Science China Chemistry最新文献_第9页

Pyrazine-fused polycyclic aromatic hydrocarbons towards efficient multiple-resonance narrowband deep-blue emission

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-31 DOI: 10.1007/s11426-024-2264-7

Yajie Wang, Wei Yang, He Zhang, Nengquan Li, Shaolong Gong, Xiang Gao, Chuluo Yang

{"title":"Pyrazine-fused polycyclic aromatic hydrocarbons towards efficient multiple-resonance narrowband deep-blue emission","authors":"Yajie Wang, Wei Yang, He Zhang, Nengquan Li, Shaolong Gong, Xiang Gao, Chuluo Yang","doi":"10.1007/s11426-024-2264-7","DOIUrl":"10.1007/s11426-024-2264-7","url":null,"abstract":"<div><p>Developing organic multiple-resonance (MR) deep-blue emitters with narrow full widths at half maximum (FWHMs) is crucial for enhancing the color purity of organic light-emitting diodes (OLEDs). However, the exploration of new MR cores remains very limited to date. Furthermore, redshifting the emission color of MR emitters is also a formidable challenge. Pyrazine, characterized by its planar and rigid structure, exhibits a strong electronegativity, which may make it a promising candidate for constructing MR emitters with a red shifted emission compared to indolo[3,2,1-<i>jk</i>]carbazole (ICz)-based MR molecules. Herein, a series of polycyclic aromatic hydrocarbons (PAHs) with MR characteristics are designed and synthesized by integrating a pyrazine core with various electron-donating segments, which exhibit the narrowband deep-blue emission peaks ranging from 423 to 459 nm with FWHMs < 50 nm in toluene. It is demonstrated that increasing donor strength and changing <i>meta</i>- to <i>para</i>-oriented nitrogen atom can induce the bathochromic emission. Theoretical investigations reveal that the non-bonding orbital characteristic of pyrazine suppress the undesired stretching vibration and promote resonance effect. The optimized deep-blue OLEDs fabricated with the pyrazine-embedded MR emitters demonstrate a high external quantum efficiency (EQE) of 23.5%, and narrowband emission with an electroluminescence peak at 454 nm.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"1018 - 1025"},"PeriodicalIF":10.4,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Deciphering fungal metabolon coupling tandem inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids 螺旋体多环生物碱生物合成中偶联反电按需Diels-Alder反应和半品萘酚重排的真菌代谢解译

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-31 DOI: 10.1007/s11426-024-2134-0

Shuai Liu, Wen-Qiang Xu, Ying-Tong Di, Man-Cheng Tang, Ding-Kang Chen, Ming-Ming Cao, Yao-Wen Chang, Hong-Yu Tang, Chun-Mao Yuan, Jun-Bo Yang, Zhi-Li Zuo, Han Guo, Zi-Fei Xu, Ying Zeng, Yun-Dong Wu, Xiao-Jiang Hao

{"title":"Deciphering fungal metabolon coupling tandem inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids","authors":"Shuai Liu, Wen-Qiang Xu, Ying-Tong Di, Man-Cheng Tang, Ding-Kang Chen, Ming-Ming Cao, Yao-Wen Chang, Hong-Yu Tang, Chun-Mao Yuan, Jun-Bo Yang, Zhi-Li Zuo, Han Guo, Zi-Fei Xu, Ying Zeng, Yun-Dong Wu, Xiao-Jiang Hao","doi":"10.1007/s11426-024-2134-0","DOIUrl":"10.1007/s11426-024-2134-0","url":null,"abstract":"<div><p>In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase SpeF and P450 monooxygenase SpeG, is identified in the biosynthesis of spiro polycyclic alkaloids (+)-notoamide B and its diastereomer (+)-versicolamide B. Using notoamide E as a substance, SpeF/SpeG metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-mA with dienyl iminium unit. Subsequently, (+)-notoamide B and (+)-versicolamide B are produced <i>via</i> tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"288 - 296"},"PeriodicalIF":10.4,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Highly efficient and cis-selective semihydrogenation of dialkyl alkynes with EtOH enforced by a catalyst-state induced color-change strategy

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-30 DOI: 10.1007/s11426-024-2311-6

