Literature DB >> 27685680

A One-Hole Cu4S Cluster with N2O Reductase Activity: A Structural and Functional Model for CuZ.

Brittany J Johnson1, William E Antholine2, Sergey V Lindeman3, Michael J Graham4, Neal P Mankad1.   

Abstract

During bacterial denitrification, two-electron reduction of N2O occurs at a [Cu4(μ4-S)] catalytic site (CuZ*) embedded within the nitrous oxide reductase (N2OR) enzyme. In this Communication, an amidinate-supported [Cu4(μ4-S)] model cluster in its one-hole (S = 1/2) redox state is thoroughly characterized. Along with its two-hole redox partner and fully reduced clusters reported previously, the new species completes the two-electron redox series of [Cu4(μ4-S)] model complexes with catalytically relevant oxidation states for the first time. More importantly, N2O is reduced by the one-hole cluster to produce N2 and the two-hole cluster, thereby completing a closed cycle for N2O reduction. Not only is the title complex thus the best structural model for CuZ* to date, but it also serves as a functional CuZ* mimic.

Entities:  

Year:  2016        PMID: 27685680      PMCID: PMC5378702          DOI: 10.1021/jacs.6b05480

Source DB:  PubMed          Journal:  J Am Chem Soc        ISSN: 0002-7863            Impact factor:   15.419


  19 in total

1.  A novel type of catalytic copper cluster in nitrous oxide reductase.

Authors:  K Brown; M Tegoni; M Prudêncio; A S Pereira; S Besson; J J Moura; I Moura; C Cambillau
Journal:  Nat Struct Biol       Date:  2000-03

2.  Activation of N2O reduction by the fully reduced micro4-sulfide bridged tetranuclear Cu Z cluster in nitrous oxide reductase.

Authors:  Somdatta Ghosh; Serge I Gorelsky; Peng Chen; Inês Cabrito; José J G Moura; Isabel Moura; Edward I Solomon
Journal:  J Am Chem Soc       Date:  2003-12-24       Impact factor: 15.419

3.  Mechanism of N2O reduction by the mu4-S tetranuclear CuZ cluster of nitrous oxide reductase.

Authors:  Serge I Gorelsky; Somdatta Ghosh; Edward I Solomon
Journal:  J Am Chem Soc       Date:  2006-01-11       Impact factor: 15.419

4.  [Cu3(mu-S)2]3+ clusters supported by N-donor ligands: progress toward a synthetic model of the catalytic site of nitrous oxide reductase.

Authors:  Eric C Brown; John T York; William E Antholine; Eliseo Ruiz; Santiago Alvarez; William B Tolman
Journal:  J Am Chem Soc       Date:  2005-10-12       Impact factor: 15.419

Review 5.  Copper active sites in biology.

Authors:  Edward I Solomon; David E Heppner; Esther M Johnston; Jake W Ginsbach; Jordi Cirera; Munzarin Qayyum; Matthew T Kieber-Emmons; Christian H Kjaergaard; Ryan G Hadt; Li Tian
Journal:  Chem Rev       Date:  2014-03-03       Impact factor: 60.622

Review 6.  Biological sources and sinks of nitrous oxide and strategies to mitigate emissions.

Authors:  Andrew J Thomson; Georgios Giannopoulos; Jules Pretty; Elizabeth M Baggs; David J Richardson
Journal:  Philos Trans R Soc Lond B Biol Sci       Date:  2012-05-05       Impact factor: 6.237

7.  Structural variation in copper(I) complexes with pyridylmethylamide ligands: structural analysis with a new four-coordinate geometry index, tau4.

Authors:  Lei Yang; Douglas R Powell; Robert P Houser
Journal:  Dalton Trans       Date:  2007-01-29       Impact factor: 4.390

8.  Determination of the active form of the tetranuclear copper sulfur cluster in nitrous oxide reductase.

Authors:  Esther M Johnston; Simone Dell'Acqua; Susana Ramos; Sofia R Pauleta; Isabel Moura; Edward I Solomon
Journal:  J Am Chem Soc       Date:  2014-01-07       Impact factor: 15.419

9.  Reduction of nitrous oxide to dinitrogen by a mixed valent tricopper-disulfido cluster.

Authors:  Itsik Bar-Nahum; Aalo K Gupta; Stefan M Huber; Mehmed Z Ertem; Christopher J Cramer; William B Tolman
Journal:  J Am Chem Soc       Date:  2009-03-04       Impact factor: 15.419

10.  Spectroscopic and electronic structure studies of the mu(4)-sulfide bridged tetranuclear Cu(Z) cluster in N(2)O reductase: molecular insight into the catalytic mechanism.

Authors:  Peng Chen; Inês Cabrito; José J G Moura; Isabel Moura; Edward I Solomon
Journal:  J Am Chem Soc       Date:  2002-09-04       Impact factor: 15.419

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  5 in total

Review 1.  Biological and Bioinspired Inorganic N-N Bond-Forming Reactions.

Authors:  Christina Ferousi; Sean H Majer; Ida M DiMucci; Kyle M Lancaster
Journal:  Chem Rev       Date:  2020-02-28       Impact factor: 60.622

2.  N2 O Reductase Activity of a [Cu4 S] Cluster in the 4CuI Redox State Modulated by Hydrogen Bond Donors and Proton Relays in the Secondary Coordination Sphere.

Authors:  Chia-Wei Hsu; Suresh C Rathnayaka; Shahidul M Islam; Samantha N MacMillan; Neal P Mankad
Journal:  Angew Chem Int Ed Engl       Date:  2019-11-14       Impact factor: 15.336

3.  Sulfur-Containing Analogues of the Reactive [CuOH]2+ Core.

Authors:  Wen Wu; Jacqui Tehranchi De Hont; Riffat Parveen; Bess Vlaisavljevich; William B Tolman
Journal:  Inorg Chem       Date:  2021-03-18       Impact factor: 5.165

4.  Probing the electronic and mechanistic roles of the μ4-sulfur atom in a synthetic CuZ model system.

Authors:  Suresh C Rathnayaka; Shahidul M Islam; Ida M DiMucci; Samantha N MacMillan; Kyle M Lancaster; Neal P Mankad
Journal:  Chem Sci       Date:  2020-02-17       Impact factor: 9.825

5.  Coordination chemistry of the CuZ site in nitrous oxide reductase and its synthetic mimics.

Authors:  Suresh C Rathnayaka; Neal P Mankad
Journal:  Coord Chem Rev       Date:  2020-12-19       Impact factor: 22.315

  5 in total

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