Chemical Science最新文献_第3页

Cordycepin: a dual-function molecular element for aptamer engineering with enhanced anticancer activity 冬虫夏草素：具有增强抗癌活性的适体工程双功能分子元件

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc02571k

Fei Gao, Li Na, Shuyue Fu, Jinsong Peng, Shipeng He, Ruowen Wang, Weihong Tan

{"title":"Cordycepin: a dual-function molecular element for aptamer engineering with enhanced anticancer activity","authors":"Fei Gao, Li Na, Shuyue Fu, Jinsong Peng, Shipeng He, Ruowen Wang, Weihong Tan","doi":"10.1039/d5sc02571k","DOIUrl":"https://doi.org/10.1039/d5sc02571k","url":null,"abstract":"Cordycepin (3′-deoxyadenosine, 3′-dA), derived from the fungus Cordyceps sinensis, has shown significant bioactivity as an inhibitor of enzymes related to 2′-deoxyadenosine (dA). However, its therapeutic efficacy is insufficient for clinical use, which may be addressed through targeted delivery systems. In this study, we designed and synthesized a 3′-dA phosphoramidite to incorporate cordycepin into the well-known cancer-targeting Sgc8c aptamer, where it functions both as a structural modulator and as a bioactive drug element for constructing aptamer–drug conjugates. Its structural similarity to dA makes cordycepin a unique molecular tool for probing the structure–activity relationship of aptamers. Additionally, cordycepin can be seamlessly integrated into aptamers, replacing dA. This led to the generation of a series of cordycepin-modified aptamers, among which Sgc8-23A demonstrated enhanced antitumor activity against HCT116 human colon cancer cells. Compared to free cordycepin, Sgc8-23A exhibited superior bioactivity and stability. In a zebrafish patient-derived xenograft (PDX) model, Sgc8-23A significantly inhibited tumor growth, highlighting its potential as an effective aptamer–drug conjugate for targeted cancer therapy. These findings emphasize the dual functional potential of cordycepin as both a structural element for aptamer optimization and a therapeutic drug component, paving the way for the development of more efficient aptamer-based drug delivery systems.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"47 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515521","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

Tuning the emission properties of luminescent 1,2,3-diazaborinates 调谐发光1,2,3-重氮硼酸盐的发射特性

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc03814f

Leonie Wüst, Johannes Chorbacher, Timo Keim, Tim Wellnitz, Julian Spieß, Nele Wieprecht, Maximilian Michel, Holger Helten, Holger Braunschweig

引用次数: 0

Mechanistic Insights into Solvent-Guided Growth and Structure of MoO2 Nanoparticles in Solvothermal Synthesis 溶剂热合成中MoO2纳米颗粒在溶剂引导下生长和结构的机理研究

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc03247d

Laura Glei Graversen, Mikkel Juelsholt, Olivia Aalling-Frederiksen, Ulrik Friis-Jensen, Maria Storm Thomsen, Andrea Kirsch, Nicolas Pierre Louis Magnard, Kirsten Marie Ørnsbjerg Jensen, Rebecca Katharina Pittkowski

{"title":"Mechanistic Insights into Solvent-Guided Growth and Structure of MoO2 Nanoparticles in Solvothermal Synthesis","authors":"Laura Glei Graversen, Mikkel Juelsholt, Olivia Aalling-Frederiksen, Ulrik Friis-Jensen, Maria Storm Thomsen, Andrea Kirsch, Nicolas Pierre Louis Magnard, Kirsten Marie Ørnsbjerg Jensen, Rebecca Katharina Pittkowski","doi":"10.1039/d5sc03247d","DOIUrl":"https://doi.org/10.1039/d5sc03247d","url":null,"abstract":"Understanding the processes involved in the nucleation and growth of nanoparticles is essential for the development of tailored nanomaterials. Here, we investigate the solvent effects on the atomic structure and size of nanocrystalline MoO2 from a solvothermal synthesis and deduce their reaction pathways. Detailed pair distribution function (PDF) analysis reveals the formation of distinct MoO2 structures, depending on the alcohol used. We show that the atomic structure and crystallite size of the formed materials can be directly related to their formation pathway. In situ PDF together with X-ray absorption spectroscopy of the reaction between MoCl5 and an alcohol solvent allows us to see that larger nanoparticles (ca. 30 nm) with the conventional MoO2 distorted rutile structure form when the initial Cl/O-ligand exchange is fast, but the subsequent condensation and crystallization is slowed down in the synthesis process. On the other hand, when the Cl/O exchange is slowed down, a [MoIVClxOy]-complex is formed, and we obtain very small nanoparticles (2-3 nm) with the MoO2 high-pressure polymorph structure. The study shows how the chemistry of the reaction solvent affects the mechanistic pathways, and consequently the intermediate formed just prior to crystallization, which is directly applicable in the process of obtaining specific nanocrystalline materials.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"24 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515528","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

