化学•材料最新文献

{"title":"Data-Driven Design of High-Temperature-Resistant Polyimides Using Hierarchical Gaussian Process Regression.","authors":"Jiale Zhang, Aocheng Fan, Ziqi Wang, Lei Zheng, Yu Liu, Zhijian Wang, Peng Kang","doi":"10.1021/acs.jpcb.5c03717","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c03717","url":null,"abstract":"<p><p>Accurate prediction of Tg for polyimides (PIs) is essential for assessing material performance in high-temperature applications in aerospace, electronics, microelectronics, and flexible display technology. However, experimental measurements remain critically challenging due to the labor-intensive synthesis, conventional instrument limits, and time-consuming characterization processes. Meanwhile, force field limitations, timescale discrepancy, and validation difficulties exist in the prediction of Tg for PIs using molecular dynamic simulation. In this study, we introduce a hierarchical Gaussian process regression machine learning method that integrates prior knowledge to predict Tg for PIs with small-sample data sets. We employ RDKit for molecular descriptor calculation and feature selection. Twenty-one key descriptors are identified, and exceptional model performance with a coefficient of determination <i>R</i>² of 0.98/0.74 on the training/test set is achieved, surpassing conventional machine learning approaches. We further use Shapley additive explanations analysis to study the actionable insights for designing thermally stable PIs. The number of rotatable bonds and minimum partial charge act as dominant factors influencing Tg. Validations through experimental synthesis and molecular dynamics simulations confirm that the prediction errors are below 15%, while a Bayesian update strategy employing a radial basis function kernel corrected systematic underestimation in the high-Tg regime (>270 °C). This work provides a robust, validated Tg prediction tool, elucidates critical structure-property relationships, and establishes a transferable framework for data-driven materials design, advancing the development of high-performance polymers.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853950","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":"Microplastic Distribution Patterns in Fish and Implications for Safe Consumption.","authors":"Xiaoxia Sun,Liujiang Meng,Junhua Liang,Qingjie Li,Juan Du,Mingliang Zhu,Yongfang Zhao,Shan Zheng","doi":"10.1021/acs.est.5c02907","DOIUrl":"https://doi.org/10.1021/acs.est.5c02907","url":null,"abstract":"Microplastics (MPs) are widely distributed in the ocean and can be ingested by fish. Despite fish being a major source of aquatic protein for humans, no study has yet addressed how to reduce the risk of human exposure to MPs when consuming fish. This study investigated 1,075 fish from 37 species across representative fishing areas, and the presence of MPs in various tissues, such as the gills, guts, and muscles, was analyzed to assess fish food safety comprehensively. MPs (particles >20 μm in size) were detected in 36.28% of the gills and 39.63% of the guts but were not detected in muscle tissues. Compared with those from deeper waters, the fish from upper layers presented greater MP abundances and smaller average sizes. A significant negative correlation was detected between the abundance of MPs in fish and their length and weight. The global per capita MP consumption from captured fish, including all tissues and muscles, is approximately 5.60 × 104 items/year. To minimize dietary exposure to MPs, humans should prioritize consuming only fish muscle and selecting fish from deeper waters and larger sizes whenever possible. Future efforts to optimize fish consumption patterns should involve systematically evaluating the combined risks of MPs and other pollutants, considering both the nutritional value and health benefits of fish consumption and adopting sustainable fishery management approaches.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"27 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tribute to Massimo Olivucci","authors":"Nicolas Ferré*,&nbsp; and ,&nbsp;Laura Pedraza-González*,&nbsp;","doi":"10.1021/acs.jpcb.5c04287","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c04287","url":null,"abstract":"","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 32","pages":"8075–8076"},"PeriodicalIF":2.9,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826261","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":"Bond Dissociation Energies and Electronic Calculations on the Actinide Halides ThX and UX (X = Cl, Br, I).","authors":"Thomas T Kawagoe, Dakota M Merriles, Michael D Morse, Kirk A Peterson","doi":"10.1021/acs.jpca.5c04025","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c04025","url":null,"abstract":"<p><p>Resonant two-photon ionization spectroscopy has been used to locate predissociation thresholds in the spectra of the actinide halides ThX and UX, where X = Cl, Br, and I. These predissociation thresholds are identified as the bond dissociation energies (BDEs) of the molecules. The resulting values show very similar BDEs for the corresponding ThX and UX species, with the thorium molecules being slightly more strongly bound: D₀(ThCl) = 5.077(6) eV, D₀(ThBr) = 4.391(4) eV, D₀(ThI) = 3.537(8) eV, D₀(UCl) = 4.989(3) eV, D₀(UBr) = 4.313(3) eV, and D₀(UI) = 3.449(8) eV. Here, the estimated error limit is given in parentheses in units of the last reported digit. Spinor-based coupled cluster calculations have also been carried out on the halides of this work, including also ThF and UF. The final D₀ values after including contributions due to basis set incompleteness, outer-core-correlation, picture-change, and QED effects are within 0.04 eV of the present experimental values in each case.