化学最新文献_第9页

Geometry Dependence of the Receding Angle of a Droplet on a Solid Cylindrical Surface

IF 3.9 2区化学

Langmuir Pub Date : 2025-04-21 DOI: 10.1021/acs.langmuir.5c00936

Mingzhu Cui, Anthony D. Dinsmore

{"title":"Geometry Dependence of the Receding Angle of a Droplet on a Solid Cylindrical Surface","authors":"Mingzhu Cui, Anthony D. Dinsmore","doi":"10.1021/acs.langmuir.5c00936","DOIUrl":"https://doi.org/10.1021/acs.langmuir.5c00936","url":null,"abstract":"Droplets that partially wet solid surfaces exhibit hysteresis in their contact angle. The values of the minimum (receding) and maximum (advancing) angles, θR and θA, are empirically well-defined and thought to be unique for a given set of materials. We measured the contact angles of water droplets hanging from hydrophobic, PDMS-functionalized glass and found that the value of θR varies with the curvature of the glass. The effect is substantial: θR changes from 86.0 ± 1.9° on a flat plate to 95.6 ± 1.9° on a 2 mm diameter rod of the same material. The measured values of θA were independent of geometry (θA = 103.2 ± 0.9°). We found a consistent trend among PDMS-functionalized glass cylinders with diameters ranging from 2 to 12.7 mm. We also measured the speed at which the contact line moved just after receding; these results showed a receding speed ∝ cos(θR) – cos(θE) and a consistent equilibrium contact angle, θE = 103.4 ± 2.3°. Finally, we measured the sliding of water droplets as rods were tilted. The larger θR (and thus smaller hysteresis) for a 2 mm-diameter rod led to droplets sliding at a tilt angle of just 21° from horizontal, compared to the 48° minimum tilt for a 7 mm rod. The results show that hysteresis arises from an energy barrier that depends on the shape of the droplet and contact line, both of which change with substrate curvature. The results may lead to designing surfaces that better trap water droplets or shed them for self-cleaning or water-harvesting applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"52 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853427","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}

引用次数: 0

Copper-Catalyzed Allylic Amination of Alkenes Using O-Acylhydroxylamines: A Direct Entry to Diverse N-Alkyl Allylamines

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-04-21 DOI: 10.1021/acscatal.5c01859

Eric J. McLaren, Guangshou Feng, Noah H. Watkins, Qiu Wang

引用次数: 0

Extending the Substrate Scope of an ω-Amine Transaminase from Aspergillus terreus by Reconstructing and Engineering an Ancestral Enzyme

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-04-21 DOI: 10.1021/acscatal.5c01779

Tingting Cai, Jie Chen, Linquan Wang, Fangfang Fan, Guo Chen, Shuai Qiu, Na Li, Lehe Mei, Jun Huang

{"title":"Extending the Substrate Scope of an ω-Amine Transaminase from Aspergillus terreus by Reconstructing and Engineering an Ancestral Enzyme","authors":"Tingting Cai, Jie Chen, Linquan Wang, Fangfang Fan, Guo Chen, Shuai Qiu, Na Li, Lehe Mei, Jun Huang","doi":"10.1021/acscatal.5c01779","DOIUrl":"https://doi.org/10.1021/acscatal.5c01779","url":null,"abstract":"Amine transaminases (ATAs) are used for synthesizing chiral amines from prochiral ketones or aldehydes through asymmetric reductive amination. However, there is still an urgent need to develop and evolve more ATAs with good performance, such as high activity, high stability, and wide substrate scope, to adapt to industrial production. Herein, a strategy of Ancestral Sequence Reconstruction-Crystal Structure Guided-Pocket Engineering (ASCP) was used to engineer R-selective ω-ATA from Aspergillus terreus (AtATA) for enhancing the thermostability and catalytic performance toward non-natural substrates. Through the ancestral sequence reconstruction (ASR) strategy, an ancestral ω-ATA (Anc101) was acquired, which showed a 10.9 °C enhancement in half-inactivation temperature (T5010) and 484-fold improvement in half-life (t1/2) at 45 °C compared with AtATA. To increase the activities of Anc101 toward non-natural substrates, the substrate binding pocket was modified based on the X-ray crystal structure of Anc101, which we solved at a resolution of 2.3 Å (PDB: 8ZM7). The best mutant Anc1016 (Anc101-H55T-E117S-R128M-V150A-L183F-L188F) showed a 133-fold improvement in catalytic activity toward 3-acetylbiphenyl as compared with Anc101. The conversions using Anc1016 toward all tested substrates were increased by 2–87% compared with Anc101. Mechanism analysis revealed that the “gate ring” covering the cavity entrance of Anc1016 was more flexible than that in Anc101, thereby increasing access of the substrates to the binding pocket. In addition, the total volume of the large and small substrate binding pockets increased. Both of these alterations contribute to the enhanced activities toward non-natural substrates of Anc1016.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"11 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853527","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

