Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates

An efficient Ni-catalyzed, Mn-mediated denitrogenative cross-electrophile coupling of <i>N</i>-alkyl-1,2,3-benzotriazinones with alkyl tosylates and mesylates for access to <i>o</i>-alkyl secondary benzamides is reported. The method uses inexpensive non-anhydrous dimethyl ace...

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Main Authors: Yingying Hong, Xuanxuan Zhang, Gang Zou
Format: Article
Language:English
Published: MDPI AG 2025-05-01
Series:Molecules
Subjects:
Online Access:https://www.mdpi.com/1420-3049/30/11/2397
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author Yingying Hong
Xuanxuan Zhang
Gang Zou
author_facet Yingying Hong
Xuanxuan Zhang
Gang Zou
author_sort Yingying Hong
collection DOAJ
description An efficient Ni-catalyzed, Mn-mediated denitrogenative cross-electrophile coupling of <i>N</i>-alkyl-1,2,3-benzotriazinones with alkyl tosylates and mesylates for access to <i>o</i>-alkyl secondary benzamides is reported. The method uses inexpensive non-anhydrous dimethyl acetamide (DMA) in combination with tetrabutyl ammonium iodide (TBAI) as a co-catalyst to convert sulfonates into iodides in situ. Scope and limitations of the protocol have been demonstrated by >30 examples with yields up to 91%, showing a large electronic effect from the <i>N</i>-substituent in benzotriazinones. An unexpected steric acceleration has been observed from the core of benzotriazinones, not only promising a highly efficient access to 2-alkyl-2,3-disubstituted benzamides but also shedding light on the rate-limiting steps in the catalytic cycle.
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institution Kabale University
issn 1420-3049
language English
publishDate 2025-05-01
publisher MDPI AG
record_format Article
series Molecules
spelling doaj-art-a36f79d55fef4f3588f786a1fd2018802025-08-20T03:46:50ZengMDPI AGMolecules1420-30492025-05-013011239710.3390/molecules30112397Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl SulfonatesYingying Hong0Xuanxuan Zhang1Gang Zou2School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Rd, Shanghai 200237, ChinaSchool of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Rd, Shanghai 200237, ChinaSchool of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Rd, Shanghai 200237, ChinaAn efficient Ni-catalyzed, Mn-mediated denitrogenative cross-electrophile coupling of <i>N</i>-alkyl-1,2,3-benzotriazinones with alkyl tosylates and mesylates for access to <i>o</i>-alkyl secondary benzamides is reported. The method uses inexpensive non-anhydrous dimethyl acetamide (DMA) in combination with tetrabutyl ammonium iodide (TBAI) as a co-catalyst to convert sulfonates into iodides in situ. Scope and limitations of the protocol have been demonstrated by >30 examples with yields up to 91%, showing a large electronic effect from the <i>N</i>-substituent in benzotriazinones. An unexpected steric acceleration has been observed from the core of benzotriazinones, not only promising a highly efficient access to 2-alkyl-2,3-disubstituted benzamides but also shedding light on the rate-limiting steps in the catalytic cycle.https://www.mdpi.com/1420-3049/30/11/2397cross-electrophile couplingnickel catalysisbenzotriazinonealkyl sulfonate
spellingShingle Yingying Hong
Xuanxuan Zhang
Gang Zou
Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
Molecules
cross-electrophile coupling
nickel catalysis
benzotriazinone
alkyl sulfonate
title Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
title_full Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
title_fullStr Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
title_full_unstemmed Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
title_short Iodide/Nickel Co-Catalyzed Manganese-Mediated Denitrogenative Cross-Electrophile Coupling of Benzotriazinones with Alkyl Sulfonates
title_sort iodide nickel co catalyzed manganese mediated denitrogenative cross electrophile coupling of benzotriazinones with alkyl sulfonates
topic cross-electrophile coupling
nickel catalysis
benzotriazinone
alkyl sulfonate
url https://www.mdpi.com/1420-3049/30/11/2397
work_keys_str_mv AT yingyinghong iodidenickelcocatalyzedmanganesemediateddenitrogenativecrosselectrophilecouplingofbenzotriazinoneswithalkylsulfonates
AT xuanxuanzhang iodidenickelcocatalyzedmanganesemediateddenitrogenativecrosselectrophilecouplingofbenzotriazinoneswithalkylsulfonates
AT gangzou iodidenickelcocatalyzedmanganesemediateddenitrogenativecrosselectrophilecouplingofbenzotriazinoneswithalkylsulfonates