化学•材料最新文献

{"title":"Machine Learning-Driven Exploration of Composition- and Temperature-Dependent Transport and Thermodynamic Properties in LiF-NaF-KF Molten Salts for Nuclear Applications.","authors":"Guang-Ying Li, Yu-Han Lv, Li Zhang, Kewei Jiang, Lei Zhang, Yuhui Liu, Xiao-Li Tan, Tao Bo","doi":"10.1021/acs.jpcb.5c03444","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c03444","url":null,"abstract":"<p><p>This study developed a high-precision deep potential (DP) model based on density functional theory (DFT) and the DP-GEN workflow to efficiently simulate the microscopic structures and thermophysical properties of LiF-NaF-KF molten salt systems with varying compositions. Through iterative optimization of the training data set using the DP-GEN active learning strategy, our DP model demonstrated excellent agreement with DFT calculations in predicting energies, forces, and stresses. Leveraging this model, we systematically investigated the local structures and properties of 22 FLiNaK molten salt compositions, including radial distribution functions (RDFs), coordination numbers (CNs), density (ρ), heat capacity (<i>C</i>_p), self-diffusion coefficients (SDCs), electrical conductivity, and shear viscosity. The analysis revealed that Li-F ion pairs exhibit the strongest localized coordination, with the coordination numbers of all cations increasing with higher LiF content. Density was found to be primarily governed by NaF concentration, showing a positive correlation with NaF content. Viscosity was significantly influenced by both temperature and composition, decreasing notably with increasing temperature - the viscosity of the eutectic composition decreased from 3.933 mPa·s at 873 K to 1.622 mPa·s at 1073 K. Higher KF content led to lower viscosity due to the weaker interactions of K-F ion pairs. Additionally, noneutectic compositions with high LiF content (e.g., 80% LiF) exhibited significantly superior <i>C</i>_p compared to the eutectic system. This work elucidates the regulatory effects of composition and temperature on the structure-property relationships of molten salts, expands the property database for noneutectic FLiNaK systems, and provides a theoretical foundation for the design and performance optimization of molten salt reactor materials.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A New Transparent Organic Glass with Unity Photoluminescence Quantum Yield.","authors":"Xingchu Mao, Jun Wei, Yuhai Zhang","doi":"10.1002/asia.202500497","DOIUrl":"https://doi.org/10.1002/asia.202500497","url":null,"abstract":"<p><p>Transparent meltable glasses are keenly desired for making color-conversion layer of Mini-LEDs. In this work, transparent luminescent organic glasses were prepared using a new matrix of heptyltriphenylphosphonium bromide (C₂₅H₃₀BrP, HTPBr). Through doping of a blue dye (9,10-diphenylanthracene, DPA), the resulting glass exhibited a high transparency (92%) and a blue emission at 436 nm. Importantly, the PL QY of glass reached up to nearly unity under 398-nm excitation. X-ray diffraction (XRD) measurement confirmed the amorphous nature of the glass. Thermal characterization revealed a glass transition temperature (T_g) of 28 °C, a melting temperature (T_m) of 178 °C, and a thermal decomposition temperature of 270 °C. Apart from the blue-emitting glass, green- and red-emitting glasses of high transparency were synthesized varied chromophores, including 9,10-bis(phenylethynyl)anthracene (BPEA) and rhodamine B. In a proof-of-concept experiment, these glasses were used to encapsulate UV LEDs via a simple dipping process, which showed a satisfactory color rendering ability. This work brought a new member into the family of transparent luminescent glasses, promising many applications in areas including full-color displays and large-area mini-LED panels.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e00497"},"PeriodicalIF":3.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Intracellular Subdegree Temperature Sensing and Dynamics by Thermoresponsive Silver Nanoclusters as Molecular Probes.","authors":"Saurabh Rai,Sameeksha Agrawal,Saptarshi Mukherjee","doi":"10.1021/acs.jpclett.5c02357","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02357","url":null,"abstract":"Reported herein are long-lived, red-luminescent silver nanoclusters (AgNCs) protected by the small-molecule ligand thiolactic acid, which exhibit exceptional stability (shelf life exceeding three years, photostability ∼100%), water-solubility, and high biocompatibility, making them suitable for diverse applications such as sensing and live-cell imaging. The AgNCs display extremely sensitive (>2% K-1) temperature-dependent luminescence, monitored by a dual approach of changes