CuOTf(Tol)1/2-Catalyzed O-Trifluoroethylation of Alcohols with 2,2,2-Trifluorodiazoethane

IF 5.2 1区化学

Organic Letters Pub Date : 2025-04-21 DOI: 10.1021/acs.orglett.5c00942

Leyi Tao, Zhiyu Lei, Lianyun Zhao, Tao Ji, Yeon-Hee Lim, James Patrick Roane, Bin Hu, Xin Wen

引用次数: 0

Synergistic Regulation of Multi‐interface Chemistry by Functional Carbon Dots for High‐Performance Composite Solid Electrolytes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-21 DOI: 10.1002/anie.202505230

Huaxin Liu, Fangjun Zhu, Yinghao Zhang, Yuming Liu, Yi Zhang, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji

{"title":"Synergistic Regulation of Multi‐interface Chemistry by Functional Carbon Dots for High‐Performance Composite Solid Electrolytes","authors":"Huaxin Liu, Fangjun Zhu, Yinghao Zhang, Yuming Liu, Yi Zhang, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji","doi":"10.1002/anie.202505230","DOIUrl":"https://doi.org/10.1002/anie.202505230","url":null,"abstract":"Low ionic conductivity, poor mechanical strength and unstable interface structure are still the main factors hindering the practical application of polymer solid‐state lithium metal batteries (SSLMBs). In this work, we have developed a unique composite filler (LLZTOCDs) for solid polymer electrolytes to address these challenges through synergistic regulation of multi‐interface chemistry. The LLZTOCDs is prepared via thermal treatment of N, S, F‐codoped carbon dots (NSFCDs) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO) inorganic electrolyte, here the detrimental Li2CO3 on the LLZTO surface is converted into a fast ion‐conducting and an electron‐insulating interlayer of LiF and Li3N, and the carbon dots self‐assemble into a functional organophilic coating on the outermost layer, which acts as a bridge between the LLZTO and the polymer. This unique structure enhances the compatibility and ion‐exchange kinetics between the LLZTOCDs and the polymer, significantly improving the mechanical strength and Li+ transport. Additionally, the oxygen vacancies formed in‐situ at the LLZTOCDs interface provide an anion confinement effect, increasing lithium salt dissociation and enhancing the Li+ transference number to 0.85. Therefore, the solid battery constructed with LLZTOCDs exhibits excellent electrochemical stability, long‐cycle life, and high ionic conductivity (1.96 × 10−4 S cm‐1 at 25 °C), providing a feasible strategy for practical applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853601","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

Stimuli-responsive metal-free phosphorescent materials: From design and mechanisms to emerging applications

IF 20.3 1区化学

Coordination Chemistry Reviews Pub Date : 2025-04-21 DOI: 10.1016/j.ccr.2025.216734

Hao Qiu , Youquan Yan , Heng Zhou, Zhenhua Gao, Shiwei Chen, Chaofeng Zhu, Zifei Wang

{"title":"Stimuli-responsive metal-free phosphorescent materials: From design and mechanisms to emerging applications","authors":"Hao Qiu , Youquan Yan , Heng Zhou, Zhenhua Gao, Shiwei Chen, Chaofeng Zhu, Zifei Wang","doi":"10.1016/j.ccr.2025.216734","DOIUrl":"10.1016/j.ccr.2025.216734","url":null,"abstract":"<div><div>Stimuli-responsive room-temperature phosphorescence (RTP) material hold great potential for diverse optoelectronic applications due to their high sensitivity and rapid response. Among these, metal-free RTP systems have emerged as a particularly promising research focus, attributed to their advantageous properties, such as low toxicity, excellent biocompatibility, and ease of processing. Despite the significant strides made in this dynamic field, a comprehensive review that consolidates the latest breakthroughs remains conspicuously absent. In this review, we highlight recent advancements in stimuli-responsive metal-free RTP materials, including organic molecules, polymers, carbon dots, and biomass. We discuss their intricate design strategies, dynamic behaviors under various external stimuli, and stimuli-responsive mechanisms, along with their potential applications in the fields of information security, sensing, bioimaging, and smart optical devices. Additionally, we present a range of perspectives that emphasize the current challenges and promising future opportunities associated with stimuli-responsive metal-free RTP materials across various domains. We anticipate that this review will offer valuable insights and guidelines to inspire more innovative research on stimuli-responsive metal-free RTP systems, thereby promoting the further development of smart luminescent materials and their multifunctional applications.</div></div>","PeriodicalId":289,"journal":{"name":"Coordination Chemistry Reviews","volume":"538 ","pages":"Article 216734"},"PeriodicalIF":20.3,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143851955","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

