Chemical Science最新文献_第2页

Recent progress in small-molecule fluorescent probes for the detection of superoxide anion, nitric oxide, and peroxynitrite anion in biological systems 用于检测生物系统中超氧化物阴离子、一氧化氮和过亚硝酸阴离子的小分子荧光探针的最新进展

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-20 DOI: 10.1039/d4sc06722c

Yongqing Zhou, Xuan Kuang, Xiaofeng Yang, Juan Li, Xianzhe Wei, Won Jun Jang, Shan-Shan Zhang, Mei Yan, Juyoung Yoon

{"title":"Recent progress in small-molecule fluorescent probes for the detection of superoxide anion, nitric oxide, and peroxynitrite anion in biological systems","authors":"Yongqing Zhou, Xuan Kuang, Xiaofeng Yang, Juan Li, Xianzhe Wei, Won Jun Jang, Shan-Shan Zhang, Mei Yan, Juyoung Yoon","doi":"10.1039/d4sc06722c","DOIUrl":"https://doi.org/10.1039/d4sc06722c","url":null,"abstract":"Superoxide anion (O2˙−), nitric oxide (NO), and peroxynitrite anion (ONOO−) play essential roles in physiological and pathological processes, which are related to various symptoms and diseases. There is a growing need to develop reliable techniques for effectively monitoring the changes in these three reactive species across different molecular events. Currently, small-molecule fluorescent probes have been demonstrated to be reliable imaging tools for the optical detection and biological analysis of reactive species in biological systems due to their high spatiotemporal resolution and in situ capabilities. In consideration of the distinct features of these three reactive species, abundant fluorescent probes have been developed to meet various requirements. In this context, we systematically summarized the latest progress (2020–2023) in organic fluorescent probes for monitoring O2˙−, NO, and ONOO− in living systems. Furthermore, the working principles and biological applications of representative fluorescent probes were illustrated. Moreover, we highlighted the current challenges and future trends of fluorescent probes, offering general insights into future research.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"57 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673845","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

Effective Design Strategy for Thermally Activated Delayed Fluorescence Emitters with Aggregation-Induced emission to Enable Sky-blue OLEDs Achieving EQE Nearly 30% 具有聚集诱导发射的热激活延迟荧光发射器的有效设计策略，使天蓝色 OLED 的 EQE 接近 30

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-20 DOI: 10.1039/d4sc06613h

Hui Dai, Yaohui Liang, Xiang Long, Tianyi Tang, Haozhi Xie, Zhiwei Ma, Gaoyu Li, Zhiyong Yang, Juan Zhao, Zhenguo Chi

引用次数: 0

Strongly Photoluminescent and Radioluminescent Copper(I) Iodide Hybrid Materials Made of Coordinated Ionic Chains 由配位离子链构成的强光发光和辐射发光碘化亚铜（I）杂化材料

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc06242f

Jingwen Chen, Kang Zhou, Jingbai Li, Guozhong Xu, Xiuze Hei, Jing Li

引用次数: 0

Switchable Magnetic Resonance Imaging Nanoplatform for in Situ MicroRNA Imaging 用于原位 MicroRNA 成像的可切换磁共振成像纳米平台

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc04675g

Yan Tan, Junren Wang, Qian Wan, Jinlong Yang, Jinkun Huang, Zijia Zhou, Haifeng Dong, Xueji Zhang

{"title":"Switchable Magnetic Resonance Imaging Nanoplatform for in Situ MicroRNA Imaging","authors":"Yan Tan, Junren Wang, Qian Wan, Jinlong Yang, Jinkun Huang, Zijia Zhou, Haifeng Dong, Xueji Zhang","doi":"10.1039/d4sc04675g","DOIUrl":"https://doi.org/10.1039/d4sc04675g","url":null,"abstract":"Aberrant microRNA (miRNA) expression is associated with various types of carcinogenesis, making miRNA a promising candidate for diagnostic and therapeutic biomarkers. However, in situ miRNA diagnostics remains a significant challenge owing to the various biological barriers. Herein, we report a novel miRNA imaging probe consisting of a PEG-Polylysine-PNIPAM polymer matrix-modified small Fe3O4 nanoparticle (PAA-Fe3O4-DNA@PPP) with an improved circulatory half-life, efficient tissue permeability, and enhanced tumor accumulation, for in situ miRNA magnetic resonance imaging (MRI). In this strategy, we employed the large size PAA-Fe3O4-DNA@PPP to improve circulatory time and utilized PEG-Polylysine-PNIPAM as a GSH-responsive moiety to dissociate PAA-Fe3O4-DNA@PPP and release small size PAA-Fe3O4-DNA for enhanced tumor permeability. Specifically, the target miRNA acts as a cross-linker for PAA-Fe3O4-DNA, forming larger assemblies that not only amplify the MRI signal for detection but also enhance retention for prolonged observation. Both in vitro and in vivo results validate that the imaging probe exhibits an enhanced MRI signal with 3.69-fold amplification for tumor interior miRNA detection, allowing the dynamic changes in miRNA to be monitored by the probe. Given its long circulation, efficient penetration, and enhanced tumor accumulation, the PAA-Fe3O4-DNA@PPP probe holds great promise for in situ miRNA imaging and spatial genomics analysis in situ.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"18 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670743","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