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853929","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":"High-entropy Prussian blue analogues-mediated flexible field-effect transistor for wearable sweat dopamine monitoring","authors":"Ting Wang ,&nbsp;Tao Liu ,&nbsp;Xinglong Zhu ,&nbsp;Minghui Zhang ,&nbsp;Jidong Jiang ,&nbsp;Zhili Zhang ,&nbsp;Yang Huang ,&nbsp;Yiqing Wang","doi":"10.1016/j.bios.2025.117889","DOIUrl":"10.1016/j.bios.2025.117889","url":null,"abstract":"<div><div>Wearable sensor offers a non-invasive platform for continuous monitoring of biomarkers, but their application remains challenging due to low target level and stability issue in sweat. Here, we proposed a wearable sensing system comprising a flexible field-effect transistor (FET) integrated with a microfluidic sweat collection channel for real-time monitoring of dopamine in sweat. By functionalizing the recognition layer of FET using high-entropy Prussian blue analogues (HEPBAs), the sensor not only enables direct and selective catalysis of dopamine but also amplifies the response signal for trace dopamine determination. Benefiting from the synergistic effects of the FET and HEPBAs, the wearable sensor achieves a broad detection range from 1 pM to 10 mM, with an ultralow limit of detection (LOD) of 0.4 pM. When integrated with a flexible printed circuit board and a mobile application via Bluetooth communication, the system enables accurate and sensitive tracking of dopamine fluctuations during daily activities, revealing significant correlations with physiological states. This study demonstrates an effective and non-invasive approach for early screening and personalized treatment of neurological disorders.</div></div>","PeriodicalId":259,"journal":{"name":"Biosensors and Bioelectronics","volume":"289 ","pages":"Article 117889"},"PeriodicalIF":10.5,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144852284","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":"Preparation and performance of high-efficiency photothermal multifunctional self-healing polyurethane coating based on MoS2@CuS@ZIS ternary heterojunction and double dynamic covalent bond","authors":"Xin Wang,&nbsp;Xinwei Zhang,&nbsp;Wen Li,&nbsp;Wei Wang,&nbsp;Jie Zhu,&nbsp;Shougang Chen","doi":"10.1016/j.compositesa.2025.109242","DOIUrl":"10.1016/j.compositesa.2025.109242","url":null,"abstract":"<div><div>Marine equipment is confronted with multiple threats such as corrosion, low-temperature freezing and microbial fouling. Therefore, it is necessary to develop multi-functional protective coatings. In this study, the wear resistance, anti-fouling, photothermal, electromagnetic wave absorption, defrosting and deicing, and long-lasting anti-corrosion performance of modified polyurethane (PU) coating were improved by incorporating MoS₂@CuS@ZIS ternary heterojunctions. The results show that the coating still maintains good corrosion resistance after being soaked for 90 days. The built-in electric field of the ternary heterostructure promotes the non-radiative recombination of electrons and holes, thereby enhancing the efficiency of photothermal conversion. In addition, with the dual dynamic covalent bonds of carbamate and oxime, the coating has a rapid self-healing performance. Defrosting and deicing under light can be completed within 130 s. In addition, the highly efficient catalytic performance of the S-type heterojunction, in synergy with Cu²⁺ ions, endows the coating with excellent antibacterial properties. The incorporation of filling materials has increased the wear resistance by 34 %. This work has important participation value for the research and development of new multifunctional PU coatings.</div></div>","PeriodicalId":282,"journal":{"name":"Composites Part A: Applied Science and Manufacturing","volume":"199 ","pages":"Article 109242"},"PeriodicalIF":8.1,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144852760","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High resolution single-cell transcriptomics towards precision profiling across multi-omics and spatial dimensions","authors":"Liyong He ,&nbsp;Wenjia Wang ,&nbsp;Kaitong Dang,&nbsp;Wenyi Zhang,&nbsp;Kaiqiang Ye,&nbsp;Handong Wang,&nbsp;Yan Huang,&nbsp;Xiangwei Zhao","doi":"10.1016/j.trac.2025.118418","DOIUrl":"10.1016/j.trac.2025.118418","url":null,"abstract":"<div><div>Cellular heterogeneity poses major researchers challenges. Tag-based single-cell RNA sequencing (scRNA-seq) methods enables cell-type classification and population diversity in biological systems but lacks resolution for splicing regulation, allele expression, isoform diversity, transcriptional mutation, and the identification of comprehensive RNA types. High-resolution full-length scRNA-seq offers significant advantages in achieving molecular resolution for transcript-level quantification, structural variations detection, and the identification of comprehensive RNA types. It has been widely applied in refines cell fate determination models. Additionally, integrating full-length scRNA-seq technology with multi-omics and spatially resolved sequencing will decipher cellular interactions and their cross-modality molecular mechanisms more precisely. This review focuses on the latest iterative technology of high resolution scRNA-seq spanning poly(A+) mRNA to total RNA full-length capture systems, precision profiling methods across multi-omics and spatial dimensions, and their applications in tumor biology, reproductive medicine, immunology, and developmental biology. Finally, current challenges and prospectives are discussed.</div></div>","PeriodicalId":439,"journal":{"name":"Trends in Analytical Chemistry","volume":"192 ","pages":"Article 118418"},"PeriodicalIF":12.0,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144841926","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}

