ACS Applied Materials & Interfaces最新文献

{"title":"Optimizing Ligand Valency to Maximize Tendon Accumulation of Peptide-Targeted Nanoparticles.","authors":"Emmanuela Adjei-Sowah, Vigneshkumar Rangasami, Alayna E Loiselle, Danielle S W Benoit","doi":"10.1021/acsami.4c13388","DOIUrl":"10.1021/acsami.4c13388","url":null,"abstract":"<p><p>In many tissues, including musculoskeletal tissues such as tendon, systemic delivery typically results in poor targeting of free drugs. Hence, we previously developed a targeted drug delivery nanoparticle (NP) system for tendon healing, leveraging a tartrate resistant acid phosphatase (TRAP) binding peptide (TBP) ligand. The greatest tendon targeting was observed with NPs functionalized with 30 000 TBP ligands per NP at day 7 during the proliferative healing phase, relative to the inflammatory (day 3) and early remodeling (day 14) phases of healing. Nevertheless, TRAP activity varies throughout healing and, therefore, may offer an opportunity for optimizing temporal therapeutic targeting through multivalent interactions. Hence, in this study, we hypothesized that the ligand density (9000-55,000 TBPs per NP) can optimize tendon accumulation on the basis of variable TRAP levels. The multivalent nanoparticles were loaded with three different fluorophores. In vitro, the ligand density and fluorophore had no effect on the physicochemical properties of the NPs, including size, charge, polydispersity index, or dye loading efficiency; however, the TRAP binding affinity correlated positively with the ligand density. In vivo, the ligand density correlated positively with NP homing and retention in the tendon, establishing opportunities to leverage ligand density for tendon targeting across the tendon healing cascade, during aging, and in other tendon pathologies, including tendinopathies.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"68864-68876"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142764552","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":"Cuboidal Deformation of Multimaterial Composites Prepared by 3-D Printing of Liquid Crystalline Elastomers.","authors":"Joselle M McCracken, Grant E Bauman, Graham Williams, Misael Santos, Lawrence Smith, Robert MacCurdy, Timothy J White","doi":"10.1021/acsami.4c14792","DOIUrl":"10.1021/acsami.4c14792","url":null,"abstract":"<p><p>Multimaterial 3-D printing (3DP) of isotropic (IsoE) and liquid crystalline elastomers (LCE) yields spatially programmed elements that undergo a cuboidal shape transformation upon heating. The thermomechanical deformation of 3DP elements is determined by the geometry and extent of the isotropic and anisotropic regions. The synthesis and experimental characterization of the 3DP elements are complemented by finite element analysis (FEA). Calculations emphasize that the cuboidal deformation of the myriad 3DP elements is a manifestation of local stress gradients imparted by local control of the material composition and anisotropy. Varying the rectilinear spatial distribution of the multimaterial elastomer composites produces complex, multistable states that provide insights into how stress gradients drive multimaterial elastomer actuation. The thermomechanical stimuli response of the multimaterial elements is explored as a tactile element.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69851-69857"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778703","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":"MoS₂-Based NH₃ Sensor for In Situ <i>Helicobacter pylori</i> Detection.","authors":"Minmin Zhao, Zhu Zhang, Chao Tan, Wei Wang, Lei Yang, Zegao Wang","doi":"10.1021/acsami.4c18702","DOIUrl":"10.1021/acsami.4c18702","url":null,"abstract":"<p><p>Detection of <i>Helicobacter pylori</i> is essential for the prevention of gastric cancer. By detecting the metabolized NH₃, it was able to noninvasively reveal the state of <i>H. pylori</i>; however, it is still a challenge since the metabolized NH₃ concentration is much lower for conventional gas sensors. Herein, we developed a MoS₂-based NH₃ sensor for continuous, real-time monitoring of <i>H. pylori</i> growth. The atomic thin layer and the all-exposed surface of MoS₂ facilitate NH₃ adsorption and charge transferring. A high-response NH₃ sensor was prepared by surface decoration of MoS₂ by depositing metal nanoparticles. The Fe-decorated MoS₂ sensor outperformed with a high response of 40.9% for 5.7 ppm of NH₃ at 25 ± 2 °C, low LOD (6.2 ppb), and long-term stability with a response of 12.5% for 5.7 ppm of NH₃ after 5 months. The Fe-decorated MoS₂ sensor was applied to the detection of <i>H. pylori</i> and the real-time in situ monitoring of its 92 h growth cycle. The NH₃ release curve of the exponential phase during <i>H. pylori</i> growth was continuously monitored, and the NH₃ concentration was quantified. The maximum specific rate of NH₃ release was 0.195 ± 0.005 h^-1, which is well-consistent with the nature of <i>H. pylori</i> growth. This study opens up a technological roadmap for noninvasive detection of <i>H. pylori</i> in the future.