Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex

We have generated a high-spin Fe(III)-OOH complex supported by tetramethylcyclam via protonation of its conjugate base and characterized it in detail using various spectroscopic methods. This Fe(III)-OOH species can be converted quantitatively to an Fe(IV)═O complex via O-O bond cleavage; this is th...

Ausführliche Beschreibung

Gespeichert in:
Bibliographische Detailangaben
Veröffentlicht in:Journal of the American Chemical Society 2011-05, Vol.133 (19), p.7256-7259
Hauptverfasser: Li, Feifei, Meier, Katlyn K, Cranswick, Matthew A, Chakrabarti, Mrinmoy, Van Heuvelen, Katherine M, Münck, Eckard, Que, Lawrence
Format: Artikel
Sprache:eng
Schlagworte:
Online-Zugang:Volltext
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
container_end_page 7259
container_issue 19
container_start_page 7256
container_title Journal of the American Chemical Society
container_volume 133
creator Li, Feifei
Meier, Katlyn K
Cranswick, Matthew A
Chakrabarti, Mrinmoy
Van Heuvelen, Katherine M
Münck, Eckard
Que, Lawrence
description We have generated a high-spin Fe(III)-OOH complex supported by tetramethylcyclam via protonation of its conjugate base and characterized it in detail using various spectroscopic methods. This Fe(III)-OOH species can be converted quantitatively to an Fe(IV)═O complex via O-O bond cleavage; this is the first example of such a conversion. This conversion is promoted by two factors: the strong Fe(III)-OOH bond, which inhibits Fe-O bond lysis, and the addition of protons, which facilitates O-O bond cleavage. This example provides a synthetic precedent for how O-O bond cleavage of high-spin Fe(III)-peroxo intermediates of non-heme iron enzymes may be promoted.
doi_str_mv 10.1021/ja111742z
format Article
fullrecord <record><control><sourceid>proquest_pubme</sourceid><recordid>TN_cdi_proquest_miscellaneous_874017337</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>874017337</sourcerecordid><originalsourceid>FETCH-LOGICAL-p125t-e6b3680b3673f63188c2f4cbf9f5aa2ec7c1ea05d73669664d2d6060e8829a2d3</originalsourceid><addsrcrecordid>eNo1kE1OwzAQRi0kREthwQWQd9BFwGMnTrJEFaWRKmUDbCM3mRBXiZPGTgU9BRsuyEkIf5uZxbzvSfMRcgHsBhiH260CgNDnhyMyhYAzLwAuJ-TU2i1jzOcRnJAJhwBCFsOUHBaV6lXusNcH5XRraFtSRSv9Unm204aa1ngVNkiXeJ0kydxL0xXVZgw0WGjlkCpTUO0s3Q3KOO1Gyx5p3po99vZb6NoR-Yk_zz8_3tPx1nQ1vp6R41LVFs__9ow8Le8fFytvnT4ki7u11wEPnIdyI2TExhGKUgqIopyXfr4p4zJQimMe5oCKBUUopIyl9AteSCYZRhGPFS_EjFz9eru-3Q1oXdZom2NdK4PtYLMo9BmEQoQjeflHDpvxu6zrdaP6t-y_LvEFzNFqNw</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>874017337</pqid></control><display><type>article</type><title>Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex</title><source>ACS Publications</source><source>MEDLINE</source><creator>Li, Feifei ; Meier, Katlyn K ; Cranswick, Matthew A ; Chakrabarti, Mrinmoy ; Van Heuvelen, Katherine M ; Münck, Eckard ; Que, Lawrence</creator><creatorcontrib>Li, Feifei ; Meier, Katlyn K ; Cranswick, Matthew A ; Chakrabarti, Mrinmoy ; Van Heuvelen, Katherine M ; Münck, Eckard ; Que, Lawrence</creatorcontrib><description>We have generated a high-spin Fe(III)-OOH complex supported by tetramethylcyclam via protonation of its conjugate base and characterized it in detail using various spectroscopic methods. This Fe(III)-OOH species can be converted quantitatively to an Fe(IV)═O complex via O-O bond cleavage; this is the first example of such a conversion. This conversion is promoted by two factors: the strong Fe(III)-OOH bond, which inhibits Fe-O bond lysis, and the addition of protons, which facilitates O-O bond cleavage. This example provides a synthetic precedent for how O-O bond cleavage of high-spin Fe(III)-peroxo intermediates of non-heme iron enzymes may be promoted.</description><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/ja111742z</identifier><identifier>PMID: 21517091</identifier><language>eng</language><publisher>United States</publisher><subject>Heme - chemistry ; Iron - chemistry ; Molecular Structure ; Organometallic Compounds ; Oxygen - chemistry</subject><ispartof>Journal of the American Chemical Society, 2011-05, Vol.133 (19), p.7256-7259</ispartof><rights>2011 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/21517091$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Li, Feifei</creatorcontrib><creatorcontrib>Meier, Katlyn K</creatorcontrib><creatorcontrib>Cranswick, Matthew A</creatorcontrib><creatorcontrib>Chakrabarti, Mrinmoy</creatorcontrib><creatorcontrib>Van Heuvelen, Katherine M</creatorcontrib><creatorcontrib>Münck, Eckard</creatorcontrib><creatorcontrib>Que, Lawrence</creatorcontrib><title>Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex</title><title>Journal of the American Chemical Society</title><addtitle>J Am Chem Soc</addtitle><description>We have generated a high-spin Fe(III)-OOH complex supported by tetramethylcyclam via protonation of its conjugate base and characterized it in detail using various spectroscopic methods. This Fe(III)-OOH species can be converted quantitatively to an Fe(IV)═O complex via O-O bond cleavage; this is the first example of such a conversion. This conversion is promoted by two factors: the strong Fe(III)-OOH bond, which inhibits Fe-O bond lysis, and the addition of protons, which facilitates O-O bond cleavage. This example provides a synthetic precedent for how O-O bond cleavage of high-spin Fe(III)-peroxo intermediates of non-heme iron enzymes may be promoted.