Dielectric stabilization controls excited-state proton transfer and ion pair dynamics in organic solvents 介质稳定控制有机溶剂中的激发态质子转移和离子对动力学

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc03404c

Tatu Kumpulainen, Amar Raj, Pragya Verma, Andrey Belyaev, Pasi Myllyperkiö

{"title":"Dielectric stabilization controls excited-state proton transfer and ion pair dynamics in organic solvents","authors":"Tatu Kumpulainen, Amar Raj, Pragya Verma, Andrey Belyaev, Pasi Myllyperkiö","doi":"10.1039/d5sc03404c","DOIUrl":"https://doi.org/10.1039/d5sc03404c","url":null,"abstract":"Excited-state proton transfer (ESPT) in aprotic organic solvents has received limited attention due to their inability to accept protons. However, bimolecular ESPT from a photoacid to an organic base in such media enables systematic studies on the influence of macroscopic solvent parameters on the ESPT as demonstrated in this work. The full photocycle starting from initial deprotonation in a hydrogen-bonded donor-acceptor complex to full dissociation in the excited state followed by slow recombination in the ground state was characterized by various spectroscopic methods in solvent mixtures of varying polarity. The initial deprotonation producing contact ion pairs is ultrafast (sub-100 fs) and requires minimal solvent reorganization. The contact ion pairs dissociate via a distinct intermediate, so-called solvent-separated ion pair, preceding the fully dissociated free ion pairs. Time scale of the ion pair dynamics is dominated by viscosity whereas the yield is determined by the polarity. In low polarity solvents (εr < 10), the population is trapped as solvent-separated ion pairs and full dissociation becomes operative only at intermediate polarity. Ground-state recombination of the intermediate ion pair species is fast and thus a significant population of fully dissociated ground-state ions is produced only above intermediate polarities.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"634 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515523","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

Ultra-Wide Time-Dependent Phosphorescence Color of Carbon Dots via Synergistic Strategy of Dual Confinement Structures Constructing Multiple Luminescent Centers 基于构建多个发光中心的双约束结构协同策略的碳点超宽时变磷光色

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc02963e

Shiwei Zhang, Cheng-Long Shen, Jiurong Li, Junfei Liao, Peng Miao, Xiujian Zhao, Xiao Gong

{"title":"Ultra-Wide Time-Dependent Phosphorescence Color of Carbon Dots via Synergistic Strategy of Dual Confinement Structures Constructing Multiple Luminescent Centers","authors":"Shiwei Zhang, Cheng-Long Shen, Jiurong Li, Junfei Liao, Peng Miao, Xiujian Zhao, Xiao Gong","doi":"10.1039/d5sc02963e","DOIUrl":"https://doi.org/10.1039/d5sc02963e","url":null,"abstract":"Phosphorescent materials with time-dependent phosphorescent color (TDPC) output have significant potential for applications in advanced optical information encryption. However, the effective construction of TDPC composites compatible with multiple phosphorescent emission centers to achieve wider phosphorescent colors evolving over time in a single material system remains a huge challenge. Here, ultra-wide TDPC composites evolving with time were firstly realized in a single system by exploiting the synergistic effect of the doubly confined structure. Utilizing organosilanes to pretreat the reactive precursor, combined with a boric acid (BA) matrix, the composite (Si-CDs@B2O3) was prepared by direct calcination. Our results reveal that the Si-CDs@B2O3 composite has significant ultra-wide TDPC properties, with the phosphorescent emission shifting from red to orange, yellow, green, and cyan blue. Characterization analysis reveals the important role of organosilanes in achieving the ultra-wide TDPC property, and also elaborates that the red phosphorescence and blue phosphorescence originate from the interaction of C=O on the surface of CDs with BA matrix and the intrinsic blue phosphorescence emitted from B-O in the BA matrix, respectively. The distinctive dynamic room-temperature phosphorescence properties of the Si-CDs@B2O3 composite were leveraged to develop a strategy for its use in information encryption on a precise time scale.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"46 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515531","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