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69798-69806"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778736","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":"Nondestructive Testing of Polymer Aging Based on Room-Temperature Phosphorescence.","authors":"Qiankun Li, Xia Huang, Hui Hou, Fengling Guo, Xiaojuan Wang, Meiyi He, Yongkang Wang, Yushuang Zhang, Lunjun Qu, Kaiti Wang, Youbing Li, Liyan Liang, Chaolong Yang","doi":"10.1021/acsami.4c16249","DOIUrl":"10.1021/acsami.4c16249","url":null,"abstract":"<p><p>Polymeric room-temperature phosphorescence (RTP) materials have attracted much attention due to their advantages of easy processing and excellent luminescent properties. However, it is still a challenge to obtain industrial production grade material through simple and green processing strategies. Herein, through the codoping strategy, different phosphors were embedded into nylon, a kind of polymer matrix, to obtain a series of highly efficient RTP materials without any organic solvents, for which the phosphorescence lifetime and brightness could reach 628.8 ms and 14 cd/m², respectively. Besides, we found that the photophysical properties of these RTP materials varied greatly among different types of nylon matrix, owing to the divergence in the number of hydrogen bonding \"sites\". The superiority of the injection molding processing strategy enables the preparation of RTP materials to achieve desolvation, which could also be processed into any complex and desiring shape. Significantly, nylon can affect molecular chain changes due to aging and other problems, so that these RTP materials are considered as potential nondestructive testing for nylon product aging levels. This strategy also paves the way for the development of large-scale, eco-friendly, and practical application RTP materials and provides new ideas to industrialized preparation of long-lived RTP materials in the future.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69891-69900"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793930","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":"Optical Centers in Cr-, Mn-, and O-Doped AlN and Their Thermodynamic Stability Designed by a Multiscale Computational Approach.","authors":"Mubashir Mansoor, Mehmet Ali Sarsil, Mehya Mansoor, Maryam Mansoor, Mert Tas, Yahya Sorkhe, Zuhal Er, Katarzyna Jabłczyńska, Bora Derin, Servet Timur, Mustafa Ürgen, Onur Ergen, Kamil Czelej","doi":"10.1021/acsami.4c12726","DOIUrl":"10.1021/acsami.4c12726","url":null,"abstract":"<p><p>The optical centers in AlN can frequently exist in various charge states and can be accompanied by many coexisting defect species, creating a complex environment where mutual interactions are inevitable. Therefore, it is an immediate quest to design AlN crystal growth protocols that can target a specific optical center of interest and tune its concentration while preventing the formation of other unwanted point defects. Here, we provide a powerful workflow for point defect engineering in wide band gap, binary semiconductors that can be readily used to design optimal crystal growth protocols through combining CALPHAD-based phase analysis, and <i>ab initio</i> defect calculations. We investigate technologically relevant chromium- and manganese-induced optical centers in AlN, followed by studying the impact of oxygen that can be unintentionally incorporated during crystal growth. We present the dominant defects in all three cases as a function of process parameters along with the optical signatures. In the case of both Cr and Mn doping, the Cr_Al and Mn_Al defects are most likely, and increasing nitrogen partial pressure tends to enhance their concentration. We show that it is possible to use nitrogen fugacity as a tool for tuning the intensity of optical signatures. We calculate the Cr_Al charge transition levels with respect to the valence-band maximum at 2.60 eV (<i>E</i>^<i>+</i>/-), 3.83 eV (<i>E</i>^0/-), and 5.41 eV (<i>E</i>^-<i>/2</i>-) and electron and hole capture transitions with luminescence bands centered at 2.82, 1.91, and 3.15 eV. Unlike the Cr doping, Mn aggregation is unlikely, and the Mn_Al-V_N is the most abundant defect after Mn_Al under most synthesis conditions. Oxygen tends to form complexes with V_Al, and O_N-V_Al is a prominent defect following O_N, with near-UV emission bands at 3.17, 3.26, and 3.81 eV. Our results agree with the available experimental optical signatures of Cr-, Mn-, and O-related centers and provide pathways on how to tune the luminous intensity of these centers through changes in growth conditions.