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Chinese Journal of Chemistry 2024年第2期42卷 129-134页

作者： Shimeng Li Yizhen Liu Zuowei Xie shenzhen grubbs institute and Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055China

This work describes a general method for the synthesis of a series of sulfenylated and selenylated carboranes at room temperature using readily available iodocarboranes as starting materials via boron-centered carboranyl radicals.Such hypervalent boron radicals are generated by a visible-light-promoted Pd(O)/Pd(I)pathway.They are useful intermediates and can be trapped by disulfides and phenylselenyl chloride for the convenient construction of B-S/Sebonds.

关键词： Carborane Sulfenylation Selenylation B-I activation Radical Photocatalysis Boron Selectivity

Atroposelective Synthesis of 2-Arylindoles via Chiral Phosphoric Acid-Catalyzed Direct Amination of Indoles

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Chinese Journal of Chemistry 2024年第7期42卷 731-735页

作者： Wen Bao Ye-Hui Chen Yu-Wei Liu Shao-Hua Xiang Bin Tan School of Pharmacy&StateKey Laboratory of Applied Organic Chemistry Lanzhou UniversityLanzhouGansu 730000China shenzhen grubbs institute Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong 518055China

Indole-based atropisomers are a very important class of axially chiral compounds.However,the atroposelective synthesis of axially chiral 2-arylindole remains largely unexplored.In this study,we report the successful synthesis of atropisomeric 2-arylindoles using direct amination of indoles with p-quinonediimines in the presence of chiral phosphoric acid as a catalyst.Quinonediimine acts as an aminating reagent through formal polarity inversion of imine.The malonate group on the 2-aryl of 2-indoles was found to be essen-tial for high enantioselectivity of the products.This could be due to the additional interaction between the ester group and the cata-lyst,as well as the intramolecular hydrogen bonding.Our findings provide a new strategy for the asymmetric construction of 2-arylindole atropisomers.

关键词： Chiral phosphoric acid Quinonediimines Direct amination Nucleophilic addition Asymmetric catalysis Enantioselectivity Axially chiral 2-arylindole Atroposelective synthesis

Total synthesis of a putative yuzurimine-type Daphniphyllum alkaloid C_(14)–epi-deoxycalyciphylline H

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Chinese Chemical Letters 2024年第4期35卷 336-339页

作者： Jingping Hu Jing Xu shenzhen grubbs institute and Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis and shenzhen Key Laboratory of Small Molecule Drug Discovery and Synthesis Southern University of Science and TechnologyShenzhen 518055China

One of the largest subfamilies within the famous Daphniphyllum alkaloid family is made up of the yuzurimine-type(or macrodaphniphyllamine-type) alkaloids. Their complex aza-polycyclic caged structures, several contiguous stereogenic centers, and vicinal all-carbon quaternary centers make these alkaloids formidable challenge for synthetic chemists. Recently, synthesis of these alkaloids has received extensive attention from our community. Herein, we wish to report the total synthesis of C_(14)–epideoxycalyciphylline H, a putative member of yuzurimine-type alkaloid subfamily. Key transformations employed in our approach include an intramolecular Prins reaction and a Pd-catalyzed enyne cycloisomerization. In addition, synthesis of a daphnezomine L-type alkaloid, paxdaphnidine A, was also studied.

关键词： Total synthesis Daphniphyllum alkaloids Yuzurimine-type alkaloids Prins reaction Enyne cycloisomerization

Strain-promoted S-arylation and alkenylation of sulfinamides using arynes and cyclic alkynes

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Science China Chemistry 2024年第3期67卷 928-935页

作者： Xi Zou Boming Shen Gao-lin Li Qian Liang Yanhua Ouyang Binghe Yang Peiyuan Yu Bing Gao State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringInstitute of Chemical Biology and NanomedicineHunan UniversityChangsha 410082China Department of Chemistry and shenzhen grubbs institute Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China

The conversion of commercially available chiral sulfinamides into pharmaceutically useful chiral sulfoximines via direct SIVfunctionalization is synthetically attractive but challenging due to the competitive reaction of N-functionalization. Herein, we disclose a novel strain-release strategy to access stereospecific and chemoselective SIV-arylation and alkenylation of sulfinamides using arynes and strained cyclic alkynes. This method tolerates an unprecedented chemical diversity of functional groups attached to the nitrogen center(N-R). The origin of the high SIV-selectivity is elucidated by density functional theory calculations, suggesting a stepwise mechanism for the aryne substrates and a concerted mechanism for the cyclic alkynes.

