Chemical Science最新文献_第9页

Enabling technology for accelerated discovery of supramolecular materials 加速发现超分子材料的技术

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-08 DOI: 10.1039/d5sc03960f

Caitlin Elise Shields, Abbie M. Scholes, Anna Grace Slater

引用次数: 0

Catalytic Asymmetric Synthesis of Indole-based Atropisomers Bearing Silicon-Stereogenic Center 含硅立体中心的吲哚基atrosomomer的催化不对称合成

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc05320j

Si-Yi Liu, Zi-Qi Zhu, Fei-Xiao Chen, Ni-Na Feng, Shaofei Ni, Feng Shi

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Reactivity of organic photocatalysts displaying thermally activated delayed fluorescence (TADF): rationalizing unexpected differences between rates of quenching of the lowest singlet and triplet states 显示热激活延迟荧光（TADF）的有机光催化剂的反应性：最低单线态和三重态猝灭率之间意想不到的差异的合理化

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc04948b

Federica Fina, Caterina Bellatreccia, Xia Wu, Pier Giorgio Cozzi, Alessandro Troisi, Sergei Vinogradov, Paola Ceroni

{"title":"Reactivity of organic photocatalysts displaying thermally activated delayed fluorescence (TADF): rationalizing unexpected differences between rates of quenching of the lowest singlet and triplet states","authors":"Federica Fina, Caterina Bellatreccia, Xia Wu, Pier Giorgio Cozzi, Alessandro Troisi, Sergei Vinogradov, Paola Ceroni","doi":"10.1039/d5sc04948b","DOIUrl":"https://doi.org/10.1039/d5sc04948b","url":null,"abstract":"Cyanoarene chromophores exhibiting thermally activated delayed fluorescence (TADF) are increasingly used in photoredox catalysis. At high concentrations of organic substrates, which are typically employed in preparative synthesis, the primary photoinduced electron transfer (PeT) steps in the photocatalytic processes can involve both singlet (S1) and triplet (T1) excited states of TADF chromophores, despite very short lifetimes (nanoseconds) of the former. However, the difference between the reactivities of these states is not well understood, while being critically important for the photocatalytic process. In this work, three representative TADF chromophores were examined in reductive and oxidative PeT quenching reactions. First, using kinetic simulations, we assert that Stern–Volmer quenching plots based on the experimentally measured prompt and delayed fluorescence lifetimes, but not integrated intensities, yield accurate bimolecular rate constants for the PeT quenching reactions involving S1 and T1 excited states. Secondly, experimental measurements of prompt and delayed fluorescence reveal significantly higher quenching constants for reductive quenching of S1 compared to T1 states, while for oxidative quenching the rate constants are nearly equal. Electronic structure calculations provide insight into the difference between the PeT rates for reductive quenching, suggesting that it might stem from the different spatial hole–electron distributions in S1 and T1 states. Taken together, our findings bring crucial information about the photocatalytic process involving TADF chromophores that should aid the design of the next-generation of TADF photocatalysts.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"81 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235482","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}

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Spontaneous deposition of boron oxide on rhodium nanostructure for selective conversion of syngas to ethanol 氧化硼在铑纳米结构上的自发沉积用于合成气选择性转化为乙醇

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc06161j

Jiale Xiao, Cao Wang, Haotian Meng, Chengtao Wang, Hangjie Li, Yu-Xiao Cheng, Ni Yi, Wentao Yuan, Wei Zhou, Liang Cao, Liang Wang, Fengshou Xiao

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Aromaticity Switching by Quantum Tunnelling 量子隧道的芳香性开关

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc05717e

Sindy Julieth Rodríguez, Julián Santoyo-Flores, Katarzyna Młodzikowska-Pieńko, Renana Gershoni-Poranne, Sebastian Kozuch

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Switchable supramolecular polycationic assemblies for tunable antibacterial strategies against antibiotic resistance 可切换的超分子聚阳离子组合物可调节抗菌策略对抗抗生素耐药性

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc05035a

Jia Chen, Xueqian Wang, Mengrui Zhang, Xue Wang, Ran Wang, Xinxing Lyu, Yunjian Xu, Xintian Shao, Luling Wu, Tony D. James

