Modular Synthesis of Dehydroprolines by an Energy‐Transfer Enabled Cloke‐Wilson Rearrangement DOI
Austin D. Marchese, Tomislav Rovis

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Дек. 4, 2024

Abstract A one‐pot photocatalytic method is reported for the generation of dehydroprolines, valuable precursors to 5‐aryl prolines. Imines, obtained via simple condensation aminocyclopropane carboxylates (ACPC) with a broad range aldehydes, were employed in this transformation without purification. We demonstrate energy‐transfer (EnT) enabled Cloke‐Wilson‐type rearrangement affords both rare 1,2‐dehydroprolines or more thermodynamically favored 1,5‐isomers up >20 : 1 selectivity directions, using an identical catalytic system from same starting material. Syntheses intermediates bioactive molecules high yields and highlight enabling transformation. Mechanistic studies support proposed triplet‐triplet EnT mode activation, distinct previously developed singlet excited states accessed UV excitation.

Язык: Английский

Low-energy photoredox catalysis DOI
David C. Cabanero, Tomislav Rovis

Nature Reviews Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 11, 2024

Язык: Английский

Процитировано

10

Radical-polar Crossover Reaction of Glycine Derivatives DOI

Youwan Ye,

Xin Zhang,

Peng Kong

и другие.

Chemical Communications, Год журнала: 2024, Номер 60(75), С. 10378 - 10381

Опубликована: Янв. 1, 2024

Here we report a visible-light facilitated radical addition strategy for the preparation of various natural or unnatural α-amino acids from readily available glycine derivatives and alkenes. A key aspect in achieving this side carbon chain introduction reaction, while circumventing well-documented cyclization pathway, was employment radical-polar crossover under redox neutral conditions.

Язык: Английский

Процитировано

5

Radical approaches for C(sp3)–N bond cleavage in deaminative transformations DOI
J. Kim,

Eun Song Lim,

Ji Yeon Park

и другие.

Chemical Communications, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review summarizes recent advancements in radical-mediated deaminative transformations, focusing on the mechanisms, substrate compatibility, and emerging applications synthetic organic chemistry.

Язык: Английский

Процитировано

0

Photoredox Catalysis DOI
Geraint H. M. Davies, Patricia Z. Musacchio, Trevor C. Sherwood

и другие.

Elsevier eBooks, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

0

Visible-Light-Mediated Nucleophilic Addition of Alkene with Aldehyde: Synthesis of Secondary Alcohols DOI

D. Hu,

Huu Phuong Dang,

Zhen Liang

и другие.

Organic Letters, Год журнала: 2024, Номер unknown

Опубликована: Дек. 10, 2024

Herein, a photocatalytic strategy for the synthesis of secondary alcohols by nucleophilic addition an alkene with aldehyde is described. This operationally simple methodology opens approach using commercially available reagents in moderate to excellent yields. Mechanistic studies indicate that formation radical anion from via single-electron transfer key step this reaction.

Язык: Английский

Процитировано

2

(2 + 2 + 1)-Cyclization of Glycine Derivatives with Alkenes and CO2 DOI

Youwan Ye,

Congde Huo

Organic Letters, Год журнала: 2024, Номер 26(37), С. 7897 - 7901

Опубликована: Сен. 5, 2024

A highly atom-economic (2 + 2 1)-cyclization of glycine derivatives with alkenes and CO

Язык: Английский

Процитировано

1

Modular Synthesis of Dehydroprolines by an Energy‐Transfer Enabled Cloke‐Wilson Rearrangement DOI
Austin D. Marchese, Tomislav Rovis

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Дек. 4, 2024

Abstract A one‐pot photocatalytic method is reported for the generation of dehydroprolines, valuable precursors to 5‐aryl prolines. Imines, obtained via simple condensation aminocyclopropane carboxylates (ACPC) with a broad range aldehydes, were employed in this transformation without purification. We demonstrate energy‐transfer (EnT) enabled Cloke‐Wilson‐type rearrangement affords both rare 1,2‐dehydroprolines or more thermodynamically favored 1,5‐isomers up >20 : 1 selectivity directions, using an identical catalytic system from same starting material. Syntheses intermediates bioactive molecules high yields and highlight enabling transformation. Mechanistic studies support proposed triplet‐triplet EnT mode activation, distinct previously developed singlet excited states accessed UV excitation.

Язык: Английский

Процитировано

1

Photomediated Deaminative Generation of Tertiary Anions DOI
Dirk Trauner, Andreas Hess

Synfacts, Год журнала: 2024, Номер 20(03), С. 0322 - 0322

Опубликована: Фев. 14, 2024

Key words photocatalysis - carbanions cross-coupling

Язык: Английский

Процитировано

0

Reductive deaminative cross-coupling of alkyl bistriflimides enabled by electrocatalysis DOI Creative Commons
Xiangzhang Tao, Wooseok Lee,

Zhimin Xu

и другие.

Science Advances, Год журнала: 2024, Номер 10(47)

Опубликована: Ноя. 22, 2024

We present a versatile nickel-electrocatalytic deaminative cross-coupling platform for the efficient construction of C(sp 3 )–C(sp ) and 2 bonds from readily available alkyl bistriflimides. This methodology involves assembly two leaving groups on amines to form bistriflimides, followed by their effective coupling with wide range halides, pseudohalides, aryl alkenyl halides under electrochemical reductive conditions. Moreover, successful application relay transition metal–free cross-electrophile further demonstrates versatility bistriflimides as valuable building blocks in organic synthesis. Combined control experiments density functional theory calculations provide insights into reaction pathway crucial role iodide catalytic process.

Язык: Английский

Процитировано

0

Modular Synthesis of Dehydroprolines by an Energy‐Transfer Enabled Cloke‐Wilson Rearrangement DOI
Austin D. Marchese, Tomislav Rovis

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Дек. 4, 2024

Abstract A one‐pot photocatalytic method is reported for the generation of dehydroprolines, valuable precursors to 5‐aryl prolines. Imines, obtained via simple condensation aminocyclopropane carboxylates (ACPC) with a broad range aldehydes, were employed in this transformation without purification. We demonstrate energy‐transfer (EnT) enabled Cloke‐Wilson‐type rearrangement affords both rare 1,2‐dehydroprolines or more thermodynamically favored 1,5‐isomers up >20 : 1 selectivity directions, using an identical catalytic system from same starting material. Syntheses intermediates bioactive molecules high yields and highlight enabling transformation. Mechanistic studies support proposed triplet‐triplet EnT mode activation, distinct previously developed singlet excited states accessed UV excitation.

Язык: Английский

Процитировано

0