关键词： arylation alkenylation sulfoximines sulfinamides arynes

Catalytic enantioselective N-silylation of sulfoximine

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Chinese Chemical Letters 2024年第4期35卷 352-356页

作者： Xingfen Huang Jiefeng Zhu Chuan He shenzhen grubbs institute and Department of Chemistry Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Hangzhou Normal UniversityHangzhou 311121China

A rhodium/diphosphine-catalyzed asymmetric cross-dehydrogenative coupling between sulfoximines and dihydrosilanes has been achieved. This is the first report on the enantioselective N-silylation of sulfoximines. The protocol gives access to a variety of Si-stereogenic N-silylated sulfoximines in decent yield(up to 99%) with excellent stereoselectivity(up to 99%), featuring high atom economy, and a cleaner manner with H2as the sole byproduct. The obtained bis-Si-stereogenic monohydrosilane product can be further converted into the corresponding chiral polymer with pendant sulfoximine groups.

关键词： N-Silylation of sulfoximine Chiral silylamine Si-stereogenic silanes Si-CADC Asymmetric catalysis

H-and J-aggregation of conjugated small molecules in organic solar cells

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Journal of Energy Chemistry 2024年第6期93卷 174-192,I0005页

作者： Qiaoqiao Zhao Feng He State Key Laboratory of Biobased Material and Green Papermaking Qilu University of TechnologyShandong Academy of SciencesJinan 250353ShangdongChina shenzhen grubbs institute and Department of Chemistry Southern University of Science and TechnologyShenzhen 518055GuangdongChina Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055GuangdongChina

As H-and J-aggregation receive more and more attention in the research of organic solar cells(OSCs),especially in small molecular systems,deep understanding of aggregation behavior is needed to guide the design of conjugated small molecular structure and the fabrication process of OSC device.For this end,this review is written.Here,the review firstly introduced the basic information about H-and J-aggregation of conjugated small molecules in OSCs.Then,the characteristics of H-and J-aggregation and the methods to identify them were summarized.Next,it reviewed the research progress of H-and J-aggregation of conjugated small molecules in OSCs,including the factors influencing H-and J-aggregation in thin film and the effects of H-and J-aggregation on OPV performance.

关键词： H-aggregation J-aggregation Organic solar cells Small molecules Efficiency Stability

Construction of a Metallacyclopentadiene Ring through the Attack of Carbanions to M≡C Bond Followed by C—H Activation

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Chinese Journal of Chemistry 2024年第3期42卷 235-242页

作者： Chun Tang Shengjie Zhang Zhengyu Lu Qian Li Ming Luo Dafa Chen Haiping Xia State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamenFujian361005 China shenzhen grubbs institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong518055 China

Metallacyclopentadienes are important metallacycles and regarded as intermediates in many reactions,therefore,new methods to achieve them are anticipated.In this study,a formal[3+2]method,through the reactions of an osmapentalyne with benzyl carbanions,was developed.The reactions underwent a nucleophilic attack of carbanions to the Os≡C bond,followed by C—H activation to form the five-membered osmacyclopentadiene ring.Most of the reactions were carried out at room temperature,the substituents on the aromatic rings of benzyl carbanions are diverse,and the resulting products contain an Os—H bond,representing a novel type of 10C-carbolong complexes.This work provides a new convenient route to construct metallacyclopentadienes,which is expected to further promote the development of such a type of substances.