{"title":"Switchable supramolecular polycationic assemblies for tunable antibacterial strategies against antibiotic resistance","authors":"Jia Chen, Xueqian Wang, Mengrui Zhang, Xue Wang, Ran Wang, Xinxing Lyu, Yunjian Xu, Xintian Shao, Luling Wu, Tony D. James","doi":"10.1039/d5sc05035a","DOIUrl":"https://doi.org/10.1039/d5sc05035a","url":null,"abstract":"Bacterial resistance significantly hampers the efficacy of antibiotics in eradicating pathogens and treating infections. Here, we introduce an Adaptive Cationic Therapeutic Integrated (ACTI) system, a design strategy integrating pyridinium cationic membrane disruption and tunable antibacterial activity to address this challenge. ACTI leverages the assembled hyper-enriched cationic domains to enhance the destruction of bacterial membranes, while also enabling the on-demand deactivation of antibacterial activity through disassembly, thereby safeguarding biocompatibility. Additionally, ACTI facilitates the photodynamic inactivation of negatively charged photosensitizers (TPPS) by promoting the interaction between the photosensitizer and bacteria as well as aiding the transport of singlet oxygen. ACTI-loaded photosensitizers (TPPS@ACTI) exhibited potent antibacterial activity (>99% pathogen elimination) against methicillin-resistant S. aureus (MRSA) and E. coli in vitro, and the antibacterial efficacy was further validated using an MRSA-infected murine wound model. ACTI establishes a paradigm shift for the design of tunable antimicrobials that balance potency and biosafety in complex biological environments.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"6 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235480","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

Isolation of a Lewis acid-base stabilized stannanone 路易斯酸碱稳定锡酮的分离

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc06549f

Mike Jörges, Daniel Knyszek, Manoj Kumar, Varre S Swamy, Viktoria H. Gessner

引用次数: 0

Turn-engineering tunes the conformational rigidity of β-hairpin AMPs in achieving membrane selectivity and killing drug-resistant ESKAPE pathogens 转向工程调节β-发夹amp的构象刚性，以实现膜选择性和杀死耐药ESKAPE病原体

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc06810j

Priyanka Lahiri, Swati Priyadarshini, Mahak Saini, Muskan Agrawal, Sk Abdul Mohid, Raju S Rajmani, Vishnu S Ammineni, Pritam Biswas, Aparna Asok, Amit K Baidya, Anirban Bhunia, Govardhan Reddy, Ranjana Pathania, Jayanta Chatterjee

{"title":"Turn-engineering tunes the conformational rigidity of β-hairpin AMPs in achieving membrane selectivity and killing drug-resistant ESKAPE pathogens","authors":"Priyanka Lahiri, Swati Priyadarshini, Mahak Saini, Muskan Agrawal, Sk Abdul Mohid, Raju S Rajmani, Vishnu S Ammineni, Pritam Biswas, Aparna Asok, Amit K Baidya, Anirban Bhunia, Govardhan Reddy, Ranjana Pathania, Jayanta Chatterjee","doi":"10.1039/d5sc06810j","DOIUrl":"https://doi.org/10.1039/d5sc06810j","url":null,"abstract":"Naturally occurring β-hairpin antimicrobial peptides (AMPs) exhibit potent membranolytic activity against bacterial and mammalian cells, limiting their therapeutic development due to the lack of selectivity. This study demonstrates that the reverse turn in these AMPs can be used to dictate their molecular rigidity, which drives their membranolytic action. By fine tuning the rigidity at the reverse turn by incorporating a moderately rigid β-II' turn-inducing motif through N-methylation of the amide bond, we achieved selectivity in targeting the bacterial membrane over human red blood cells. The selectivity results from the hairpin-nucleation efficiency of the engineered β-turn within these linear AMPs devoid of disulfide bridges and their interaction with the neutral mammalian and negatively charged bacterial membrane. Such fine-tuning of the structure at the β-turn, allowed us to develop molecules derived from naturally occurring toxic AMPs, which displayed selective killing of drug-resistant bacterial pathogens over mammalian cells with in vivo efficacy.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"49 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235484","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

Enhancing the Statistical Probability Factor in Triplet-Triplet Annihiltaion Photon Upconversion via TIPS Functionalization 利用TIPS功能化提高三重-三重湮灭光子上转换的统计概率因子

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc05248c

Lukas Naimovicius, Manvydas Dapkevičius, Edvinas Radiunas, Mila Miroshnichenko, Gediminas Kreiza, Carles Alcaide, Paulius Baronas, Yoichi Sasaki, Nobuhiro Yanai, Nobuo Kimizuka, Andrew Brian Pun, Miquel Solà, Pankaj Bharmoria, Karolis Kazlauskas, Kasper Moth-Poulsen