{"title":"Exploring Molecular Structure Influence on Effective Conjugate Length of Carotenoids.","authors":"Fuyang Liu, Wenhui Fang, Xin Wang, Xinyu He, Chen Zheng, Wei Zhang, Zhiwei Men","doi":"10.1021/acs.jpca.5c02800","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c02800","url":null,"abstract":"<p><p>The functions of carotenoids, including light collection, protection, antioxidation and anticancer activities, are closely related to their molecular structures. The conjugated systems confer notable electronic and photoelectricity properties. We employed UV-vis and Raman spectroscopies to characterize the conjugation of five carotenoids. Their conjugated lengths were determined as zeaxanthin < β-carotene < canthaxanthin < astaxanthin < lycopene. The molecular structures of these five carotenoids were optimized by density functional theory. Based on the optimized structures, we obtained parameters such as the HOMO-LUMO gap, bond-length alternation, and the torsion angle of ionone rings. Through analysis, the effects of hydroxyl and carbonyl groups on the effective conjugation length were obtained. In addition, the hydroxyl and carbonyl groups in astaxanthin form a unique intramolecular hydrogen bond structure, which decreases the torsion of the ionone rings. The intramolecular hydrogen bonding energy of astaxanthin was calculated to be 5.03 kcal/mol through the molecular tailoring approach.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853931","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":"Polystyrene-Induced Dehydration of Lipid Membranes: Insights from Atomistic Simulations.","authors":"Zeke A Piskulich, Zeev Rosenzweig, Qiang Cui","doi":"10.1021/acs.jpcb.5c03171","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c03171","url":null,"abstract":"<p><p>Nanoplastics, small plastic particles smaller than microplastics, have been suggested to have a wide-range of unique interactions when they encounter lipid membranes. Recent studies have demonstrated that the smaller size of nanoplastic particles may allow them to penetrate and dissolve in lipid membranes. Following this penetration, however, there is not yet a clear picture of how such particles impact the local lipid environment. A recent study by the present authors found that when lipid vesicles that included laurdan, a fluorescent dye molecule typically thought to report on the membrane phase, were exposed to polystyrene nanoparticles, they exhibited a concentration-dependent blue shift consistent with a fluid-to-gel phase transition. However, coarse-grained simulations suggested that no such transition was taking place; instead, the simulations observed that polymer chains from the polystyrene nanoparticles penetrated into the liposome membrane. In the present work, we use all-atom molecular dynamics simulations to demonstrate that the inclusion of polystyrene within a lipid membrane causes significant changes to the local hydration and structure of that membrane while maintaining the membrane phase. Specifically, through the explicit incorporation of laurdan within the present simulations, we demonstrate that the local hydration environment of the dye molecule changes significantly but continuously as membranes are exposed to polystyrene, thus suggesting a possible explanation for the previously reported experimental observation. The present results provide a picture of the complex heterogeneity generated within polymer-containing membranes.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853953","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":"Geopolymers as a sustainable alternative to Portland cement: Synthesis, durability, applications, environmental impacts, and cost analysis","authors":"Saifurahman Zaland ,&nbsp;Junjie Wang ,&nbsp;Kefei Li ,&nbsp;Said Ikram Sadat ,&nbsp;Khalid Akhunzada","doi":"10.1016/j.rser.2025.116157","DOIUrl":"10.1016/j.rser.2025.116157","url":null,"abstract":"<div><div>Geopolymers are emerging as a sustainable alternative to ordinary Portland cement (OPC), offering reduced CO₂ emissions, excellent mechanical and durability performance, and the potential to utilize industrial byproducts. Although numerous studies have reviewed the properties of geopolymers, limited attention has been given to their durability, environmental impact, and cost analysis. This paper explores the geopolymerization process and atomic structure of geopolymers. The durability properties, cost, and environmental impacts of geopolymer concrete were comprehensively reviewed and compared with those of OPC concrete. In addition, alternative alkaline activator replacements with commercial alkaline activators have been introduced. The literature indicates that the global warming potential (GWP) of geopolymer concrete is 16 % to 90 % lower than that of OPC concrete. However, geopolymer concrete has some minor drawbacks, including higher costs and other environmental impacts. The results also reveal that using alternative activators can reduce GWP by up to 61 % and the cost of geopolymer concrete by up to 58 % compared to commercially available activators. Finally, future perspectives are outlined to address current challenges and promote the wider adoption of geopolymers in construction.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"225 ","pages":"Article 116157"},"PeriodicalIF":16.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144842674","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}