Insights from designing an artificial cascade catalysis system using principles from substrate channeling in enzymes 利用酶的底物通道原理设计人工级联催化系统的见解

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc02781k

Frances A. Houle, Peter Agbo, Junko Yano

{"title":"Insights from designing an artificial cascade catalysis system using principles from substrate channeling in enzymes","authors":"Frances A. Houle, Peter Agbo, Junko Yano","doi":"10.1039/d5sc02781k","DOIUrl":"https://doi.org/10.1039/d5sc02781k","url":null,"abstract":"Generalizing the key requirements of highly-selective, multi-step chemical conversions involving spatially separated reaction centers remains one of the grand challenges of chemistry. Much work towards this effort has focused on decomposing multi-step conversions into their constituent reactions, whose intermediates are successively upgraded in a chemical cascade via diffusion from center to center. This approach for synthesizing more complex molecules takes its cues from biochemical networks, where near-unit conversion of even complex carbohydrates is achieved by upgrading chemical precursors via enzymatic cascades. In this computational study we examine a simple cascade involving coupled Ag and Cu catalysts that sequentially converts CO2 to CO and then CO2 and CO to reduced products, generically named CO2Product and COProduct. The system architecture is inspired by the phenomenon of biological substrate channeling, and components are examined to evaluate their effects on conversion efficiency in the cascade. Aside from a substrate channel linking two reaction centers, we find efficient cascades must also incorporate directional substrate diffusion, compartmentalization of the reaction centers, and proper timing of substrate arrival at the active center. We make explicit linkages between these requirements and chemical conversion in known biological systems, revealing additional control elements that could be incorporated.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"9 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515524","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

Single-Molecule Graphene Quantum Dot: a Novel Efficient Photosensitizer for Photodynamic Cancer Therapy 单分子石墨烯量子点：一种用于光动力癌症治疗的新型高效光敏剂

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc03226a

Jintao Chen, Shiru Yin, futing Yang, Shengnan Guo, Jiaojiao Zhang, Zhenming Lu, Tian Gao

{"title":"Single-Molecule Graphene Quantum Dot: a Novel Efficient Photosensitizer for Photodynamic Cancer Therapy","authors":"Jintao Chen, Shiru Yin, futing Yang, Shengnan Guo, Jiaojiao Zhang, Zhenming Lu, Tian Gao","doi":"10.1039/d5sc03226a","DOIUrl":"https://doi.org/10.1039/d5sc03226a","url":null,"abstract":"Graphene quantum dots (GQDs) can efficiently generate reactive oxygen species (ROS) under light irradiation, demonstrating significant potential for photodynamic therapy (PDT) applications. However, GQDs are often multicomponent mixtures with highly complex structures, which significantly hinders their clinical applications. Therefore, it is urgent to design and synthesize well-defined GQDs with excellent PDT performance. In this work, a novel single-molecule hydrophilic pure graphene quantum dot (HPGQD), containing 132 sp² conjugated carbon atoms, was prepared through an organic synthetic route using single-benzene-ring molecules as precursors. The HPGQD features a unique D-12A structure, comprising one large electron donor center and 12 electron acceptors, which grants it exceptional ROS release capabilities with a singlet oxygen (1O2) quantum yield of 0.85. Notably, under light irradiation, HPGQD can rapidly generate abundant ROS within 30 s and scavenge them after 10 min, which holds promise for eliminating the need for prolonged light avoidance in patients undergoing PDT. It has been successfully applied to both in vitro (IC50: 0.22 μmol L-1) and in vivo (tumor weight inhibition rate: 71%) PDT for cancer treatment. The innovative design, synthesis, and PDT application of single-molecule HPGQD pave towards accelerated clinical applications of carbon nanomaterials, advancing the frontier of nanotherapeutic research.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"36 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515530","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

