ACS Publications最新文献_第6页

α-Lipoic Acid Mediates Rapid Spiro-OMeTAD Doping for High-Performance Perovskite Solar Cells. α-硫辛酸介导高性能钙钛矿太阳能电池的快速Spiro-OMeTAD掺杂。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c13347

Jiarong Wang, Shibing Zou, Ligang Yuan, Wei Cheng, Yan Liu, Jianwu Wei, Huiming Luo, Zheng Zhang, Peng Huang, Jiaonan Sun, Keyou Yan

{"title":"α-Lipoic Acid Mediates Rapid Spiro-OMeTAD Doping for High-Performance Perovskite Solar Cells.","authors":"Jiarong Wang, Shibing Zou, Ligang Yuan, Wei Cheng, Yan Liu, Jianwu Wei, Huiming Luo, Zheng Zhang, Peng Huang, Jiaonan Sun, Keyou Yan","doi":"10.1021/acsami.5c13347","DOIUrl":"https://doi.org/10.1021/acsami.5c13347","url":null,"abstract":"The instability of 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (spiro-OMeTAD)-based n-i-p perovskite solar cells (PSCs) with lithium bis(trifluoromethane)sulfonimide doping arises from ionic shuttling and uncontrolled oxidation. Here, we introduce α-lipoic acid (LA) as a multifunctional additive to address these challenges. LA creates an acidic environment and accelerates the radical oxidation of spiro-OMeTAD, enabling the rapid formation of a stable hole transport layer while simultaneously precipitating excess Li+ ions to mitigate ion migration. Additionally, the carboxyl and disulfide groups of LA passivate interfacial defects between the perovskite and spiro-OMeTAD layers, suppressing nonradiative recombination and enhancing hole extraction. The optimized LA-doped devices achieve a power conversion efficiency (PCE) of 25.05% and show enhanced stability with a T83 of 1056 h under maximum power point (MPP) tracking, far exceeding the control's PCE of 22.54% and T80 of 528 h, respectively. This strategy not only streamlines the fabrication process by eliminating prolonged oxidation steps but also provides valuable insights into enhancing the operational stability of spiro-OMeTAD-based PSCs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038636","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}

引用次数: 0

Size Dependent Uncatalyzed Sulfite Oxidation in Aqueous Microdroplets. 粒径依赖性非催化亚硫酸盐在水微滴中的氧化作用。

IF 11.3 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-11 DOI: 10.1021/acs.est.5c01509

Kedong Gong, Sandhya Sethuraman, Adriane Tam, Zifeng Tang, V Faye McNeill, Vicki H Grassian

{"title":"Size Dependent Uncatalyzed Sulfite Oxidation in Aqueous Microdroplets.","authors":"Kedong Gong, Sandhya Sethuraman, Adriane Tam, Zifeng Tang, V Faye McNeill, Vicki H Grassian","doi":"10.1021/acs.est.5c01509","DOIUrl":"https://doi.org/10.1021/acs.est.5c01509","url":null,"abstract":"Aqueous aerosols and microdroplets exhibit unique chemical kinetics relative to the bulk phase, impacting air quality and climate via multiphase atmospheric processes. Here, we investigate uncatalyzed oxidation of sulfite to sulfate by O2 in aqueous microdroplets deposited on a superhydrophobic substrate, as a function of size, gas-phase composition, and temperature utilizing in situ micro-Raman spectroscopy. We show that the uncatalyzed sulfite oxidation is size-dependent across varying O2 concentrations and temperatures. Reaction rates scale with the surface-area to volume ratio (1/radius) of the microdroplet. We use a resistor-based approach to model multiphase mass transfer and reactions in the experimental system, confirming that the observed size-dependent kinetics reflect slow bulk kinetics coupled with an efficient reaction at the interface─k2 = 9.43 × 10-3 (+2.26 × 10-3/-2.38 × 10-3) M-1 s-1, γs,0 = 9.27 × 10-10 (+9.30 × 10-11/-1.70 × 10-10) at 298 K and 21% O2. Above a critical droplet radius, bulk kinetics dominate, but for sufficiently small atmospherically relevant sizes, rates are accelerated due to the role of the interfacial reaction. These results provide insights into chemistry in microcompartments and provide an outlook for improved representations of sulfate formation in atmospheric droplets and aerosols in large-scale atmospheric chemistry models.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038785","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}

引用次数: 0

Heavy Metal Free Ag₂Se Quantum Dot Inks for Near to Short-Wave Infrared Detection. 用于近短波红外探测的无重金属Ag2Se量子点油墨。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c12011