Zhuangxing Li, Guixia Liu, Zheng Huang

{"title":"Highly efficient and cis-selective semihydrogenation of dialkyl alkynes with EtOH enforced by a catalyst-state induced color-change strategy","authors":"Zhuangxing Li, Guixia Liu, Zheng Huang","doi":"10.1007/s11426-024-2311-6","DOIUrl":"10.1007/s11426-024-2311-6","url":null,"abstract":"<div><p>Synthesis of valuable (<i>Z</i>)-1,2-dialkyl alkenes via <i>cis</i>-semihydrogenation of alkynes is often plagued by side reactions such as alkene isomerization and over-reduction. Here we report a catalyst-state induced color-change (CatSICC) strategy for precise detection of reaction endpoint of transfer hydrogenation (TH), enabling highly efficient and <i>cis</i>-selective semihydrogenation of dialkyl alkynes with EtOH as H-donor. A series of NHC carbene-containing pincer iridium complexes (PCC<sub>NHC</sub>)IrHX (X = Br or I) have been prepared and applied to the TH reaction. Monitoring the TH process reveals a vibrant color-change of the solution from purple to yellow-orange as a result of transition of the catalyst-state from (PCC<sub>NHC</sub>)Ir(alkyne) to (PCC<sub>NHC</sub>)IrHMe(CO), signifying the complete conversion of alkyne substrate. Quenching the reaction timely according to the color-change allows access to (<i>Z</i>)-1,2-dialkyl alkenes with very high efficiency, exquisite precision, and broad functional group tolerance. The reliability and practicability of this protocol is demonstrated by <i>cis</i>-semihydrogenation of complex polyfunctionalized bioactive molecules. Mechanistic studies establish that the propensity of (PCC<sub>NHC</sub>)Ir to undergo facile EtOH decarbonylation to form <b>isomerization-inactive</b> species (PCC<sub>NHC</sub>)IrHMe(CO) only when the semihydrogenation reaction is completed is important to stereo- and chemoselectivity control.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1392 - 1401"},"PeriodicalIF":10.4,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Phenyl-extended resorcin[4]arene opens up a new avenue for highly efficient iodine adsorption

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-30 DOI: 10.1007/s11426-024-2343-5

Jingyu Chen, Jiong Zhou

引用次数: 0

Asymmetric construction of axial and planar chirality with N-heterocyclic carbene (NHC) organocatalysis

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-30 DOI: 10.1007/s11426-024-2363-4

Meng Zhang, Xiaoqun Yang, Xiaolin Peng, Xiangyang Li, Zhichao Jin

引用次数: 0

Co-assembly of chiral copper(I) complexes and achiral polymer for enhanced circularly polarized luminescence

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-29 DOI: 10.1007/s11426-024-2238-8

Ting Liu, Muxin Yu, Yangxingyu Ye, Yunfang Zhao, Zhijia Li, Zhiyuan Wu, Feilong Jiang, Lian Chen, Maochun Hong

{"title":"Co-assembly of chiral copper(I) complexes and achiral polymer for enhanced circularly polarized luminescence","authors":"Ting Liu, Muxin Yu, Yangxingyu Ye, Yunfang Zhao, Zhijia Li, Zhiyuan Wu, Feilong Jiang, Lian Chen, Maochun Hong","doi":"10.1007/s11426-024-2238-8","DOIUrl":"10.1007/s11426-024-2238-8","url":null,"abstract":"<div><p>Circularly polarized luminescence (CPL) has attracted growing attention for their promising applications in chiral functional devices. Achieving CPL materials with both high luminescence dissymmetry factors (<i>g</i><sub>lum</sub>) and emission efficiency is attractive but remains great challenges. In this study, a pair of chiral Cu(I) complexes named <i>R/S</i>-CuI with <i>C</i><sub>2</sub> symmetry were synthesized, exhibiting no emission in solution and weak CPL with <i>g</i><sub>lum</sub> = ± 3.3×10<sup>−3</sup> in crystalline state. Transparent chiral films (<i>R/S</i>-CuI-film) were developed through the co-assembly of <i>R/S</i>-CuI and achiral polymer PMMA. The films show bright green luminescence with the quantum yields about 200 times higher than those in crystalline state. Meanwhile, the maximum |<i>g</i><sub>lum</sub>| value is also amplified by approximately 2.5 times, reaching to 8.7×10<sup>−3</sup>. Mechanism investigation suggests that the notable enhancement of luminescence efficiency can be ascribed to the restriction of the intramolecular motions and the elimination of the oxygen quenching effect, while the improvement in <i>g</i><sub>lum</sub> values may be explained by the chirality transfer from the axially chiral molecule <i>R/S</i>-CuI to the achiral polymer PMMA. Furthermore, <i>R/S</i>-CuI-film were used for advanced information encryption applications based on its CPL characteristics. This work may provide new inspirations for the construction of CPL-active films with high performance, thereby expediting their further development.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"935 - 942"},"PeriodicalIF":10.4,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Visible-light-induced controllable transformations of cumulative aryldienes through an energy transfer process

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-28 DOI: 10.1007/s11426-024-2310-4

Ling Qian, Ziqi Yu, Jiaxin Liu, Yin Wei, Min Shi

引用次数: 0

Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules 揭示分子间相互作用对高效有机太阳能电池和组件形态进化的影响

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-28 DOI: 10.1007/s11426-024-2272-3

Xueqing Ma, Yingying Cheng, Yuqiang Liu, Xinming Zheng, Guangliu Ran, Hongxiang Li, Xinyue Cui, Andong Zhang, Wenkai Zhang, Pei Cheng, Wenchao Huang, Zhishan Bo