in photoluminescence intensity and excited-state lifetime, enabling precise local thermal environment monitoring with a very high-resolution temperature sensing down to subdegree levels (<0.5 K). MTT assay, confocal fluorescence imaging, and fluorescence lifetime imaging microscopy (FLIM) analysis of mammalian cells suggest that the non-cytotoxic AgNCs specifically stain lysosomes in live cells, functioning as an organelle-specific biomarker and providing critical insights into lysosomal dynamics and intracellular temperature fluctuations. The unique properties of these AgNCs, corroborated by detailed mechanistic studies, open new avenues for studying nanoscale subcellular physiology and developing temperature-sensitive diagnostics and preservation strategies.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"35 1","pages":"9316-9324"},"PeriodicalIF":6.475,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Impact of Monomer Sequence and Interaction Parameter on Polymer Glass Transition Temperature.","authors":"Lauren W Taylor, Rodney D Priestley, Richard A Register","doi":"10.1021/acs.jpcb.5c03909","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c03909","url":null,"abstract":"<p><p>Control of the glass transition temperature (<i>T</i>_g) is a major goal in polymer engineering as <i>T</i>_g is a key determinant of mechanical behavior, barrier properties, and material processability. In copolymers of nonpolar monomers, the Fox equation can provide an approximate description of the dependence of <i>T</i>_g on copolymer composition (monomer ratio), based on a harmonic weighted average of <i>T</i>_g values for the individual homopolymers. However, the Fox equation does not consider the influence of intermonomer interactions, nor does it account for self-concentration effects. Here, we explore changes in <i>T</i>_g by altering copolymer sequence and the interaction parameter (χ) between monomer units, with the Fox equation as a benchmark. We synthesized styrene/isoprene random copolymers with varying sequence at a 50:50 wt % overall styrene:isoprene composition and a molecular weight of approximately 100 kg/mol. The sequence was altered from an entirely random copolymer by incorporating short (∼5-10 kg/mol) homopolymer blocks of either polystyrene (PS) or polyisoprene (PI) at either the end or center of a random copolymer chain. Fully random styrene-isoprene copolymers show only a slight negative deviation (∼3 °C) from the Fox equation. Incorporation of a short homopolymer block of either PS or PI into the chain resulted in an additional depression of the <i>T</i>_g (by ∼2 °C). This depression is not influenced by the location of the block but instead reflects self-concentration of the blocks. Additionally, we hydrogenated the isoprene units to increase χ and observed even larger negative deviations from the Fox equation (by ∼13 °C). These results demonstrate that both sequence and monomer interactions are polymer design parameters that can be used to manipulate bulk <i>T</i>_g.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999252","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"When <i>B</i>₂ is Not Enough: Evaluating Simple Metrics for Predicting Phase Separation of Intrinsically Disordered Proteins.","authors":"Wesley W Oliver, William M Jacobs, Michael A Webb","doi":"10.1021/acs.jpcb.5c04955","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c04955","url":null,"abstract":"<p><p>Understanding and predicting the phase behavior of intrinsically disordered proteins (IDPs) is of significant interest due to their role in many biological processes. However, effectively characterizing phase behavior and its complex dependence on protein primary sequence remains challenging. In this study, we evaluate the efficacy of several simple computational metrics to quantify the propensity of single-component IDP solutions to phase separate; specific metrics considered include the single-chain radius of gyration, the second virial coefficient, and a newly proposed quantity termed the expenditure density. Each metric is computed using coarse-grained molecular dynamics simulations for 2,034 IDP sequences. Using machine learning, we analyze this data to understand how sequence features correlate with the predictive performance of each metric and to develop insight into their respective strengths and limitations. The expenditure density is determined to be a broadly useful metric that combines simplicity, low computational cost, and accuracy; it also provides a continuous measure that remains informative across both phase-separating and non-phase-separating sequences. Additionally, this metric shows promise in its ability to improve predictions of other properties for IDP systems. This work extends existing literature by advancing beyond binary classification, which can be useful for rapidly screening phase behavior or predicting other properties of IDP-related systems.