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69529-69547"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142794025","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":"Biomimetic Metallacage Nanoparticles with Aggregation-Induced Emission for NIR-II Fluorescence Imaging-Guided Synergistic Immuno-Phototherapy of Tumors.","authors":"Jingpei Zhang, Wei Ma, Boyu Yang, Tingyu Shi, Shenglong Liao, Yang Li, Shouchun Yin","doi":"10.1021/acsami.4c17413","DOIUrl":"10.1021/acsami.4c17413","url":null,"abstract":"<p><p>The integration of theranostics, which combines diagnostics with therapeutics, has markedly improved the early detection of diseases, precise medication management, and assessment of treatment outcomes. In the realm of oncology, organoplatinum-based supramolecular coordination complexes (SCCs) that can coload therapeutic agents and imaging molecules have emerged as promising candidates for multimodal theranostics of tumors. To address the challenges of tumor-targeted delivery and multimodal theranostics for SCCs, this study employs a cell membrane cloaking strategy to fabricate biomimetic metallacage nanoparticles (MCNPs) with multimodal imaging capabilities and homologous targeting capabilities. Specifically, a photosensitizer molecule (BTTP) containing AIE-active groups was assembled into a metallacage of C-BTTP through Pt-N coordination. This process endows the metallacage with strong NIR-II fluorescence in the aggregated state and significantly superior ROS generation compared to that of the precursor ligand. After being encapsulated with F127, the MCNPs were further cloaked with U87 cancer cell membranes, creating biomimetic MCNPs that achieve tumor-targeting capabilities. Verified by in vitro and in vivo experiments, MCNPs enable multimodal imaging and initiate immunotherapy under photothermal and photodynamic stimulation, leading to synergistic antitumor effects. Furthermore, the evaluation of immunogenic cell death and dendritic cell maturation rate in U87 tumor-bearing mice confirmed the mechanism of photothermal and photodynamic synergistic immunotherapy. This study provides an innovative strategy for enhancing the tumor-targeting and therapeutic efficiency of SCCs, offering a versatile strategy for efficient and minimally invasive theranostics of tumors. The development of such biomimetic nanoparticles represents a significant advancement in the field of nanomedicine, potentially transforming cancer treatment through personalized and targeted therapies.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69028-69044"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778694","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":"Thermal Rectification in Telescopic Nanowires: Impact of Thermal Boundary Resistance","authors":"Yashpreet Kaur, Saeko Tachikawa, Milo Yaro Swinkels, Miquel López-Suárez, Matteo Camponovo, Alicia Ruiz Caridad, Wonjong Kim, Anna Fontcuberta i Morral, Riccardo Rurali, Ilaria Zardo","doi":"10.1021/acsami.4c14920","DOIUrl":"https://doi.org/10.1021/acsami.4c14920","url":null,"abstract":"A thermal diode, which, by analogy to its electrical counterpart, rectifies heat current, is the building block for thermal circuits. To realize a thermal diode, we demonstrate thermal rectification in a GaAs telescopic nanowire system using the thermal bridge method. We measured a preferred direction of heat flux, achieving rectification values ranging from 2 to 8% as a function of applied thermal bias. We demonstrate that the thermal boundary resistance between the thin part with the wurtzite crystal phase and the thick part with the zinc-blende crystal phase of the telescopic nanowire plays a crucial role in determining the amount and direction of heat flux rectification. This effect is confirmed by numerical solutions of the one-dimensional heat equation based on ab initio data. Additionally, we accounted for the effect of the thermal contact resistance. This work is the first experimental indication of rectification using a telescopic nanowire where we reveal the importance and role of the thermal boundary resistance in determining thermal rectification.