{"title":"Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules","authors":"Xueqing Ma, Yingying Cheng, Yuqiang Liu, Xinming Zheng, Guangliu Ran, Hongxiang Li, Xinyue Cui, Andong Zhang, Wenkai Zhang, Pei Cheng, Wenchao Huang, Zhishan Bo","doi":"10.1007/s11426-024-2272-3","DOIUrl":"10.1007/s11426-024-2272-3","url":null,"abstract":"<div><p>Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells (OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene (EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene (DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-eC9-4F results in pre-aggregation and longer crystallization duration of BTP-eC9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in blade-coated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"264 - 272"},"PeriodicalIF":10.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide 有机离子对控制l -丙交酯阳离子开环聚合：制备富等规结晶型聚丙交酯的新方法

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-28 DOI: 10.1007/s11426-024-2370-6

Zhiqiang Ding, Mingqian Wang, Zijing Zhou, Bin Wang, Yuesheng Li

{"title":"Controlled cationic ring-opening polymerization of L-lactide by organic ion pair: novel approach to isotactic-rich and crystalline polylactide","authors":"Zhiqiang Ding, Mingqian Wang, Zijing Zhou, Bin Wang, Yuesheng Li","doi":"10.1007/s11426-024-2370-6","DOIUrl":"10.1007/s11426-024-2370-6","url":null,"abstract":"<div><p>Living/controlled cationic ring-opening polymerization (ROP) of <i>L</i>-lactide is a promising approach to isotactic-rich and crystalline poly(<i>L</i>-lactide). In contrast with the unsubstituted lactones, <i>L</i>-LA can not be polymerized by organic Lewis acids or carbenium ions, and the state of the art in this field is the cationic ROP of <i>L</i>-LA catalyzed by Brønsted acid/alcohol system <i>via</i> activated monomer mechanism. Herein, we reported the first example of controlled cationic ROP of <i>L</i>-LA by using Meerweintype ion pair [Me<sub>3</sub>O]<sup>+</sup>[B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub>]<sup>−</sup> as the catalyst. [Me<sub>3</sub>O]<sup>+</sup>[B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub>]<sup>−</sup> promoted rapid <i>L</i>-LA cationic polymerization in the absence of alcohol, producing isotactic-rich and crystalline PLLA without transesterification and epimerization side reactions. An activated chain end mechanism, involving twice S<sub>N</sub>2 substitution and configuration-inversion (<i>S</i>→<i>R</i>→<i>S</i>) with the assistance of released Me<sub>2</sub>O, was proposed and further verified by density functional theory and control experiments. This work expands the catalytic toolbox of isotactic-rich and crystalline polylactide synthesis. It represents a unique example of cationic-controlled polymerization of <i>L</i>-LA catalyzed by an organic ion pair.</p></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"394 - 402"},"PeriodicalIF":10.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Donor-acceptor modulation of coordination polymers for effective photothermal conversion 配位聚合物有效光热转换的供体-受体调制

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-25 DOI: 10.1007/s11426-024-2253-y

Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu

{"title":"Donor-acceptor modulation of coordination polymers for effective photothermal conversion","authors":"Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu","doi":"10.1007/s11426-024-2253-y","DOIUrl":"10.1007/s11426-024-2253-y","url":null,"abstract":"<div><p>The targeted construction of donor-acceptor (D-A) materials featuring efficient photothermal (PT) conversion properties has been an attractive but challenging goal. Herein, a new series of coordination polymers (CPs) featuring different PT performances were constructed with flexible linker 1,1′-Ferrocenedicarboxylic acid (FCA) and 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (TPT) as acceptor and donor molecules including coronene and tetrathiafulvalene (TTF). Based on the flexible configurations of FCA ligand and the directing of donor dependent D-A interactions, the structures of <b>TF-1</b> to <b>TF-3</b> featuring distinctive dimension were obtained based on Cd(II) ions for investigating the PT property in configurational perspectives. A systematic investigation of the PT properties of the CPs was performed. Notably, <b>TF-3</b> exhibits the finest PT conversion effect under the irradiation of 560 nm laser, while <b>TF-2</b> shows optimal PT conversion under 808 nm laser irradiation required for biological PT therapy, illustrating the correlation between the structural and component features of the CPs and their PT performances. Furthermore, Zn(II) as bio-friendly ion was utilized to construct hypotoxic <b>TF-4</b> that reveals similar structure to that of <b>TF-2</b> for potential application. Polydimethylsiloxane (PDMS) patches doped with <b>TF-4</b> exhibits considerable NIR PT conversion effect under 808 nm, represented by the nearly 80 °C temperature increased in 120 s for <b>TF-4</b>@PDMS patch (1.2 wt%) under 0.9 W cm<sup>−2</sup> irradiation, the results of which herein indicate the potential of D-A CPs as versatile platform for the modulation of PT materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4175 - 4183"},"PeriodicalIF":10.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757993","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0