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145005628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-phosphorylating DNAzyme DK1 enables programmable multi-analyte readout via PfAgo","authors":"Tao Hu ,&nbsp;Hongmei Feng ,&nbsp;Xinxin Ke ,&nbsp;Yao Liu ,&nbsp;Shengsheng Ma ,&nbsp;Wei Li ,&nbsp;Wenqing Xiang ,&nbsp;Jia-hui Zhao ,&nbsp;Zichuan Wang ,&nbsp;Tengfei Xu ,&nbsp;Chuanxia Chen ,&nbsp;Chunyi Hu","doi":"10.1016/j.bios.2025.117968","DOIUrl":"10.1016/j.bios.2025.117968","url":null,"abstract":"<div><div>DNAzymes possessing kinase-like activities have long held theoretical promise, yet their practical implementation has remained significantly limited. Notably, DNAzyme kinase 1 (DK1), discovered over two decades ago, exhibits a unique self-phosphorylation capability upon encountering specific substrates like ATP, but its broad-based and programmable applications have not yet been fully realized. In this study, we innovatively couple DK1's autophosphorylation mechanism with the <em>Pf</em>Ago to establish a novel programmable cascade sensing platform named RASTEN (<u>R</u>obust <em>pf</em><u>A</u>go-based <u>S</u>trategy for POC <u>Te</u>sting <u>N</u>on-nucleic Acid and Nucleic Acid). Upon activation by ATP-induced DK1 self-phosphorylation, RASTEN leverages <em>Pf</em>Ago to initiate a sequential cleavage of two reporter probes, enabling rapid, one-pot, visual detection of diverse biomolecular targets. Utilizing this DK1-<em>Pf</em>Ago cascade system, we successfully developed a practical point-of-care (POC) diagnostic assay using test strips, demonstrated through highly sensitive detection of ATP in simulated human serum samples. Additionally, RASTEN exhibits exceptional versatility by harnessing alkaline phosphatase (ALP) activity as another example, effectively achieving sensitive visual detection of protein biomarkers. The inherent programmability of RASTEN, facilitated by the modifiable DK1 substrate sequences, further broadens its applicability across various nucleic acid and non-nucleic acid targets. Clinical validation highlights RASTEN's substantial advantages over commercial diagnostic kits, including significantly reduced costs, streamlined user experience, and instrument-free operation. This innovative integration of DK1 and <em>Pf</em>Ago establishes a robust and adaptable biosensing platform, presenting compelling opportunities for versatile, cost-effective, and practical multi-analyte diagnostics.</div></div>","PeriodicalId":259,"journal":{"name":"Biosensors and Bioelectronics","volume":"290 ","pages":"Article 117968"},"PeriodicalIF":10.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145004897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Palladium-Catalyzed Carbonylative Synthesis of Amide-Containing 3,4-Dihydroisoquinolin-1(2H)-ones from N-Propargylamides.","authors":"Wei Chen,Shuwei Li,Xiaolong Wang,Linqi Wang,Jianwei Wang,Yan Cao,Jun Ying","doi":"10.1021/acs.joc.5c01621","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01621","url":null,"abstract":"A palladium-catalyzed cyclization and carbonylation of N-propargylamides with amines has been developed, which incorporates an amide unit into 3,4-dihydroisoquinolin-1(2H)-one scaffolds. By using benzene-1,3,5-triyl triformate (TFBen) as the safe and convenient CO source, the reaction proceeded smoothly to afford a variety of amide-containing 3,4-dihydroisoquinolin-1(2H)-one derivatives in high yields.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"30 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995851","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Health prognostics and maintenance decision-making for wind energy: A comprehensive overview","authors":"Mingxin Li ,&nbsp;Zifei Xu ,&nbsp;Shen Li ,&nbsp;Yuka Kikuchi ,&nbsp;You Dong ,&nbsp;Konstantinos C. Gryllias ,&nbsp;Piero Baraldi ,&nbsp;Enrico Zio ,&nbsp;James Carroll","doi":"10.1016/j.rser.2025.116269","DOIUrl":"10.1016/j.rser.2025.116269","url":null,"abstract":"<div><div>As wind power installations continue to expand rapidly, ensuring reliable and cost-effective Operation and Maintenance (O&amp;M) over the wind turbine lifetime has become increasingly important. With the development of Industry 4.0, predicting the health status of wind turbines and making informed maintenance decisions has become an urgent challenge that must be addressed to enable the next generation of O&amp;M paradigms. This paper starts with presenting a comprehensive review of health prognostics for wind turbines. Existing