Iron-Catalyzed Aerobic Carbonylation of Methane via Ligand-to-Metal Charge Transfer Excitation

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 6, 2025

The integration of ligand-to-metal charge transfer (LMCT) catalytic paradigms with radical intermediates has transformed the selective functionalization inert C-H bonds, facilitating use nonprecious metal catalysts in demanding transformations. Notably, aerobic carbonylation methane to acetic acid remains formidable due rapid oxidation methyl radicals, producing undesired C1 oxygenates. We present an iron terpyridine catalyst utilizing LMCT achieve exceptional C2/C1 selectivity through synergistic photoexcitation, generation, and carbonylation. Mechanistic studies highlight critical roles Fe(II) Fe-carbonyl complexes bypassing via a rebound-like pathway, unlocking unprecedented efficiency

Язык: Английский

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Circulating microdroplet-driven self-Fenton for micropollutant elimination: the overlook of ligand-to-metal charge transfer and chloride radical

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125214 - 125214

Опубликована: Фев. 1, 2025

Язык: Английский

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Visible-light induced direct C(sp³)–H functionalization: recent advances and future prospects

Organic Chemistry Frontiers, Год журнала: 2024, Номер 11(18), С. 5278 - 5305

Опубликована: Янв. 1, 2024

This review summarizes the latest methodological advances in photocatalytic C(sp 3 )–H functionalization, with a particular emphasis on formation of C–P, C–B, C–S bonds, etc ., and some prominent efforts asymmetric C–H functionalization.

Язык: Английский

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Unified approaches in transition metal catalyzed C(sp³)–H functionalization: recent advances and mechanistic aspects

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Direct alteration of unactivated C–H bonds organic building blocks.

Язык: Английский

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Iron-Catalyzed Ipso-Nitration of Aryl Borides via Visible-Light-Induced β-Homolysis

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3306 - 3313

Опубликована: Фев. 7, 2025

Herein, we reported a practical method to realize ipso-nitration of boronic acids, their pinacol esters, and trifluoroborate salts with alkali metal salt NaNO3 as nitrating reagent. A FeIII/FeIV catalytic cycle involving an unusual visible-light-induced β-homolysis pathway the N–O bond in simple iron complex effectively provides nitryl radical key species. This protocol bears mild reaction conditions, broad scope (up 99% yield), good functional group compatibility, convenient scale-up synthesis.

Язык: Английский

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Ir-Catalyzed, Nitrogen-Directed C(sp³)–H and C(sp²)–H Borylation with a Spiro-Fluorene-Indenoindenyl Ligand

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 4061 - 4068

Опубликована: Фев. 21, 2025

Язык: Английский

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Selective Arene Photonitration via Iron-Complex β-Homolysis

JACS Au, Год журнала: 2024, Номер 4(12), С. 4899 - 4909

Опубликована: Ноя. 21, 2024

Nitroaromatics, as an important member and source of nitrogen-containing aromatics, is bringing enormous economic benefits in fields pharmaceuticals, dyes, pesticides, functional materials, fertilizers, explosives. Nonetheless, the notoriously polluting nitration industry, which suffers from excessive discharge fumes waste acids, poor group tolerance, tremendous purification difficulty, renders mild, efficient, environmentally friendly a formidable challenge. Herein, we develop visible-light-driven biocompatible arene C–H strategy with good efficiency regioselectivity, marvelous substrate applicability wide application scale-up synthesis, total late-stage functionalization. A nitryl radical delivered through unusual β-homolysis photoexcited ferric-nitrate complex proposed to be key nitrification reagent this system.

Язык: Английский

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Visible-light-mediated synthesis of polysubstituted pyrroles via C_Ar–I reduction triggered 1,5-hydrogen atom transfer process

Organic Chemistry Frontiers, Год журнала: 2024, Номер 11(16), С. 4522 - 4528

Опубликована: Янв. 1, 2024

A novel strategy for the construction of polysubstituted pyrroles has been developed through visible-light-induced single-electron reduction C Ar –I bonds and following 1,5-hydrogen atom transfer (HAT) process.

Язык: Английский

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Bifunctional iron-catalyzed alkyne Z-selective hydroalkylation and tandem Z-E inversion via radical molding and flipping

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 4, 2024

The challenging synthesis of thermodynamic-unfavored cis-olefins through catalytic cross-coupling reactions requires the synergistic interaction substrate-activating units and configuration-regulating catalysts. Successfully hitting these two birds with one stone, we herein develop a convenient photoredox access to Z-alkenes from alkynes light alkanes bifunctional iron-catalyzed system possessing both C(sp

Язык: Английский

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Photochemical C–H Borylation in Organic Synthesis

ACS Catalysis, Год журнала: 2025, Номер 15(3), С. 1753 - 1770

Опубликована: Янв. 16, 2025

Although C–H bond functionalization has been extensively studied since its discovery in 1955, the borylation of organic compounds by activating bonds only became popular valuable Hartwig 1995 who considered a wider application these transformations synthetic chemistry. For borylation, catalytic activation this generally low-reactivity can be performed many ways. Among approaches reported are use and stoichiometric reagents, thermal activation, photochemical suitable substrates. Iridium-, ruthenium-, rhodium-based protocols using have played crucial role toward establishment area. Photochemical though, scarcely explored despite fact that it represents comparably environmentally benign protocol light as renewable energy source. In literature survey, we highlight recent developments from initial inception up to latest advancements.

Язык: Английский

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