关键词： Metallacyclopentadiene Carbolong chemistry Osmium C–H activation Nucleophilic addition

Pincer Ru with a single stereogenic identity for highly efficient asymmetric transfer hydrogenation of ketones

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Science China Chemistry 2023年第5期66卷 1443-1449页

作者： Xingjun Xu Yipeng You Ming Yu Jin Fan-Jie Meng Chen Xu Xiangyou Xing shenzhen grubbs institute and Department of Chemistry Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China

The asymmetric reduction of carbonyl compounds by means of the Ru-chiral diphosphine-chiral diamine catalysts is widely useful in organic synthesis where high levels of enantioselectivities have been attributed to multiple ligand chiral elements as well as essential stereochemical matching synergies within them.Described here is the design and discovery of new pincer-type Ru-catalysts that feature only single stereogenic element within ligands,yet the such significantly simplified structure is demonstrated to be well competent for effecting asymmetric reductions as well as kinetic resolutions over a broad range of highly functionalized ketones/alcohols,including heteroaryl substituted substrates that were challenging by known catalyst systems.Alcohols were furnished not only in excellent enantioselectivities,but with turnover numbers(up to 100,000 TONs)that reach the highest levels known to date in asymmetric transfer hydrogenation of ketones.This work should help shed light on the intricate origin of enantioselection in these important processes,and further stimulate rational understanding as well as optimization of chiral catalysts towards efficiency and simplicity.

关键词： pincer Ru-catalysts asymmetric transfer hydrogenation turnover numbers heteroaryl ketones kinetic resolution

Rapid Access to Free Phenols by Photocatalytic Acceptorless Dehydrogenation of Cyclohexanones at Room Temperature

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Chinese Journal of Chemistry 2023年第21期41卷 2773-2778页

作者： Lin Min Jiani Lin Wei Shu shenzhen grubbs institute Department of Chemistryand Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhenGuangdong518055 China

Phenols are ubiquitous substructures in natural products and bioactive compounds.However,practical methods for the direct construction of phenols under mild conditions remain challenging.Herein,a photocatalytic acceptorless hydrogen-evolution aromatization of cyclohexanones or cyclohexenones at room temperature has been developed.The reaction features the visible-light and cobalt co-catalyzed sequential dehydrogenation of in-situ formed enol silyl ethers,which are regarded as a challenging process.This operationally simple method enables the synthesis of a series of phenols with diverse substitution patterns from cyclohexanones or cyclohexenones.Moreover,diverse substituted 1,2-,1,3-,and 1,4-benzenediols were obtained from cyclohexanediones,providing a general and straightforward method for the synthesis of phenols from simple starting materials under mild conditions.

关键词： Phenols Photocatalysis Dehydrogenation Cyclohexanones Cobalt catalysis Radicals

Material and device design for organic solar cells: towards efficiency and stability

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Science China Chemistry 2023年第12期66卷 3484-3494页

作者： Mingrui Pu Feng He shenzhen grubbs institute and Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055China

Organic solar cells(OSCs) have garnered significant attention as a novel photovoltaic technology and have been extensively investigated. In recent years, OSCs have made rapid strides in power conversion efficiency(PCE), demonstrating their significant potential in practical applications. In addition to high PCE, the practical application of OSCs demands a prolonged operating lifespan. The rational design of materials and devices to achieve efficient and stable OSCs is pivotal. This feature article presents a thorough analysis of our group's studies on enhancing efficiency and stability through material and device design. We introduce a range of exceptional chlorine-mediated organic photovoltaic materials and systematically summarize chlorine atom(Cl) induced effects on energy levels, molecular stacking, active layer film morphology and photovoltaic performance. Furthermore, the use of single-crystal diffraction technology allows for a comprehensive understanding of intermolecular packing and interaction at the molecular level. A series of highly efficient non-fullerene acceptors(NFAs) with threedimensional(3D) network packing structures are developed and discussed. Subsequently, based on efficient 3D network brominated NFAs, the studies on polymer and oligomer acceptor materials are carried out and achieve efficient and stable OSCs.In addition to materials design, the development of the “quasiplanar heterojunction”(Q-PHJ) based OSC device also plays an important role in achieving superior efficiency and stability. These design experiences of materials and devices hope to provide valuable guidance for the development of efficient and stable OSCs.

关键词： chlorine-mediated photovoltaic materials single-crystal 3D network efficiency stability