here, we present a comparative study on the chemical and catalytic properties of these two precursors. Previous studies show that oxidative activation of Cp*Ir-based precursors with NaIO4 results in formation of a blue IrIV species. This activation is concomitant with the loss of the placeholder Cp* ligand which oxidatively degrades to form acetic acid, iodate, and other obligatory byproducts. The activation process requires substantial amounts of primary oxidant, and the degradation products complicate analysis of the resulting IrIV species. The species formed from oxidation of the Ir(CO)2(pyalc) precursor, on the other hand, lacks these degradation products (the CO ligands are easily lost upon oxidation) which allows for more detailed examination of the resulting Ir(pyalc) active species both catalytically and spectroscopically, although complete structural analysis is still elusive. Once Ir(CO)2(pyalc) is activated, the system requires acetic acid or acetate to prevent the formation of nanoparticles. Investigation of the activated bis-carbonyl complex also suggests several Ir(pyalc) isomers may exist in solution. By 1H NMR, activated Ir(CO)2(pyalc) has fewer isomers than activated Cp*Ir complexes, allowing for advanced characterization. Future research in this direction is expected to contribute to a better structural understanding of the active species. A diol crystallization agent was needed for the structure determination of 3.Consejo Nacional de Ciencia, Tecnología e Innovación Tecnológica - ConcytecengACS PublicationsInorganic Chemistryinfo:eu-repo/semantics/openAccesswater oxidation catalystatom-efficient precursor-1atom-efficient precursor-1oxidation catalysis-1https://purl.org/pe-repo/ocde/ford#1.04.00-1New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysisinfo:eu-repo/semantics/articlereponame:CONCYTEC-Institucionalinstname:Consejo Nacional de Ciencia Tecnología e Innovacióninstacron:CONCYTEC#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#20.500.12390/1080oai:repositorio.concytec.gob.pe:20.500.12390/10802024-05-30 15:36:24.059http://purl.org/coar/access_right/c_14cbinfo:eu-repo/semantics/closedAccessmetadata only accesshttps://repositorio.concytec.gob.peRepositorio Institucional CONCYTECrepositorio@concytec.gob.pe#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#<Publication xmlns="https://www.openaire.eu/cerif-profile/1.1/" id="f5634574-5dbc-4be0-8f66-962712c28959"> <Type xmlns="https://www.openaire.eu/cerif-profile/vocab/COAR_Publication_Types">http://purl.org/coar/resource_type/c_1843</Type> <Language>eng</Language> <Title>New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis</Title> <PublishedIn> <Publication> <Title>Inorganic Chemistry</Title> </Publication> </PublishedIn> <PublicationDate>2016</PublicationDate> <DOI>https://doi.org/10.1021/acs.inorgchem.5b02809</DOI> <ISI-Number>371753500053</ISI-Number> <Authors> <Author> <DisplayName>Huang, DL</DisplayName> <Person id="rp03077" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Beltran-Suito, R</DisplayName> <Person id="rp03078" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Thomsen, JM</DisplayName> <Person id="rp03076" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Hashmi, SM</DisplayName> <Person id="rp03073" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Materna, KL</DisplayName> <Person id="rp03075" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Sheehan, SW</DisplayName> <Person id="rp03079" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Mercado, BQ</DisplayName> <Person id="rp03080" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Brudvig, GW</DisplayName> <Person id="rp03074" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> <Author> <DisplayName>Crabtree, RH</DisplayName> <Person id="rp03081" /> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> </Authors> <Editors> </Editors> <Publishers> <Publisher> <DisplayName>ACS Publications</DisplayName> <OrgUnit /> </Publisher> </Publishers> <Keyword>water oxidation catalyst</Keyword> <Keyword>atom-efficient precursor</Keyword> <Keyword>atom-efficient precursor</Keyword> <Keyword>oxidation catalysis</Keyword> <Abstract>This paper introduces IrI(CO)2(pyalc) (pyalc = (2-pyridyl)-2-propanoate) as an atom-efficient precursor for Ir-based homogeneous oxidation catalysis. This compound was chosen to simplify analysis of the water oxidation catalyst species formed by the previously reported Cp*IrIII(pyalc)OH water oxidation precatalyst. Here, we present a comparative study on the chemical and catalytic properties of these two precursors. Previous studies show that oxidative activation of Cp*Ir-based precursors with NaIO4 results in formation of a blue IrIV species. This activation is concomitant with the loss of the placeholder Cp* ligand which oxidatively degrades to form acetic acid, iodate, and other obligatory byproducts. The activation process requires substantial amounts of primary oxidant, and the degradation products complicate analysis of the resulting IrIV species. The species formed from oxidation of the Ir(CO)2(pyalc) precursor, on the other hand, lacks these degradation products (the CO ligands are easily lost upon oxidation) which allows for more detailed examination of the resulting Ir(pyalc) active species both catalytically and spectroscopically, although complete structural analysis is still elusive. Once Ir(CO)2(pyalc) is activated, the system requires acetic acid or acetate to prevent the formation of nanoparticles. Investigation of the activated bis-carbonyl complex also suggests several Ir(pyalc) isomers may exist in solution. By 1H NMR, activated Ir(CO)2(pyalc) has fewer isomers than activated Cp*Ir complexes, allowing for advanced characterization. Future research in this direction is expected to contribute to a better structural understanding of the active species. A diol crystallization agent was needed for the structure determination of 3.</Abstract> <Access xmlns="http://purl.org/coar/access_right" > </Access> </Publication> -1
score 13.33131
New Ir Bis-Carbonyl Precursor for Water Oxidation Catalysis
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