approaches are generally divided into two main categories: (1) model-based methods, including physics-based and knowledge-based approaches, and (2) data-driven methods, which encompass statistical methods as well as Artificial Intelligence (AI)-based methods, including both traditional and emerging AI methods. Subsequently, the maintenance decision-making problem informed by wind turbine health information is systematically summarized, with a particular focus on the historical evolution, problem formulation, data challenges, modeling techniques, optimization objectives, and solving techniques. Finally, key open challenges in the context of future digital and intelligent O&amp;M are highlighted, and potential research directions are outlined to address these challenges.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"226 ","pages":"Article 116269"},"PeriodicalIF":16.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144996752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advanced approaches for mitigating impact of pre-treatment generated inhibitors in lignocellulosic hydrolysates: A comprehensive review","authors":"Ajay Kumar Pandey ,&nbsp;Harpreet Kaur ,&nbsp;Naseem A. Gaur","doi":"10.1016/j.rser.2025.116266","DOIUrl":"10.1016/j.rser.2025.116266","url":null,"abstract":"<div><div>Second-generation (2G) bioethanol generation from lignocellulosic biomass (LCB) is a renewable and sustainable alternative to fossil fuels. However, the recalcitrant character of LCB, requires physicochemical pretreatment, which generates some toxic inhibitors (furans, carboxylic acids, and phenolic compounds). These inhibitors inhibit microbial growth during fermentation by disrupting cellular redox balance, damaging membranes integrity, and inhibiting metabolic activities, leading to decreased ethanol yield and productivity. This review discusses generation and toxicity mechanism of these inhibitors, and detoxification strategies such as physical, chemical, and biological to hybrid approaches. It also highlights microbial bioprospecting, metabolic engineering, and adaptive evolution for developing robust inhibitor-tolerant strains. Integration of systems biology tools (such as genomics, transcriptomics, proteomics, metabolomics, and fluxomics) with artificial intelligence (AI)-based modeling is emphasized for revealing intricate cellular stress response pathway to guide précised strain engineering. Key challenges are, optimizing pretreatment method to minimize inhibitors, while maximizing cellulose accessibility for low-lignin biomass, however for high-lignin biomass an efficient cost-effective detoxification strategy is essential. Moreover, microbial inhibitors tolerance and fermentation strategies for overcoming synergistic toxicity are also critical. Therefore, future research should focus on integrating multi-omics approaches, statistical/AI-driven optimization, and leveraging synthetic biology for developing commercially viable and environmentally friendly 2G bioethanol biorefineries. To the best of our knowledge, this is the first review that comprehensively summarizes inhibitors generation, toxicity mechanism, detoxification strategies, robust strain development strategies, and system biology- AI integration for advancing sustainable lignocellulosic bioethanol production.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"226 ","pages":"Article 116266"},"PeriodicalIF":16.3,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144988799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unveiling the X-ray-Induced Rabi Dynamics in Resonant Auger Fragment Spectra","authors":"Quan Wei Nan, Victor Kimberg, Chao Wang, Maomao Gong, Yongjun Cheng, Kiyoshi Ueda, Song Bin Zhang","doi":"10.1021/acs.jpclett.5c02116","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02116","url":null,"abstract":"Vibrationally resolved resonant Auger spectroscopy (RAS) on bound-continuum transitions enables highly sensitive probing of ultrafast dissociation in molecular core-excited states, where a distinct fragment band arises from Auger decay in dissociation fragments. Here, we theoretically investigate fragment band formation driven by ultrashort X-ray pulses. Unlike conventional molecular bands, fragment RAS peaks exhibit an insensitivity to strong X-ray Rabi oscillations. Numerical simulations on water molecules reveal that combining RAS with a fragment’s kinetic energy release spectra enables clear observation of Rabi oscillation when the pulse broadening is smaller than the fragment’s vibrational frequencies. This work establishes a framework for controlling ultrafast electron–nuclear dynamics in fragmentation by using X-ray pulses.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}