ACS Central Science最新文献_第6页

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-07-23

Albert Marten Schulte, Jorrit W. A. Schoenmakers, Marleen van Oosten, Paul C. Jutte, Jan Maarten van Dijl*, Wiktor Szymanski* and Ben L. Feringa*,

引用次数: 0

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-07-23

Xiang-Qian Xie, Wen Guo, Yin-Zheng Xia, Li-Juan Liao, Meng-Xin Sun, Jing-Xue Wang, Jiang-Tao Gao*, Hong-Wei Yao* and Huan Wang*,

引用次数: 0

Entropy Drives the Predictive Discovery of an Optimal Cleavable Comonomer for ROMP 熵驱动ROMP最佳可切割共聚体的预测发现

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-23 DOI: 10.1021/acscentsci.5c00521

Kwangwook Ko, Piper L. MacNicol, Mingming Zhu, Lei Zhang, Saifudin M. Abubakar and Jeremiah A. Johnson*,

{"title":"Entropy Drives the Predictive Discovery of an Optimal Cleavable Comonomer for ROMP","authors":"Kwangwook Ko, Piper L. MacNicol, Mingming Zhu, Lei Zhang, Saifudin M. Abubakar and Jeremiah A. Johnson*, ","doi":"10.1021/acscentsci.5c00521","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00521","url":null,"abstract":"Ring-opening metathesis polymerization (ROMP) of norbornene derivatives enables access to polymeric materials for applications ranging from targeted drug delivery to high-performance thermosets; however, the carbon–carbon backbones of ROMP-derived poly(norbornenes) resist deconstruction under mild, selective conditions. Cleavable comonomers (CCs) have been introduced to address this limitation, yet their implementation has been hindered by prohibitive costs and/or suboptimal reactivity. Moreover, the discovery of existing CCs has been largely empirical, lacking clear design principles. Here, we identify the entropy of ring-opening as one of the key determinants of ROMP copolymerization behavior of the best-performing CCs reported to date. Guided by this insight, we establish predictive design criteria and introduce Me4Si2O9, a CC that exhibits near-ideal room temperature copolymerization with a broad range of norbornene-based (macro)monomers. Me4Si2O9 is significantly less expensive than leading silyl ether-based CCs and enables uniform incorporation of cleavable linkages into polymer backbones at low loadings. Beyond delivering a cost-effective and high-performance CC, this work provides fundamental insights into ROMP copolymerization that will enable predictive CC development and expand the functional scope of deconstructable polymeric materials.A novel predictive workflow and entropy-maximizing design enabled the development of a cost-effective cleavable comonomer─Me4Si2O9─that uniformly embeds deconstructable bonds in ROMP-derived polymers.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1408–1416"},"PeriodicalIF":10.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00521","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-07-23

引用次数: 0

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-07-23

Zhangyi Xiong, Shitao Wu, Liang Gu, Mengyang Zhai, Yuke Pan, Yanhang Ma* and Zhijie Chen*,

引用次数: 0

Accelerating and Enhancing Thermodynamic Simulations of Electrochemical Interfaces 加速和加强电化学界面的热力学模拟

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-21 DOI: 10.1021/acscentsci.5c00547

Xiaochen Du, , , Mengren Liu, , , Jiayu Peng, , , Hoje Chun, , , Alexander Hoffman, , , Bilge Yildiz, , , Lin Li, , , Martin Z. Bazant, , and , Rafael Gómez-Bombarelli*,

{"title":"Accelerating and Enhancing Thermodynamic Simulations of Electrochemical Interfaces","authors":"Xiaochen Du, , , Mengren Liu, , , Jiayu Peng, , , Hoje Chun, , , Alexander Hoffman, , , Bilge Yildiz, , , Lin Li, , , Martin Z. Bazant, , and , Rafael Gómez-Bombarelli*, ","doi":"10.1021/acscentsci.5c00547","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00547","url":null,"abstract":"Electrochemical interfaces are crucial in catalysis, energy storage, and corrosion, where their stability and reactivity depend on complex interactions between the electrode, adsorbates, and electrolyte. Predicting stable surface structures remains challenging, as traditional surface Pourbaix diagrams tend to either rely on expert knowledge or costly ab initio sampling and neglect thermodynamic equilibration with the environment. Machine learning (ML) potentials can accelerate static modeling but often overlook dynamic surface transformations. Here, we extend the Virtual Surface Site Relaxation-Monte Carlo (VSSR-MC) method to autonomously sample surface reconstructions modeled under aqueous electrochemical conditions. Through fine-tuning foundational ML force fields, we accurately and efficiently predict surface energetics, recovering known Pt(111) phases and revealing new LaMnO3(001) surface reconstructions. By explicitly accounting for bulk-electrolyte equilibria, our framework enhances electrochemical stability predictions, offering a scalable approach to understanding and designing materials for electrochemical applications.By combining automated sampling, fine-tuned machine learning force fields, and a new thermodynamic framework, we accelerate the prediction of realistic surface Pourbaix diagrams.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 9","pages":"1558–1572"},"PeriodicalIF":10.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00547","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145117301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Superior Catalytic Selectivity by Merging Carbon-Decorated Pd Species with Zeolite Micropores 碳修饰钯与沸石微孔融合的优越催化选择性

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-19 DOI: 10.1021/acscentsci.5c01175

Hai Wang, and , Feng-Shou Xiao,

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Photoinduced Immobilization on Two-Dimensional Nano Borophene Spatially Orients Capture Antibody for Highly Sensitive Biological Interactions 光诱导固定化二维纳米硼罗芬空间定向捕获抗体用于高度敏感的生物相互作用

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-17 DOI: 10.1021/acscentsci.5c00474