Ru(II)-catalyzed regioselective oxidative Heck reaction with internal olefins that tolerated strongly coordinating heterocycles Ru(II)-catalyzed regioselective oxidative Heck reaction with internal olefins that tolerated strongly coordinating heterocycles（Ru(II)催化的可容忍强配位杂环的内部烯烃的区域选择性氧化 Heck 反应

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc07036d

Ci Chen, Qiaoya Zhang, Zhiwei Huang, Wensen Ouyang, Yang Gao, Jiye Luo, Yuan Liu, Yanping Huo, Qian Chen, Xianwei Li

引用次数: 0

Main-chain stiff-stilbene photoswitches in solution, in bulk, and at surfaces 溶液、块体和表面的主链硬芪光开关

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc06470d

Naoki Kaneda, Keiichi Imato, Ayane Sasaki, Ryo Tanaka, Ichiro Imae, Toyoaki Hirata, Takuya Matsumoto, Yousuke Ooyama

{"title":"Main-chain stiff-stilbene photoswitches in solution, in bulk, and at surfaces","authors":"Naoki Kaneda, Keiichi Imato, Ayane Sasaki, Ryo Tanaka, Ichiro Imae, Toyoaki Hirata, Takuya Matsumoto, Yousuke Ooyama","doi":"10.1039/d4sc06470d","DOIUrl":"https://doi.org/10.1039/d4sc06470d","url":null,"abstract":"Molecular photoswitches have been incorporated into polymer backbones to control the macromolecular conformations by structural changes of the main-chain photoswitches. However, previous photoswitches installed in the main chains are thermolabile, which precludes deep understanding, precise regulation, and practical applications of the macromolecular conformational changes. Herein, we focus on sterically hindered stiff stilbene (HSS), an emerging photoswitch offering large structural changes in isomerization between the thermally bistable E and Z isomers, and disclose the chemistry of main-chain HSS photoswitches in solution, in bulk, and at thin film surfaces. We synthesize and investigate three types of linear polymers with different chemical linkages between HSS repeating units, polyurethane, polyester, and polyene. The polymer conformations in solution, i.e., hydrodynamic volume, are reversibly photocontrollable in a precise manner by the E/Z ratio. Further, the nanoscopic conformational transformations are amplified to macroscopic photoswitching of the solution transmittance and the surface wettability synergistically with changes between interchain and intrachain hydrogen bonding in the polyurethanes. Additionally, the Z-to-E photoisomerization in the glassy state yields above 70%, which is comparable to that in solution and extraordinarily high despite the restricted molecular mobility. The findings in this study will pave the way for practical and unconventional applications of smart polymer systems based on photoswitches.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"78 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670700","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

Dithienoarsinines: Stable and Planer π-Extended Arsabenzenes 二噻吩胂：稳定的平面π-扩展砷苯

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc06590e

Akifumi Sumida, Akinori Saeki, Kyohei Matsuo, Kensuke Naka, Hiroaki Imoto

引用次数: 0

Unlocking Regioselectivity: Steric Effects and Conformational Constraints of Lewis Bases in Alkyllithium-Initiated Butadiene Polymerization 开启区域选择性：烷基锂引发的丁二烯聚合中路易斯碱的立体效应和构象约束

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-19 DOI: 10.1039/d4sc05144k

Jian Tang, Yuan Fu, Jing Hua, Jiahao Zhang, Shuoli Peng, Zhibo Li

{"title":"Unlocking Regioselectivity: Steric Effects and Conformational Constraints of Lewis Bases in Alkyllithium-Initiated Butadiene Polymerization","authors":"Jian Tang, Yuan Fu, Jing Hua, Jiahao Zhang, Shuoli Peng, Zhibo Li","doi":"10.1039/d4sc05144k","DOIUrl":"https://doi.org/10.1039/d4sc05144k","url":null,"abstract":"In nonpolar solvents, alkyllithium-initiated 1,3-butadiene polymerization exhibits high 1,4-selectivity, which shifts towards 1,2-selectivity upon the addition of Lewis bases. For the past 50 years, the prevailing hypothesis has suggested that Lewis bases primarily influence regioselectivity through electronic effects. However, our study reveals that steric hindrance also plays a crucial role. Using X-ray single-crystal diffraction, we analyzed the structure of the active species and proposed a new model for the chain-growth transition state. Techniques such as in-situ NMR spectroscopy, isotope labeling studies, and density functional theory (DFT) calculations were employed to compare the impact of electronic and steric effects of various Lewis bases on regioselectivity. Our findings demonstrate that during 1,4-addition, the butadiene monomer is forced into close proximity with the Lewis base ligand, leading to significant steric interference and thus favoring 1,2-addition. Furthermore, we applied the concepts of “conformational restriction” to explain the enhanced 1,2-selectivity observed with ring-containing Lewis bases such as 1,2-dipiperidylethane. Building on this understanding, we have designed several highly efficient and cost-effective Lewis bases which achieves close to 100% 1,2-selectivity under mild con-ditions and significantly outperforms the best previously reported Lewis base, 1,2-dipiperidylethane, across a broad temperature range.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"33 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670702","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