Synthesis of polymer-grafted thermally reduced graphene oxide by RAFT polymerization and their effects on properties of cured unsaturated polyester resins. II. Volume shrinkage, mechanical properties, thermal conductivity, and surface resistivity

IF 2.6 4区化学

Journal of Polymer Research Pub Date : 2025-04-21 DOI: 10.1007/s10965-025-04376-2

Rong-Woei Chang, Yeong-Jenq Wang, Jy-Ning Yang, Yan-Jyi Huang

{"title":"Synthesis of polymer-grafted thermally reduced graphene oxide by RAFT polymerization and their effects on properties of cured unsaturated polyester resins. II. Volume shrinkage, mechanical properties, thermal conductivity, and surface resistivity","authors":"Rong-Woei Chang, Yeong-Jenq Wang, Jy-Ning Yang, Yan-Jyi Huang","doi":"10.1007/s10965-025-04376-2","DOIUrl":"10.1007/s10965-025-04376-2","url":null,"abstract":"<div>Effects of concentration (0–0.5 wt%) and type of thermally reduced graphene oxide (TRGO) and diblock copolymer-grafted TRGO, namely, TRGO-g-poly(butyl acrylate)-b-poly(methyl acrylate-co-glycidyl methacrylate) (TRGO-Gx-yK) with GMA compositions in P(MA-co-GMA) at 10 or 20 mol% (x = 10 or 20) and Mn for grafted polymer PBA-b-P(MA-co-GMA) at 30 K, 17 K, or 8 K (y = 30, 17, or 8), as low-profile additives (LPA) for unsaturated polyester resins (UP), on cured sample morphologies and properties of low-shrink UP after cure at 110 °C have been investigated. The decreasing order of compatibility for styrene (St)/UP/TRGO-polymer system before reaction, as predicted by the molecular polarity difference per unit volume between UP and grafted polymer of TRGO-polymer, showed that TRGO-Gx- 8 K > TRGO-Gx- 17 K > TRGO-Gx- 30 K, and TRGO-G20-yK > TRGO-G10-yK. The trend was in agreement with that of decreasing mutual miscibility of St/UP/TRGO-polymer system after cure at 110 °C, as observed from SEM and TEM micrographs. Adding 0.5 wt% of TRGO-polymer with Mn = 8000 for PBA-b-P(MA-co-GMA) and 20 mol% GMA in P(MA-co-GMA) as LPA can lead to a decrease of volume shrinkage by 64%, an increase of Young’s modulus by 12%, a slight decrease of tensile strength by 9%, a decrease of impact strength by 14%, an increase of thermal conductivity by 22%, and a decrease of surface resistivity by 99.9%, when compared with that of neat St/UP cured system. All properties depended on Mn and GMA composition for grafted polymer onto TRGO, and followed the decreasing order of TRGO-Gx- 8 K > TRGO-Gx- 17 K > TRGO-Gx- 30 K and TRGO-G20-yK > TRGO-G10-yK > TRGO.</div>","PeriodicalId":658,"journal":{"name":"Journal of Polymer Research","volume":"32 5","pages":""},"PeriodicalIF":2.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10965-025-04376-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143852531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Enhancing the performance of fused filament fabricated ABS through carbon fiber reinforcement: a study on structural integrity and material behavior

IF 2.6 4区化学

Journal of Polymer Research Pub Date : 2025-04-21 DOI: 10.1007/s10965-025-04387-z