Satheesh Natarajan, Ketan Dighe, Teresa Aditya, Pranay Saha, David Skrodzki, Purva Gupta, Nivetha Gunaseelan, Shraddha Krishnakumar and Dipanjan Pan*,

{"title":"Photoinduced Immobilization on Two-Dimensional Nano Borophene Spatially Orients Capture Antibody for Highly Sensitive Biological Interactions","authors":"Satheesh Natarajan, Ketan Dighe, Teresa Aditya, Pranay Saha, David Skrodzki, Purva Gupta, Nivetha Gunaseelan, Shraddha Krishnakumar and Dipanjan Pan*, ","doi":"10.1021/acscentsci.5c00474","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00474","url":null,"abstract":"Two-dimensional (2D) nanomaterials are of great interest due to their unique properties and broad biological applications. Among these, borophene, a single-atom-thick boron sheet with a honeycomb structure, exhibits exceptional structural, electronic, and mechanical characteristics, making it a promising candidate for sensing, electronics, and biosensing. In this study, we report on a liquid-phase exfoliation method to synthesize stable borophene nanosheets and introduce a photoinduced immobilization technique to functionalize their surfaces with antibodies. By exploiting borophene’s electron-deficient nature, we enable strong covalent bonding with electron-rich thiol groups in antibodies. UV irradiation cleaves antibody disulfide bonds, generating free thiols that form stable boron–sulfur bonds with borophene, resulting in spatially oriented antibodies that preserve antigen-binding activity. We demonstrate the application of these functionalized nanosheets in a lateral flow immunoassay (LFIA), a key tool in point-of-care diagnostics that is often limited by poor antibody orientation. The developed LFIA detects HMGB-1, a potential endometriosis biomarker, in menstrual effluent with results in 10 min and a limit of detection of 40 pg/mL. This performance surpasses that of conventional LFIAs, showing high sensitivity, specificity, and no cross-reactivity with common blood proteins. This study highlights a novel, reagent-free strategy for functionalizing borophene, enhancing its potential in biosensing applications.A lateral flow assay platform featuring novel 2D borophene nanosheets and photoimmobilized antibodies enables ultrasensitive and rapid detection of endometriosis biomarkers in menstrual blood.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1492–1511"},"PeriodicalIF":10.4,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00474","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902112","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Radiotherapy-Activated Prodrug: Past, Present and Beyond 放射治疗激活前药：过去，现在和未来

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-16 DOI: 10.1021/acscentsci.5c00875

Changlun Wang, Zihang Zhang and Zhibo Liu*,

{"title":"Radiotherapy-Activated Prodrug: Past, Present and Beyond","authors":"Changlun Wang, Zihang Zhang and Zhibo Liu*, ","doi":"10.1021/acscentsci.5c00875","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00875","url":null,"abstract":"Radiotherapy-activated prodrug (RAP) is defined as a type of prodrug that features low toxicity before activation, transforms into an active form upon ionizing radiation exposure, and exhibits targeted therapeutic effects within the irradiated area. In clinical practice, clear evidence demonstrates that the combination of radiotherapy and chemotherapy elicits a significant synergistic antitumor response, thereby enhancing patients’ overall survival rates. As a novel therapeutic modality, RAP has recently emerged as an active area of scientific research. The primary mechanism of RAP involves utilizing the reactive species from water radiolysis under ionizing radiation to trigger controlled cleavage of covalent bonds, enabling the controlled release of active drugs. In this Outlook, we summarize the advancements in the field of RAP, encompassing the types of ionizing radiation, novel chemical structures, and diverse prodrug formats. In addition, we discuss the current challenges and future directions of this promising field.Radiotherapy-activated prodrug (RAP) exploits tumor-localized radicals (e−aq/•OH/H•) generated from water radiolysis during radiotherapy to trigger spatiotemporally controlled drug release.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1306–1320"},"PeriodicalIF":10.4,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00875","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902111","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Brightening New Horizons: Luminescent Transition Metal Complexes in Optical Imaging and Theranostic Applications 照亮新视野：发光过渡金属配合物在光学成像和治疗中的应用

IF 10.4 1区化学

ACS Central Science Pub Date : 2025-07-16 DOI: 10.1021/acscentsci.5c00975

Lawrence Cho-Cheung Lee, and , Kenneth Kam-Wing Lo*,

{"title":"Brightening New Horizons: Luminescent Transition Metal Complexes in Optical Imaging and Theranostic Applications","authors":"Lawrence Cho-Cheung Lee,  and , Kenneth Kam-Wing Lo*, ","doi":"10.1021/acscentsci.5c00975","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00975","url":null,"abstract":"Small-molecule fluorescent probes have revolutionized fluorescence imaging in both biological research and clinical applications, allowing the exploration of intricate cellular processes and aiding disease diagnosis and treatment. Advances in the designs of molecular probes have led to the development of fluorescent theranostics that combine therapeutic and diagnostic modalities in a single platform. These dual-functional agents enable simultaneous disease diagnosis, treatment, and monitoring, representing an innovative approach to precision medicine. Luminescent transition metal complexes have emerged as promising alternatives to traditional organic fluorophores for optical imaging and theranostic applications, and they offer distinctive advantages such as high photostability, long emission lifetimes, and efficient generation of reactive oxygen species. In this Outlook, we highlight emerging trends in the designs and applications of luminescent transition metal complexes as optical imaging and theranostic agents, leveraging their unique photophysical and photochemical properties. We also discuss current challenges to the clinical applications of these complexes and outline potential directions to inspire the development of next-generation theranostics for advancing disease management and improving patient care.Luminescent transition metal complexes are emerging as novel optical imaging and theranostic agents, leveraging their unique photophysical and photochemical behavior for disease diagnosis and therapy.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1289–1305"},"PeriodicalIF":10.4,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00975","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902110","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0