Revealing Dinitrogen Activation via Mesoionic Carbenes: A Computational Design with Frustrated Lewis Pairs DOI
Shiqing Huang, Tian Wang, Zengyu Zhang

и другие.

Asian Journal of Organic Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 13, 2024

Abstract Activating dinitrogen under metal‐free conditions remains a significant challenge in chemistry. In this study, we computationally designed frustrated Lewis pair (FLP) system incorporating bis(trimethylsilyl)boryl substituent on mesoionic carbene (MIC) framework. Our models show both kinetic and thermodynamic favorability for activation. Aromaticity enhancement along the potential energy surface (PES) plays critical role driving reaction. This work provides insights into utilizing main‐group elements activation offers applications inert molecule optical materials.

Язык: Английский

Benzothiazolines Acting as Carbanion and Radical Transfer Reagents in Carbon–Carbon Bond Construction DOI Creative Commons
Xiaotang Chen,

Bao‐Chen Qian

Molecules, Год журнала: 2025, Номер 30(8), С. 1711 - 1711

Опубликована: Апрель 11, 2025

Traditionally employed as hydrogenation reagents, benzothiazolines have emerged versatile carbanion and radical transfer playing a vital role in the construction of various carbon-carbon bonds. The cutting-edge progress photochemistry chemistry prompted study visible light-driven reactions, bringing into vibrant focus. Their chemical processes been uncovered to encompass variety activation mechanisms, with five distinct modes having identified. This work reviews innovative applications donors alkyl or acyl groups, achieving hydroalkylation hydroacylation substitution. By examining their diverse this review highlights potential serving groups for further research development. Moreover, will offer exemplary inspiration synthetic chemists, contributing ongoing evolution utility organic synthesis.

Язык: Английский

Процитировано

0

Switching Mesoionic Carbene-Organocatalysis from Radical to Ionic Pathway through Base-Controlled Formation of Breslow Intermediates versus Breslow Enolates DOI Creative Commons
J. B. Jiao, Zengyu Zhang,

Guangyin Lu

и другие.

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

N-heterocyclic carbene (NHC) organocatalysis has experienced significant advancements. Two distinct reaction pathways have been developed, ionic and radical, through Breslow intermediates (BIs) enolates (BI-s), respectively. The ability to selectively generate these is crucial for optimizing outcomes. In this paper we show that with mesoionic carbenes (MICs) it possible control the formation of BIs versus BI-s, use weak bases strong bases, Of particular interest coupling aldehydes alkyl halides yield ketones via an pathway.

Язык: Английский

Процитировано

0

Construction of C–S and C–Se Bonds via Photocatalytic Aromatization-Driven Deconstructive Diversification of Spiro-Dihydroquinazolinones Derived from Unstrained Ketones DOI
Tao Wang,

Jin‐Long Dai,

Yifeng Jiang

и другие.

The Journal of Organic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Май 13, 2025

A novel and robust deconstructive functionalization reaction of spiro-dihydroquinazolinones with sulfenylating reagents in the presence base has been realized under visible light irradiation. This enabled direct ring-opening unstrained cyclic ring systems, producing skeletally diverse functionalized quinazolinones moderate to good yields. range variety including diaryl disulfide, thiosulfonate, dithiosulfonate 1-[(trifluoromethyl)thio]-2,5-pyrrolidinedione were compatible for this transformation. In addition, diselenide selenosulfonate could also couple form C-Se Bonds. Mechanistic studies revealed that proceeds via a radical-radical coupling pathway.

Язык: Английский

Процитировано

0

Redox-Paired Reductive Heck Reaction and Oxidative Esterification Catalyzed by Mesoionic Carbenes DOI

B. HUANG,

Zengyu Zhang, J. B. Jiao

и другие.

Organic Letters, Год журнала: 2024, Номер 26(35), С. 7419 - 7424

Опубликована: Авг. 22, 2024

Paring a reductive reaction and an oxidative in one could be immensely important achieving atom economic environmental advantages. Herein, we report simple protocol that combines two such Heck reactions esterification by using mesoionic carbenes as catalysts to synthesize multiple valuable products under mild conditions.

Язык: Английский

Процитировано

3

Cooperative Photoredox and N-Heterocyclic Carbene-Catalyzed Formal C-H Acylation of Cyclopropanes via Deconstruction-Reconstruction Strategy DOI Creative Commons
Fan Gao,

Tian Wang,

Xiaoyu Yan

и другие.

Chemical Science, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

Cooperative NHC/photoredox catalyzed deconstruction–reconstruction of aryl cyclopropanes was described to access various α-acylated cyclopropane derivatives.

Язык: Английский

Процитировано

2

Ketone Skeletal Modification via a Metallaphotoredox-Catalyzed Deacylation and Acylation Strategy DOI

Ke‐Han He,

Na Jin, J. Paul Chen

и другие.

Organic Letters, Год журнала: 2024, Номер 26(44), С. 9503 - 9507

Опубликована: Окт. 28, 2024

Herein, we describe a dual catalytic strategy that employs dihydroquinazolinones, derived from ketone analogs, as versatile intermediates for acylation via α C–C cleavage with 2-pyridyl esters, facilitating the efficient synthesis of variety ketones. The reaction accommodates wide range ketones and carboxylic acids, showing tolerance to various functional groups. versatility this synthetic technique is further highlighted through its application in late-stage modification pharmaceuticals biologically active natural products.

Язык: Английский

Процитировано

1

Electrochemical C H alkylation of N-heterocycles via aromatization-driven C C fragmentation of unstrained ketones DOI
Peng Ye, Yi Xiong, Bo Zhang

и другие.

Tetrahedron Letters, Год журнала: 2024, Номер 155, С. 155440 - 155440

Опубликована: Дек. 27, 2024

Язык: Английский

Процитировано

1

Deuteration Degree Controllable Synthesis of Aryl Deuteromethyl Ethers Through Dual photoredox and Thiol Catalysis DOI
Junjie Yang, Zhongxian Li,

Zhihui Huang

и другие.

Chemistry - A European Journal, Год журнала: 2024, Номер 30(62)

Опубликована: Авг. 22, 2024

Herein, we report a facile and efficient deuteration degree controllable method for the preparation of aryl deuteromethyl ethers through dual photoredox thiol catalysis using phenols as starting materials inexpensive D

Язык: Английский

Процитировано

0

Photoredox decarboxylative acylation of carboxylic acid by 4-acyl-1,2,3-triazoliums DOI Creative Commons
Zengyu Zhang, Shiqing Huang, Fan Gao

и другие.

Green Synthesis and Catalysis, Год журнала: 2024, Номер unknown

Опубликована: Окт. 1, 2024

Язык: Английский

Процитировано

0

Revealing Dinitrogen Activation via Mesoionic Carbenes: A Computational Design with Frustrated Lewis Pairs DOI
Shiqing Huang, Tian Wang, Zengyu Zhang

и другие.

Asian Journal of Organic Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 13, 2024

Abstract Activating dinitrogen under metal‐free conditions remains a significant challenge in chemistry. In this study, we computationally designed frustrated Lewis pair (FLP) system incorporating bis(trimethylsilyl)boryl substituent on mesoionic carbene (MIC) framework. Our models show both kinetic and thermodynamic favorability for activation. Aromaticity enhancement along the potential energy surface (PES) plays critical role driving reaction. This work provides insights into utilizing main‐group elements activation offers applications inert molecule optical materials.

Язык: Английский

Процитировано

0