Shlok J Paul, Letian Li, Zheng Li, Thomas Kywe, Ana Vataj, Ayaskanta Sahu

{"title":"Heavy Metal Free Ag2Se Quantum Dot Inks for Near to Short-Wave Infrared Detection.","authors":"Shlok J Paul, Letian Li, Zheng Li, Thomas Kywe, Ana Vataj, Ayaskanta Sahu","doi":"10.1021/acsami.5c12011","DOIUrl":"https://doi.org/10.1021/acsami.5c12011","url":null,"abstract":"Infrared (IR) photodetection underpins critical applications, from environmental monitoring to national defense and autonomous navigation. Existing technologies derived from epitaxial HgCdTe and InGaAs are constrained by high cost, complex fabrication, and limited scalability. Colloidal quantum dots (cQD) such as HgTe and PbS have emerged as promising solution-processable alternatives, but their reliance on toxic heavy metals impedes broad adoption under increasingly stringent regulatory frameworks. Here, we report high-performance, heavy-metal-free Ag2Se cQD photodetectors utilizing a solution phase ligand exchange (SPLE), which produces reproducible devices through a single-step deposition, eliminating the need for multistep layer-by-layer depositions used in conventional solid-state ligand exchange approaches. The SPLE-based photoconductors exhibit responsivities of ∼150 mA/W under a 0.3 V bias in the 800-1250 nm range. We also demonstrate a self-powered photodiode achieving a specific detectivity of 6.5 × 1010 Jones at 1200 nm, with a 3 dB bandwidth of 18 kHz and sub-50 μs response times, rivaling those of other heavy-metal-free cQDs. This work positions Ag2Se cQDs as a viable, regulatory compliant alternative for near- to short-wave IR detection and offers a strategy for improving performance in larger Ag2Se cQDs active in the midwave IR regime.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038624","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}

引用次数: 0

Temperature Abetted Synthesis of Zeolitic Imidazolate Framework-Derived 3D Zn@N-C with MXene and Gold Nanostars-Based Immunosensor for the Detection of Prostate-Specific Antigen. 温度诱导下MXene和金纳米星形免疫传感器合成三维咪唑酸分子筛骨架Zn@N-C用于前列腺特异性抗原的检测。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c02634

Rajalakshmi Sakthivel, Chia-Heng Chan, Lu-Yin Lin, Subbiramaniyan Kubendhiran, Yu-Chien Lin, Ting-Yu Liu, Ren-Jei Chung

{"title":"Temperature Abetted Synthesis of Zeolitic Imidazolate Framework-Derived 3D Zn@N-C with MXene and Gold Nanostars-Based Immunosensor for the Detection of Prostate-Specific Antigen.","authors":"Rajalakshmi Sakthivel, Chia-Heng Chan, Lu-Yin Lin, Subbiramaniyan Kubendhiran, Yu-Chien Lin, Ting-Yu Liu, Ren-Jei Chung","doi":"10.1021/acsami.5c02634","DOIUrl":"https://doi.org/10.1021/acsami.5c02634","url":null,"abstract":"Prostate cancer (PC) is a malignant tumor that develops in the prostate cells of males and is the second most common cancer in men. Therefore, an early and accurate diagnosis of PC is crucial. Current diagnostic approaches are insufficient, highlighting an urgent need for alternative analytical platforms that target specific PC biomarkers in body fluids. With this instigation, we designed an environmentally friendly, disposable, and label-free electrochemical immunosensor based on gold nanostars decorated on ZIF-8-derived zinc with nitrogen-doped carbon at different temperatures (600-1000 °C) with a titanium carbide (MXene) nanosheet (AuNSs/Zn@N-C/MXene) composite modified with a screen-printed carbon electrode (SPCE) to detect prostate-specific antigen (PSA). Zn@N-C-800 °C with MXene possesses high conductivity and catalytic activity, a large surface area, and abundant active sites for PSA immunosensors. The AuNSs further enhanced the conductivity of Zn@N-C/MXene/SPCE. Cysteamine (Cys) and glutaraldehyde (Glut) were connected to the antibody (Ab) PSA to form an Ab/Glut/Cys/AuNSs/Zn@N-C-800 °C/MXene/SPCE immunosensor, which showed a direct relationship between the PSA concentration and the current response of the immunosensor. It has a linear range of 0.1 pg/mL to 1 μg/mL, with an R2 = 0.993 (n = 5; RSD <2%), and a detection limit (LOD) of 8.48 fg/mL. The resultant immunosensor was highly selective, stable, and reproducible, making it a promising tool for the early diagnosis and treatment of PC.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038633","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}