</description><subject>Heme - chemistry</subject><subject>Iron - chemistry</subject><subject>Molecular Structure</subject><subject>Organometallic Compounds</subject><subject>Oxygen - chemistry</subject><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2011</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNo1kE1OwzAQRi0kREthwQWQd9BFwGMnTrJEFaWRKmUDbCM3mRBXiZPGTgU9BRsuyEkIf5uZxbzvSfMRcgHsBhiH260CgNDnhyMyhYAzLwAuJ-TU2i1jzOcRnJAJhwBCFsOUHBaV6lXusNcH5XRraFtSRSv9Unm204aa1ngVNkiXeJ0kydxL0xXVZgw0WGjlkCpTUO0s3Q3KOO1Gyx5p3po99vZb6NoR-Yk_zz8_3tPx1nQ1vp6R41LVFs__9ow8Le8fFytvnT4ki7u11wEPnIdyI2TExhGKUgqIopyXfr4p4zJQimMe5oCKBUUopIyl9AteSCYZRhGPFS_EjFz9eru-3Q1oXdZom2NdK4PtYLMo9BmEQoQjeflHDpvxu6zrdaP6t-y_LvEFzNFqNw</recordid><startdate>20110518</startdate><enddate>20110518</enddate><creator>Li, Feifei</creator><creator>Meier, Katlyn K</creator><creator>Cranswick, Matthew A</creator><creator>Chakrabarti, Mrinmoy</creator><creator>Van Heuvelen, Katherine M</creator><creator>Münck, Eckard</creator><creator>Que, Lawrence</creator><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>7X8</scope></search><sort><creationdate>20110518</creationdate><title>Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex</title><author>Li, Feifei ; Meier, Katlyn K ; Cranswick, Matthew A ; Chakrabarti, Mrinmoy ; Van Heuvelen, Katherine M ; Münck, Eckard ; Que, Lawrence</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p125t-e6b3680b3673f63188c2f4cbf9f5aa2ec7c1ea05d73669664d2d6060e8829a2d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2011</creationdate><topic>Heme - chemistry</topic><topic>Iron - chemistry</topic><topic>Molecular Structure</topic><topic>Organometallic Compounds</topic><topic>Oxygen - chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Feifei</creatorcontrib><creatorcontrib>Meier, Katlyn K</creatorcontrib><creatorcontrib>Cranswick, Matthew A</creatorcontrib><creatorcontrib>Chakrabarti, Mrinmoy</creatorcontrib><creatorcontrib>Van Heuvelen, Katherine M</creatorcontrib><creatorcontrib>Münck, Eckard</creatorcontrib><creatorcontrib>Que, Lawrence</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>MEDLINE - Academic</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Feifei</au><au>Meier, Katlyn K</au><au>Cranswick, Matthew A</au><au>Chakrabarti, Mrinmoy</au><au>Van Heuvelen, Katherine M</au><au>Münck, Eckard</au><au>Que, Lawrence</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J Am Chem Soc</addtitle><date>2011-05-18</date><risdate>2011</risdate><volume>133</volume><issue>19</issue><spage>7256</spage><epage>7259</epage><pages>7256-7259</pages><eissn>1520-5126</eissn><abstract>We have generated a high-spin Fe(III)-OOH complex supported by tetramethylcyclam via protonation of its conjugate base and characterized it in detail using various spectroscopic methods. This Fe(III)-OOH species can be converted quantitatively to an Fe(IV)═O complex via O-O bond cleavage; this is the first example of such a conversion. This conversion is promoted by two factors: the strong Fe(III)-OOH bond, which inhibits Fe-O bond lysis, and the addition of protons, which facilitates O-O bond cleavage. This example provides a synthetic precedent for how O-O bond cleavage of high-spin Fe(III)-peroxo intermediates of non-heme iron enzymes may be promoted.</abstract><cop>United States</cop><pmid>21517091</pmid><doi>10.1021/ja111742z</doi><tpages>4</tpages></addata></record>
fulltext fulltext
identifier EISSN: 1520-5126
ispartof Journal of the American Chemical Society, 2011-05, Vol.133 (19), p.7256-7259
issn 1520-5126
language eng
recordid cdi_proquest_miscellaneous_874017337
source ACS Publications; MEDLINE
subjects Heme - chemistry
Iron - chemistry
Molecular Structure
Organometallic Compounds
Oxygen - chemistry
title Characterization of a high-spin non-heme Fe(III)-OOH intermediate and its quantitative conversion to an Fe(IV)═O complex
url https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-02-03T23%3A50%3A06IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_pubme&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Characterization%20of%20a%20high-spin%20non-heme%20Fe(III)-OOH%20intermediate%20and%20its%20quantitative%20conversion%20to%20an%20Fe(IV)%E2%95%90O%20complex&rft.jtitle=Journal%20of%20the%20American%20Chemical%20Society&rft.au=Li,%20Feifei&rft.date=2011-05-18&rft.volume=133&rft.issue=19&rft.spage=7256&rft.epage=7259&rft.pages=7256-7259&rft.eissn=1520-5126&rft_id=info:doi/10.1021/ja111742z&rft_dat=%3Cproquest_pubme%3E874017337%3C/proquest_pubme%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=874017337&rft_id=info:pmid/21517091&rfr_iscdi=true