Synthesis, Characterization, and Reactivity of a Hypervalent‐Iodine‐Based Nitrooxylating Reagent


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Date

2020-09-21

Publication Type

Journal Article

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yes

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Abstract

Herein, the synthesis and characterization of a hypervalent‐iodine‐based reagent that enables a direct and selective nitrooxylation of enolizable C−H bonds to access a broad array of organic nitrate esters is reported. This compound is bench stable, easy‐to‐handle, and delivers the nitrooxy (‐ONO2) group under mild reaction conditions. Activation of the reagent by Brønsted and Lewis acids was demonstrated in the synthesis of nitrooxylated β‐keto esters, 1,3‐diketones, and malonates, while its activity under photoredox catalysis was shown in the synthesis of nitrooxylated oxindoles. Detailed mechanistic studies including pulse radiolysis, Stern–Volmer quenching studies, and UV/Vis spectroelectrochemistry reveal a unique single‐electron‐transfer (SET)‐induced concerted mechanistic pathway not reliant upon generation of the nitrate radical.

Publication status

published

Editor

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Volume

59 (39)

Pages / Article No.

17162 - 17168

Publisher

Wiley-VCH

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Edition / version

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Subject

hypervalent iodine compounds; nitrate esters; photoredox catalysis; pulse radiolysis; spectroelectrochemistry

Organisational unit

03512 - Günther, Detlef / Günther, Detlef check_circle

Notes

Funding

168043 - Development of Novel Iron-Catalyzed Oxidative Transformations of Inert C(sp3)-H Bonds (SNF)
169134 - Molecular Approach to Heterogeneous Catalysis (SNF)
192050 - Molecular Approach and Understanding in Heterogeneous Catalysis (SNF)

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