引用次数: 0

Competitive Adsorption in Polymer Nanocomposites: The Molecular Weight and End-Group Effect Revealed by SANS and MD Simulations. 聚合物纳米复合材料的竞争吸附：SANS和MD模拟揭示的分子量和端基效应。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c14834

Tae Yeon Kong, WooJin Kim, YongJoo Kim, So Youn Kim

{"title":"Competitive Adsorption in Polymer Nanocomposites: The Molecular Weight and End-Group Effect Revealed by SANS and MD Simulations.","authors":"Tae Yeon Kong, WooJin Kim, YongJoo Kim, So Youn Kim","doi":"10.1021/acsami.5c14834","DOIUrl":"https://doi.org/10.1021/acsami.5c14834","url":null,"abstract":"Understanding polymer adsorption at interfaces is essential for designing advanced polymer-based nanomaterials with tailored interfacial properties. Although adsorption significantly influences the macroscopic properties of polymer composites and thin films, a comprehensive understanding of molecular weight (MW)-dependent adsorption remains challenging and controversial, particularly in polydisperse polymer systems, due to the limitations of experimental approaches. Here, we investigate competitive adsorption in bidisperse poly(ethylene glycol) (PEG) melts and demonstrate that shorter chains preferentially adsorb onto nanoparticle surfaces. Combined experiments and molecular dynamics simulations reveal that the high density of terminal hydroxyl groups in short PEG chains strengthens hydrogen bonding at the interface, thereby inducing enthalpy-driven adsorption despite identical polymer backbones. This results in a densely packed interfacial layer that alters the conformation of longer chains. These findings highlight the critical role of end-group functionality in interfacial polymer behavior and provide new insights for tailoring nanocomposite properties.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038644","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}

引用次数: 0

Molecular Carrier-Assisted Self-Assembly of st-PMMA Helical Complexes for Fluorescence Sensing of Nitroaromatics in Aqueous Medium. 分子载体辅助st-PMMA螺旋配合物自组装用于硝基芳烃在水介质中的荧光传感。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c13301

Yu-Hao Wang, Wen-Tsung Tseng, Kuan-Yi Wu

{"title":"Molecular Carrier-Assisted Self-Assembly of st-PMMA Helical Complexes for Fluorescence Sensing of Nitroaromatics in Aqueous Medium.","authors":"Yu-Hao Wang, Wen-Tsung Tseng, Kuan-Yi Wu","doi":"10.1021/acsami.5c13301","DOIUrl":"https://doi.org/10.1021/acsami.5c13301","url":null,"abstract":"In nature, the cooperative binding of enzyme, coenzyme, and substrate forms a functional ternary complex that activates catalytic activity essential for biological functions. Inspired by this mechanism, we present a supramolecular strategy employing pyrene as a molecular carrier to facilitate the encapsulation of nonbinding nitroaromatic compounds (NACs) into the helical structure of syndiotactic poly(methyl methacrylate) (st-PMMA) via charge-transfer (CT) interactions. Structure characterization revealed that NACs and st-PMMA only form amorphous mixtures due to the weak binding affinity. In contrast, pyrene guests can coassemble with st-PMMA host to form helical complexes. Upon adding NACs to the st-PMMA/pyrene system, CT complexation between pyrene and NACs occurs readily in solution. Given the specific molecular recognition between pyrene and the st-PMMA host, pyrene can act as the carrier, enabling the pyrene-tagged NACs to be subsequently encapsulated within the st-PMMA helix during the transition to the solid state. Spectroscopic analyses confirm that the nonradiative CT complex of pyrene/NACs suppresses pyrene excimer formation in the st-PMMA helix and leads to the fluorescence quenching. Notably, owing to the dynamic nature of molecular carrier-induced self-assembly, the transparent st-PMMA/pyrene complex films demonstrate effective detection of explosive NACs in aqueous medium. Therefore, these findings establish a cooperative self-assembled strategy for modulating inclusion behavior in helical polymers, offering new avenues for advanced sensing platforms and precision-controlled molecular encapsulation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038668","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}

引用次数: 0

Quantitation by Liquid Chromatography-Nanoelectrospray Ionization-High Resolution Tandem Mass Spectrometry of Methyl and Ethyl DNA Adducts in Oral Cells from Cigarette Smokers and Nonsmokers of the Shanghai Cohort Study. 上海队列研究中吸烟者和非吸烟者口腔细胞甲基和乙基DNA加合物的液相色谱-纳米电喷雾电离-高分辨率串联质谱定量