{"title":"Enhancing the Statistical Probability Factor in Triplet-Triplet Annihiltaion Photon Upconversion via TIPS Functionalization","authors":"Lukas Naimovicius, Manvydas Dapkevičius, Edvinas Radiunas, Mila Miroshnichenko, Gediminas Kreiza, Carles Alcaide, Paulius Baronas, Yoichi Sasaki, Nobuhiro Yanai, Nobuo Kimizuka, Andrew Brian Pun, Miquel Solà, Pankaj Bharmoria, Karolis Kazlauskas, Kasper Moth-Poulsen","doi":"10.1039/d5sc05248c","DOIUrl":"https://doi.org/10.1039/d5sc05248c","url":null,"abstract":"We investigated the influence of triisopropylsilyl (TIPS) functionalization on annihilators in triplet-triplet annihilation photon upconversion, specifically focusing on their spin statistical probability factor. A new green-emitting annihilator 3,9-bis((triisopropylsilyl)ethynyl)perylene (TIPS-PY) displaying a record red-to-green TTA-UC quantum yield of 13.7% (50% theoretical maximum) is synthesized. This remarkable efficiency was achieved due to the following features of the TIPS functionalization of PY: 1) retaining a high fluorescence quantum yield of 95%, 2) reduced triplet energy to 1.29 eV enabling efficient triplet energy transfer (~100%) from the sensitizer, PdTPBP (T1= 1.55 eV), and 3) a high efficiency of singlet generation after triplet coupling, indicated by the statistical probability factor, f = 39.2% ± 2.4%. Notably, the f value of TIPS-PY surpasses other annihilators in the 470-570 nm emission range. Excited state computational analysis using TheoDORE, revealed a higher percentage of charge transfer character in S0S1 in TIPS-PY compared to PY, indicative of higher singlet-like character in their triplet-pair state 1(T1T1), which can enhance the coupling of the triplet-pair state with the excited singlet-state, thereby increasing the efficiency of singlet generation, a phenomenon undisclosed before. Furthermore, the suitable T1 of TIPS-PY enables upconversion of 730 nm light when sensitized with Os(m-peptpy)2(TFSI)2 (T1 = 1.63 eV), demonstrating the broad upconversion range of TIPS-PY in the phototherapeutic window desired for biological applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"20 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235483","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

Towards Large-scale Chemical Reaction Image Parsing via a Multimodal Large Language Model 基于多模态大语言模型的大规模化学反应图像解析

IF 8.4 1区化学

Chemical Science Pub Date : 2025-10-07 DOI: 10.1039/d5sc04173b

Yufan Chen, Ching Ting Leung, Jianwei Sun, Yong Huang, Linyan Li, Hao Chen, Hanyu Gao

{"title":"Towards Large-scale Chemical Reaction Image Parsing via a Multimodal Large Language Model","authors":"Yufan Chen, Ching Ting Leung, Jianwei Sun, Yong Huang, Linyan Li, Hao Chen, Hanyu Gao","doi":"10.1039/d5sc04173b","DOIUrl":"https://doi.org/10.1039/d5sc04173b","url":null,"abstract":"Artificial intelligence (AI) has demonstrated significant promise in advancing organic chemistry research; however, its effectiveness depends on the availability of high-quality chemical reaction data. Currently, most published chemical reactions are not available in machine-readable form, limiting the broader application of AI in this field. The extraction of published chemical reactions into structured databases still relies heavily on manual curation, and robust automatic parsing of chemical reaction images into machine-readable data remains a significant challenge. To address this, we introduce the Reaction Image Multimodal large language model (RxnIM), the first multimodal large language model specifically designed to parse chemical reaction images into machine-readable reaction data. RxnIM not only extracts key chemical components from reaction images but also interprets the textual content that describes reaction conditions. Together with a specially designed large-scale dataset generation method to support model training, our approach achieves excellent performance, with an average F1 score of 88% on various benchmarks, surpassing state-of-the-art methods by an average of 5%. This represents a crucial step toward the automatic construction of large databases of machine-readable reaction data parsed from images in the chemistry literature, providing essential data resources for AI research in chemistry. The source code, model checkpoints, and datasets developed in this work are released under permissive licenses.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"39 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235485","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