6,6'-Biindeno[1,2-b]fluorene: an open-shell indenofluorene dimer 6,6'-联茚并[1,2-b]芴：一种开壳茚芴二聚体

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-18 DOI: 10.1039/d4sc03996c

Himanshu Sharma, Palash Jana, Dibyendu Mallick, Subhajit Bandyopadhyay, Soumyajit Das

{"title":"6,6'-Biindeno[1,2-b]fluorene: an open-shell indenofluorene dimer","authors":"Himanshu Sharma, Palash Jana, Dibyendu Mallick, Subhajit Bandyopadhyay, Soumyajit Das","doi":"10.1039/d4sc03996c","DOIUrl":"https://doi.org/10.1039/d4sc03996c","url":null,"abstract":"Nakano et al. reported that the antiaromatic indenofluorene (IF) isomers are diradicaloid molecules having varying degrees of open-shell character, with indeno[1,2-b]fluorene displaying a weaker diradical character index (y0 = 0.072). Unlike 6,12-trimethylsilylethynyl disubstituted [1,2-b]IF, the 6,12-aryl disubstituted [1,2-b]IF derivatives did not show any experimental evidence of diradical properties. This raised the question of whether an [1,2-b]IF dimer would prefer a closed-shell or an open-shell ground state. To address it, herein we report the synthesis of a 6,6'-biindeno[1,2-b]fluorene derivative, which is an [1,2-b]IF dimer, constructed by linking two [1,2-b]IF units with a C-C single bond at carbons 6 and 6' bearing the largest orbital coefficients for the highest occupied and lowest unoccupied molecular orbitals (HOMO and LUMO). The C6-C6' linkage effectively narrowed the HOMO-LUMO gap while the strong desire to avoid s-indacene antiaromaticity restored two Clar sextets in two proaromatic para-quinodimethane subunits, resulting in an open-shell bifluorenylidene-type diradicaloid (y0 = 0.268) ground state with minor tetraradical character index (y1 = 0.007). The open-shell nature was confirmed by single crystal X-ray and electron paramagnetic resonance analyses, and supported by theoretical calculations.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"135 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665398","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

Dithienonaphthobisthiadiazole synthesized by thienannulation of electron-deficient rings: an acceptor building unit for high-performance π-conjugated polymers 通过缺电子环的噻吩化合成的二噻吩基萘双噻二唑：高性能 π 共轭聚合物的受体构建单元

IF 8.4 1区化学

Chemical Science Pub Date : 2024-11-18 DOI: 10.1039/d4sc05793g

Tsubasa Mikie, Tomokazu Morioku, Shota Suruga, Momoka Hada, Yuki Sato, Hideo Ohkita, Itaru Osaka

{"title":"Dithienonaphthobisthiadiazole synthesized by thienannulation of electron-deficient rings: an acceptor building unit for high-performance π-conjugated polymers","authors":"Tsubasa Mikie, Tomokazu Morioku, Shota Suruga, Momoka Hada, Yuki Sato, Hideo Ohkita, Itaru Osaka","doi":"10.1039/d4sc05793g","DOIUrl":"https://doi.org/10.1039/d4sc05793g","url":null,"abstract":"The development of building units for π-conjugated polymers is a driving force in advancing the field of organic electronics. In this study, we designed and synthesized dithienonaphthobisthiadiazole (TNT) as a thiophene-fused acceptor (A) building unit and two TNT-based π-conjugated polymers named PTNT2T and PTNT1-F. We found that the microwave-assisted thiophene annulation reaction (thienannulation) of arylethynylated naphthobisthiadiazole (NTz) via C–H functionalization effectively produced TNT moieties. With the π-extended structure of TNT, the polymers had rigid backbones that benefited in-plane and out-of-plane charge carrier transport. Organic field-effect transistors (OFETs) based on PTNT2T exhibited hole mobilities as high as 1.10 cm2 V−1 s−1. Furthermore, organic photovoltaic cells (OPVs) based on PTNT1-F showed high power conversion efficiencies of up to 17.4% when combined with a nonfullerene acceptor. This work provides an efficient method for the thienannulation of electron-deficient rings to access thiophene-fused A building units and shows the great promise of TNT as a building unit for high-performance π-conjugated polymers for organic electronic devices.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"22 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665352","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