IF 3.8 3区医学

Chemical Research in Toxicology Pub Date : 2025-09-11 DOI: 10.1021/acs.chemrestox.5c00223

Guang Cheng, Matthew W Luedtke, Renwei Wang, Jian-Min Yuan, Silvia Balbo, Stephen S Hecht

{"title":"Quantitation by Liquid Chromatography-Nanoelectrospray Ionization-High Resolution Tandem Mass Spectrometry of Methyl and Ethyl DNA Adducts in Oral Cells from Cigarette Smokers and Nonsmokers of the Shanghai Cohort Study.","authors":"Guang Cheng, Matthew W Luedtke, Renwei Wang, Jian-Min Yuan, Silvia Balbo, Stephen S Hecht","doi":"10.1021/acs.chemrestox.5c00223","DOIUrl":"https://doi.org/10.1021/acs.chemrestox.5c00223","url":null,"abstract":"We used liquid chromatography-nanoelectrospray ionization-high resolution tandem mass spectrometry (LC-NSI-HRMS/MS) to quantify DNA adducts released from human oral cell DNA upon neutral thermal hydrolysis followed by acid hydrolysis. The assay was applied to 80 buccal cell samples selected from those collected in the Shanghai Cohort Study, a prospective epidemiology study of 18,244 Chinese men 45-64 years old who resided in Shanghai, China when the samples were collected in 2001-2003. The DNA adducts quantified were 3-methyladenine (3-Me-Ade), 3-ethyladenine (3-Et-Ade), and 7-ethylguanine (7-Et-Gua). The method used hydrolysis of DNA samples containing the stable isotope labeled internal standards, solid phase extraction for adduct enrichment, and analysis by LC-NSI-HRMS/MS. Accuracy and precision of the analytical method were established with detection limits of 10-20 amol on column. Median levels of 3-Me-Ade -187 adducts/109 nucleotides in smokers and 129 adducts/109 nucleotides in nonsmokers; and 7-Et-Gua -49 adducts/109 nucleotides in smokers and 21 adducts/109 nucleotides in nonsmokers─were significantly higher in smokers than in nonsmokers (both P values <0.01). Levels of 3-Et-Ade -50 adducts/109 nucleotides in smokers and 43 adducts/109 nucleotides in nonsmokers - were not significantly different. These results demonstrate the applicability of a highly sensitive LC-NSI-HRMS/MS method for the analysis of human oral cell DNA for adducts released by neutral thermal and acid hydrolysis and show the significant effects of cigarette smoking on levels of 3-Me-Ade and 7-Et-Gua in this DNA. This is apparently the first study to characterize 3-Me-Ade in intact DNA isolated from any human tissue.","PeriodicalId":31,"journal":{"name":"Chemical Research in Toxicology","volume":" ","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Multistate Kinetic Model of the Sodium-Potassium ATPase. 钠钾atp酶的多态动力学模型。

IF 2.9 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-09-11 DOI: 10.1021/acs.jpcb.5c04069

Jose Guerra, Huan Rui, Benoît Roux

{"title":"Multistate Kinetic Model of the Sodium-Potassium ATPase.","authors":"Jose Guerra, Huan Rui, Benoît Roux","doi":"10.1021/acs.jpcb.5c04069","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c04069","url":null,"abstract":"The Na,K-ATPase is a complex membrane protein that exploits the hydrolysis of ATP as a source of chemical energy to actively transport K+ and Na+ ions against their electrochemical potential gradient across the cellular membrane. The function of this ATP-driven ion pump is broadly explained by the schematic Post-Albers alternating-access mechanism. Accordingly, the free energy gained from the phosphorylation/dephosphorylation processes, where the γ-phosphate of ATP is transferred to a conserved Asp located on a cytoplasmic domain of the protein, is used by the enzyme to interconvert between two main conformational states. As a result of experimentally determined structures at atomic resolution, a detailed Post-Albers transport cycle of Na,K-ATPase can comprise more than 20 conformational states of the system. This presents a great opportunity to formulate a detailed multistate kinetic framework model of the transport cycle of the Na,K-ATPase, displaying the thermodynamic and biophysical constraints under which it must operate. Particular attention is given to the effect of coupling to the membrane potential via incremental displacement charges for the microscopic steps of the transport cycle. On the multistate kinetic framework, a simplified continuous model of the transport cycle based on the Smoluchowski equation is formulated, and its consequences on the kinetic efficiency of the turnover rate are explored. These considerations lead to the conjecture that the free energy of the microstates of Na,K-ATPase is optimized for achieving a fast turnover rate when the membrane is depolarized.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038859","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