Sovan Sahoo, Subhash Chandra Panja, Debashis Sarkar

{"title":"Enhancing the performance of fused filament fabricated ABS through carbon fiber reinforcement: a study on structural integrity and material behavior","authors":"Sovan Sahoo, Subhash Chandra Panja, Debashis Sarkar","doi":"10.1007/s10965-025-04387-z","DOIUrl":"10.1007/s10965-025-04387-z","url":null,"abstract":"<div>The mechanical properties of components manufactured via fused filament fabrication (FFF) are generally lower than those of injection-molded parts due to the layer-by-layer deposition process and its reliance on interlayer diffusion. Fiber reinforcement offers a potential solution by improving strength, but its influence extends beyond mechanical performance. Despite extensive research, a significant gap remains in understanding interlayer diffusion, mechanical anisotropy, and the thermal and surface effects of fiber reinforcement in FFF composites. This study examines the effects of 10 wt% carbon fiber (CF) reinforcement in acrylonitrile butadiene styrene (ABS) on interlayer diffusion across varying layer thicknesses and its influence on mechanical properties. Increasing the layer thickness from 0.18 mm to 0.34 mm in pure ABS raises pore density from 3.35% to 11.20%, significantly reducing tensile strength. In contrast, ABS-CF composites exhibit a 41.98% average increase in tensile strength and reduced sensitivity to layer thickness variations. Anisotropy analysis, further incorporating raster angle and build orientation, shows a reduction in tensile strength and strain variation by 57.32% and 78.09%, respectively, indicating improved mechanical consistency. Furthermore, ABS-CF demonstrates enhanced thermal stability, with increased thermal expansion of deposited strands promoting interlayer diffusion. This not only improves mechanical performance but also results in distinct surface characteristics, where overall surface roughness remains comparable or lower, yet individual layer-level roughness rises by 57.30%. Additionally, surface hardness improves by 26.67%. However, these enhancements come with a transition from ductile to brittle failure, likely due to non-uniform fiber distribution and thermal mismatch between ABS and CF during fabrication.</div>","PeriodicalId":658,"journal":{"name":"Journal of Polymer Research","volume":"32 5","pages":""},"PeriodicalIF":2.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143852532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Molecular Modeling, Cheminformatics Analysis, and Synthesis of Trifluoromethylated Aromatic Sulfonamides as Putative Inhibitors of Cholesteryl Ester Transfer Protein

IF 1.9 4区化学

ChemistrySelect Pub Date : 2025-04-21 DOI: 10.1002/slct.202405697

Reema Abu Khalaf, Rawan Hamadah, Nataly Abu Ajamieh, Rima Hajjo, Mahmoud Al-Sha'er, Dima Sabbah

{"title":"Molecular Modeling, Cheminformatics Analysis, and Synthesis of Trifluoromethylated Aromatic Sulfonamides as Putative Inhibitors of Cholesteryl Ester Transfer Protein","authors":"Reema Abu Khalaf, Rawan Hamadah, Nataly Abu Ajamieh, Rima Hajjo, Mahmoud Al-Sha'er, Dima Sabbah","doi":"10.1002/slct.202405697","DOIUrl":"https://doi.org/10.1002/slct.202405697","url":null,"abstract":"Elevated lipid profile is a major risk factor for diseases like dyslipidemia. Cholesteryl ester transfer protein (CETP) inhibitors are explored for their potential to raise HDL and lower LDL, offering a promising approach to reducing cardiovascular risk. In this study, a series of ortho- and meta-trifluoromethylated sulfonamides 6a-6t were synthesized and evaluated for their CETP inhibitory activity at 10 µM concentration. Compounds 6a-6t featured various aromatic substituents, positioned at different sites. Results revealed that compound 6f demonstrated the highest inhibitory efficacy, achieving a 100% inhibition. CETP inhibition was compared to computational models Hypo-1 and Hypo-1-shaped to predict potential biological efficacy. The findings indicate that electron-withdrawing groups, particularly Cl and NO₂, significantly enhance CETP inhibitory potency, especially when located at the ortho or meta positions. These compounds exhibited a strong correlation between Hypo-1 activity and % inhibition, suggesting improved interaction with CETP. In contrast, methyl electron-donating substitutions resulted in lower activity, indicating their inadequacy for this scaffold. Further cheminformatics analyses based on molecular descriptors indicated that 6f has enhanced lead-like and drug-like properties in comparison to the second most potent compound 6i (82%). Developing new compounds with CETP inhibitory properties shows promise for future interventions to regulate lipid profiles.","PeriodicalId":146,"journal":{"name":"ChemistrySelect","volume":"10 16","pages":""},"PeriodicalIF":1.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143852786","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Facile, Metal-free, Highly Para-Selective Room Temperature Monobromination of Aniline Analogs

IF 1.9 4区化学

ChemistrySelect Pub Date : 2025-04-21 DOI: 10.1002/slct.202500544

Dr. Pakorn Bovonsombat, Amber Hocks, Phutawan Kittithanaluk, Jing Ting We, Pratheep Khanthapura, Dr. Sirirat Choosakoonkriang, Nattawadee Srikamhom, Fahsai Ploymanee

引用次数: 0