Coumarin C-H Functionalization by Mn(I) Carbonyls: Mechanistic Insight by Ultra-Fast IR Spectroscopic Analysis.

coumarin cyclomanganation infrared spectroscopy manganese organomanganese

Journal

Chemistry (Weinheim an der Bergstrasse, Germany)
ISSN: 1521-3765
Titre abrégé: Chemistry
Pays: Germany
ID NLM: 9513783

Informations de publication

Date de publication:
02 May 2023
Historique:
received: 29 09 2022
medline: 11 1 2023
pubmed: 11 1 2023
entrez: 10 1 2023
Statut: ppublish

Résumé

Mn(I) C-H functionalization of coumarins provides a versatile and practical method for the rapid assembly of fused polycyclic pyridinium-containing coumarins in a regioselective manner. The synthetic strategy enables application of bench-stable organomanganese reagents in both photochemical- and thermal-promoted reactions. The cyclomanganated intermediates, and global reaction system, provide an ideal testing ground for structural characterization of the active Mn(I) carbonyl-containing species, including transient species observable by ultra-fast time-resolved spectroscopic methods. The thermodynamic reductive elimination product, solely encountered from reaction between alkynes and air-stable organometallic cyclomanganated coumarins, has enabled characterization of a critical seven-membered Mn(I) intermediate, detected by time-resolved infrared spectroscopy, enabling the elucidation of the temporal profile of key steps in the reductive elimination pathway. Quantitative data are provided. Manganated polycyclic products are readily decomplexed by AgBF

Identifiants

pubmed: 36625067
doi: 10.1002/chem.202203038
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e202203038

Subventions

Organisme : Engineering and Physical Sciences Research Council
ID : EP/ N509413/1
Organisme : Central Laser Facility, Science and Technology Facilities Council
ID : Non-applicable
Organisme : Syngenta International
ID : Non-applicable

Informations de copyright

© 2023 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.

Références

Nat Chem. 2015 Dec;7(12):987-94
pubmed: 26587714
Angew Chem Int Ed Engl. 2015 Nov 16;54(47):14137-40
pubmed: 26418747
J Am Chem Soc. 2019 Feb 13;141(6):2316-2328
pubmed: 30698423
Chem Rev. 2022 Jun 8;122(11):10126-10169
pubmed: 34402611
Angew Chem Int Ed Engl. 2018 Apr 9;57(16):4234-4241
pubmed: 29228463
Angew Chem Int Ed Engl. 2020 Apr 6;59(15):6239-6243
pubmed: 31917507
Inorg Chem. 2011 Jun 6;50(11):4798-810
pubmed: 21517013
J Am Chem Soc. 2021 Jan 27;143(3):1356-1364
pubmed: 33428402
Acc Chem Res. 2018 Mar 20;51(3):816-827
pubmed: 29443496
J Org Chem. 2020 Aug 7;85(15):9514-9524
pubmed: 32515197
Angew Chem Int Ed Engl. 2018 Jan 22;57(4):923-928
pubmed: 29205747
Angew Chem Int Ed Engl. 2016 Sep 26;55(40):12455-9
pubmed: 27603008
Chem Sci. 2022 Jul 8;13(34):9902-9913
pubmed: 36199635
Chemistry. 2023 May 2;29(25):e202203038
pubmed: 36625067
Chem Commun (Camb). 2012 Oct 7;48(77):9613-5
pubmed: 22908116
Mini Rev Med Chem. 2018;18(2):113-141
pubmed: 27488585
Angew Chem Int Ed Engl. 2017 Mar 13;56(12):3172-3176
pubmed: 28181732
ACS Cent Sci. 2016 May 25;2(5):281-92
pubmed: 27294201
J Am Chem Soc. 2013 Jan 30;135(4):1264-7
pubmed: 23286776
Chem Asian J. 2018 Jul 4;13(13):1664-1668
pubmed: 29676048
Appl Spectrosc. 2016 Apr;70(4):645-53
pubmed: 26887988
Dalton Trans. 2019 Nov 21;48(43):16426-16436
pubmed: 31650147
Bioorg Chem. 2018 Apr;77:311-319
pubmed: 29421707
Chemistry. 2021 Feb 24;27(12):3979-3985
pubmed: 33135818

Auteurs

Thomas J Burden (TJ)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Kathryn P R Fernandez (KPR)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Mary Kagoro (M)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Jonathan B Eastwood (JB)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Theo F N Tanner (TFN)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Adrian C Whitwood (AC)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Ian P Clark (IP)

Central Laser Facility, Research Complex at Harwell STFC Rutherford Appleton Laboratory Harwell Campus Didcot, Oxfordshire, OX11 0QX, UK.

Michael Towrie (M)

Central Laser Facility, Research Complex at Harwell STFC Rutherford Appleton Laboratory Harwell Campus Didcot, Oxfordshire, OX11 0QX, UK.

Jean-Philippe Krieger (JP)

Syngenta Crop Protection AG, Breitenloh 5, 4333, Münchwilen, Switzerland.

Jason M Lynam (JM)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Ian J S Fairlamb (IJS)

Department of Chemistry, University of York Heslington, York, YO10 5DD, UK.

Classifications MeSH