Versatile Polypeptide-Anchored Antifouling Dip-Coatings for Common Medical Implant Materials. 通用医用植入材料多肽锚定防污浸渍涂料。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c13513

Rahul Nisal, Jie Song

{"title":"Versatile Polypeptide-Anchored Antifouling Dip-Coatings for Common Medical Implant Materials.","authors":"Rahul Nisal, Jie Song","doi":"10.1021/acsami.5c13513","DOIUrl":"https://doi.org/10.1021/acsami.5c13513","url":null,"abstract":"Implant-associated infections represent a critical global healthcare challenge, exacerbated by recalcitrant biofilm formation and rising antimicrobial resistance. While antifouling polymer coatings could deter bacterial adhesion, common grafting methods such as surface-initiated polymerization face scalability and regulatory challenges. Dip-coating of antifouling polymers, facilitated by catechol-mediated anchorage to common medical implants, serves as a translationally appealing alternative. Although 3,4-dihydroxyphenylalanine (DOPA)-lysine-based oligopeptides were shown to exhibit mussel adhesive-like properties, they are not suitable for tethering high-molecular-weight (MW) antifouling polymers required for achieving adequate surface coverage. To facilitate unbiased screening for robust higher MW surface anchors, we synthesized a library of azide-terminated polypeptides─composed of DOPA alone or copolymerized with lysine, glutamate, or both randomly or in blocks in varying ratios─using N-carboxyanhydride ring-opening polymerization, achieving narrow polydispersity and excellent compositional control. These polypeptides were dip-coated onto Ti6Al4V and poly(ether ether ketone) substrates and conjugated with high-MW zwitterionic poly(sulfobetaine methacrylate) (pSBMA) by strain-promoted azide-alkyne cycloaddition. Using surface hydrophilicity as a readout of dip-coating efficiency and validated by X-ray photoelectron spectroscopy, we identified DOPA homopolymers as the optimal surface anchor for both substrates, significantly outperforming all copolymers containing lysine, glutamate, or both. The resulting pSBMA coatings resisted nonspecific protein adsorption or bacterial colonization and remained stable over one month in aqueous buffer at physiological pH and temperature. This DOPA homopolypeptide-mediated dip-coating strategy was also successfully extended to other implant substrates such as polyethylene terephthalate and silicone, establishing it as a potential universal implant surface modification approach.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038703","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}

引用次数: 0

Thermally Driven Wrinkle Realignment for Morphology-Controlled Enhancement of Dry Adhesion Performance. 热驱动的皱纹调整，形态学控制的干燥粘附性能的增强。

IF 8.2 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2025-09-11 DOI: 10.1021/acsami.5c15362

Yu-Fang Lai, Jui-Yuan Ho, Jun-Rong Chen, Yu-Fang Tsai, Han-Yu Hsueh

{"title":"Thermally Driven Wrinkle Realignment for Morphology-Controlled Enhancement of Dry Adhesion Performance.","authors":"Yu-Fang Lai, Jui-Yuan Ho, Jun-Rong Chen, Yu-Fang Tsai, Han-Yu Hsueh","doi":"10.1021/acsami.5c15362","DOIUrl":"https://doi.org/10.1021/acsami.5c15362","url":null,"abstract":"In this study, we developed a novel and scalable strategy for fabricating aligned wrinkle patterns through thermal expansion and contraction. Carbon nanotubes were incorporated into polydimethylsiloxane to enhance its (i.e., PDMS) heat transfer within the bilayer structure. This thermal activation enabled reversible wrinkle arrangement, allowing for the formation of highly ordered wrinkle morphologies through a purely physical process, without the need for vacuum conditions or complex precursor synthesis. The influences of geometric parameters (the sample aspect ratio and size) on wrinkle alignment were systematically investigated. We identified that the synergistic coexistence of flat regions and aligned wrinkle patterns enhances dry adhesion. The flat region increases the real contact area, whereas the wrinkled region provides mechanical interlocking and suppresses crack propagation. This study found that surface roughness, wrinkle morphology, and spatial wrinkle arrangement play critical roles in determining dry adhesion performance. In summary, this paper presents a facile, reversible, and industrially viable approach for generating functional surface patterns that can be employed in a wide range of emerging technologies.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145038715","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}

引用次数: 0