Light-controlled genome editing by activation of Cas9-mRNA translation 激活Cas9-mRNA翻译的光控基因组编辑

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc01999k

Helena Schepers, Greta Charlotte Dahm, Martin Sumser, Sabine Huewel, Andrea Rentmeister

引用次数: 0

Spatially Programmed Regioisomeric Conjugated Microporous Polymers Modulating Zinc Sites for Selective CO2 Photoreduction to CH4 空间编程区域异构体共轭微孔聚合物调节锌位点选择性CO2光还原为CH4

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc02835c

Xingwang Lan, Juan Wang, Lu Chen, Haobo Xu, Tianjun Zhang, Yong Chen

{"title":"Spatially Programmed Regioisomeric Conjugated Microporous Polymers Modulating Zinc Sites for Selective CO2 Photoreduction to CH4","authors":"Xingwang Lan, Juan Wang, Lu Chen, Haobo Xu, Tianjun Zhang, Yong Chen","doi":"10.1039/d5sc02835c","DOIUrl":"https://doi.org/10.1039/d5sc02835c","url":null,"abstract":"Conjugated microporous polymers show great potential for photocatalytic CO2 reduction into value-added products. However, their catalytic activity and selectivity remain significantly limited due to poor charge separation efficiency and the lack of suitable active sites. Herein, we propose a topology-driven dipole programming strategy that synergistically decouples atomic-level electronic configuration control from spatially resolved active site engineering. Crucially, the regioisomer-dependent π-topology governs light-harvesting ability, dipole polarization hierarchy, and directional charge transport networks. As a result, the designed Zn-TPA-BPy-1, featuring dipole polarization fields and extra-channel Zn-N₂O₂ sites, exhibits exceptional photocatalytic CO2 conversion activity, with a CH4 evolution rate of 753.18 μmol g-1 h-1 and a high selectivity of 89.7%. Experimental and theoretical results reveal that asymmetric dipole arrays lower the energy barrier for *COOH and *CO intermediates while stabilizing *CHO intermediates through dynamic charge compensation, which contributed to the high activity and selectivity. This finding offers new insights into designing polymer-photocatalysts by subtle structural modulation for CO2 conversion.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"91 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515526","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

Multi-dimensional analysis of single particles with sequential dual-nanopipette sensors 单粒子序列双纳米吸管传感器的多维分析

IF 8.4 1区化学

Chemical Science Pub Date : 2025-06-30 DOI: 10.1039/d5sc02604k

Rui-Xue Gao, Si-Yu Tian, Ying Chen, Yu-Ting Qi, Limin Xiang, Wei-Hua Huang, Xin-Wei Zhang

{"title":"Multi-dimensional analysis of single particles with sequential dual-nanopipette sensors","authors":"Rui-Xue Gao, Si-Yu Tian, Ying Chen, Yu-Ting Qi, Limin Xiang, Wei-Hua Huang, Xin-Wei Zhang","doi":"10.1039/d5sc02604k","DOIUrl":"https://doi.org/10.1039/d5sc02604k","url":null,"abstract":"Nanoparticles play crucial roles in a wide range of scientiﬁc and industrial fields. Analysing the physicochemical characteristics of nanoparticles is of paramount importance in identifying and classifying different particles. However, due to their small size and inherent heterogeneity, comprehensive analysis of the size and shape, especially the complex surface characters, of individual particles is still confronted with challenges. In this work, we reported a facile strategy to construct a sequential dual-nanopipette sensor (SDNS) with two sensing interfaces for multi-parameter detection of nanoparticles at the single particle level. The collaboration of the two sensing interfaces enabled dual recognition of the same particle, which improved the detection accuracy effectively. With this platform, it was not only possible to perform concentration quantification and size characterization, but also effectively classify the particles via dual determination of the surface charge or the biochemical components of the particles. As the sensing interfaces of SDNS can be varied to meet the detection requirements, this approach can be easily adjusted to analyse more kinds and dimensions of surface characters of single nanoparticles, which opens up new avenues for the exploration of biological or other kinds of nanoparticles as well as the deeper comprehension of particle functions and evolution.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"186 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515529","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