Chemistry - A European Journal, Год журнала: 2024, Номер 30(66)
Опубликована: Авг. 22, 2024
Encapsulation of transition metals represents a crucial method for modifying the electronic structure and regulating reactivity fullerene, thereby expanding its applications. Herein, we present calculations with density functional theory methods to investigate mechanisms Diels-Alder (DA) reactions cyclopentadiene La@C
Язык: Английский
ACS Catalysis, Год журнала: 2024, Номер 14(9), С. 6973 - 6980
Опубликована: Апрель 19, 2024
Development of photocatalytic systems that facilitate mechanistically divergent steps in complex catalytic manifolds by distinct activation modes can enable previously inaccessible synthetic transformations. However, multimodal remain understudied, impeding their implementation methodology. We report herein a access to thiols directly merges the structural diversity carboxylic acids with ready availability elemental sulfur without substrate preactivation. The transformation provides direct radical-mediated segue one most biologically important and synthetically versatile organosulfur functionalities, whose accessibility remains largely dominated two-electron-mediated processes based on toxic uneconomical reagents precursors. two-phase radical process is facilitated reactivity acridine photocatalysis enables both singlet excited state PCET-mediated decarboxylative carbon–sulfur bond formation unknown reductive disulfur cleavage photoinduced hydrogen atom transfer silane–triplet system. study points significant potential providing unexplored directions
Язык: Английский
Процитировано
11
Journal of the American Chemical Society, Год журнала: 2025, Номер 147(6), С. 4736 - 4742
Опубликована: Янв. 31, 2025
The preparation of alcohols with anti-Markovnikov selectivity directly from olefins and water is a sought-after reaction due to its atom-economy potential cost-effectiveness. Herein, we present the first general method for direct, catalytic hydration unconjugated tri- disubstituted olefins. key advancement made possible by an oxidative (E*red = 2.15 V) N-H acridinium catalyst, which allowed functionalization alkenes that were previously unreactive in such transformations their high oxidation potential. developed protocol not limited but also enables other hydrofunctionalizations, as hydroetherifications, following same mechanistic pathway.
Язык: Английский
Процитировано
1
Chemical Science, Год журнала: 2025, Номер unknown
Опубликована: Янв. 1, 2025
An applicable cobalt-hydride-mediated selective, divergent hydroetherification and sequential hydroetherification/hydroarylation of 1,3-dienes with simple phenol feedstocks under a photoredox cobalt catalytic system have been developed. A variety allyl aryl ethers value-added chroman derivatives can be obtained in good to excellent yields stereoselectivity. This method not only obviates the need for extra hydrosilanes stoichiometric oxidants, thereby offering exceedingly mild conditions alkene hydroetherification, but also represents first case CoH-HAT-catalyzed double hydrofunctionalization alkenes sole nucleophile. The continuous selective bond-forming expands applications cobalt-hydride MHAT reaction provides novel approach design synthesis heterocyclic molecules.
Язык: Английский
Процитировано
1
Journal of the American Chemical Society, Год журнала: 2024, Номер unknown
Опубликована: Сен. 12, 2024
Alkyl radicals generated via an acridine photocatalyzed decarboxylation reaction of feedstock carboxylic acids engage with a range cyclic imine-BF
Язык: Английский
Процитировано
5
Chemistry - A European Journal, Год журнала: 2024, Номер 30(58)
Опубликована: Авг. 8, 2024
Abstract Mild and inexpensive copper‐catalyzed aromatization‐driven ring‐opening amination oxygenation of spiro dihydroquinazolinones are presented, respectively. These protocols provide facile atom‐economical access to the aminated carbonyl‐containing quinazolin‐4(3 H )‐ones in good yields with functional group compatibility, which difficult obtain by conventional methods. Remarkably, a telescoped procedure involving condensation ring‐opening/functionalization for simple cycloalkanone was found be accessible. Mechanistic studies suggest radical pathway this transformation.
Язык: Английский
Процитировано
3
Organic Letters, Год журнала: 2025, Номер unknown
Опубликована: Фев. 14, 2025
Herein, we report a visible-light-driven and cobalt-mediated 1,4-hydroamination reaction of 1,3-dienes with arylmines as the nucleophiles. The involves regioselective addition [CoIII]–H to 1,3-diene, followed by oxidation nucleophilic substitution amines. Using Ir(ppy)3 photocatalyst enables cobalt redox cycle be implemented without using an external oxidant hydride regent. This protocol can applied well forge carbon–oxygen carbon–sulfur bonds in analogous way.
Язык: Английский
Процитировано
0
Chem Catalysis, Год журнала: 2025, Номер unknown, С. 101414 - 101414
Опубликована: Май 1, 2025
Язык: Английский
Процитировано
0
Опубликована: Фев. 29, 2024
Development of photocatalytic systems that facilitate mechanistically different steps in complex catalytic manifolds by distinct activation modes can enable previously inaccessible synthetic transformations. However, multimodal remain understudied, impeding their implementation methodology. We report herein a access to thiols directly merges the structural diversity carboxylic acids with ready availability elemental sulfur without substrate preactivation. The transformation provides direct radical-mediated segue one most biologically important and synthetically versatile organosulfur functionalities, whose accessibility remains largely dominated two-electron-mediated processes based on toxic uneconomical reagents precursors. two-phase radical process is facilitated reactivity acridine photocatalysis enables both singlet excited state PCET-mediated decarboxylative carbon–sulfur bond formation unknown reductive disulfur cleavage photoinduced HAT silane–triplet system. study points significant potential providing new directions
Язык: Английский
Процитировано
2
Mendeleev Communications, Год журнала: 2024, Номер 34(5), С. 673 - 675
Опубликована: Сен. 1, 2024
Язык: Английский
Процитировано
2
Chemical Research in Chinese Universities, Год журнала: 2024, Номер unknown
Опубликована: Авг. 29, 2024
Язык: Английский
Процитировано
1