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"28 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849757","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":"Analysis of Tribological and Cytotoxicity Assays of a Biocompatible Mg–Zn–Ca–Pr Alloy","authors":"Sabina Lesz, Julia Popis, Barbara Grzegorczyk, Aleksandra Drygała, Bartłomiej Hrapkowicz, Wojciech Pakieła, Dariusz Ozimina, Julia Lisoń-Kubica, Klaudiusz Gołombek, Dariusz Garbiec, Marcin Basiaga","doi":"10.1021/acsami.4c13285","DOIUrl":"https://doi.org/10.1021/acsami.4c13285","url":null,"abstract":"This work covers a Mg–Zn–Ca–Pr alloy fabricated by a novel method of mechanical alloying and spark plasma sintering (SPS). Currently, magnesium alloys used as biomaterials are mostly commercial alloys without consideration of cytotoxicity from the perspective of biosafety. So far, the tribological and cytotoxic properties of Mg–Zn–Ca–Pr alloys have not been investigated. Hence, in the article, the tribological properties, considering wear rate, wear resistance, coefficient of friction, and the roughness of the sintered Mg–Zn–Ca–Pr alloy, are investigated. Cytotoxicity assays have also been carried out. The ball-on-a-disc method is used in the tribological test. Samples before sintering by the SPS method are milled at varying times of 13, 20, and 70 h. Results show that increasing the milling time affects tribology and cytotoxic tests. The longer the milling time, the lower the cell survival rate. The conducted tests reveal cell survival of 90, 82, and 61% for 13, 20, and 70 h, respectively. A reduction of cell viability by over 30% is considered a cytotoxic effect, which was observed only in the 70 h milling-time samples.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"31 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849755","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":"Study on the Effect of Temperature and Pressure Environments on the Mechanical and Electronic Properties of Titanium Carbon Nitride Ceramics","authors":"Yi Qin, Zhengang Zhang, Wenjia Liang, Yi Tian, Jianyi Ma","doi":"10.1021/acsami.4c16864","DOIUrl":"https://doi.org/10.1021/acsami.4c16864","url":null,"abstract":"As a high-performance cermet, TiCN possesses extensive potential for application in various fields, including coating materials, ceramic products, and electronic materials. Here, the effects of temperature and pressure on the physical properties of the TiCN cermet have been investigated by high-pressure techniques and first-principles calculations. Experimentally, the phase, microstructure, mechanical properties, and electrical conductivity of bulk TiCN ceramics were analyzed. In high-pressure sintering, the sintering temperature rhythmically regulated the porosity and grain size within the ceramics. The TiCN prepared at 5.5 GPa/1200 °C has a Vickers hardness of ∼23.81 GPa, a Young’s modulus of 445.24 GPa, and an electrical conductivity of ∼(20.4 ± 0.55) × 10⁵ S/m. Moreover, the responses of the mechanical and electronic properties of TiCN to pressure were evaluated by first-principles, which matched the experimental results. The research findings have revealed that the pressure effects work not only on the microstructure and mechanical properties but also on the atoms and electrons. The study integrates both theoretical and experimental approaches to enhance our comprehension of the microstructure and physical properties of TiCN ceramics, insights that are instrumental in broadening the application scope of TiCN-based ceramic materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"20 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849779","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":"Microwave-Driven Reduction Accelerates Oxygen Exchange in Perovskite Oxides.","authors":"Aitor Domínguez-Saldaña, Alfonso J Carrillo, María Balaguer, Laura Navarrete, Joaquín Santos, David Catalán-Martínez, Beatriz García-Baños, Pedro J Plaza-González, José D Gutierrez-Cano, Felipe Peñaranda, José Manuel Catalá-Civera, José Manuel Serra","doi":"10.1021/acsami.4c15150","DOIUrl":"10.1021/acsami.4c15150","url":null,"abstract":"<p><p>Microwave-assisted oxide reduction has emerged as a promising method to electrify chemical looping processes for renewable hydrogen production. Moreover, these thermochemical cycles can be used for thermochemical air separation, electrifying the O₂ generation by applying microwaves in the reduction step. This approach offers an alternative to conventional cryogenic air separation, producing pure streams of O₂ and N₂. The electrification by microwaves lowers the requirements for titanate perovskites (CaTi_1-<i>x</i>Mn_<i>x</i>O_3-δ), which typically demand high temperatures for thermochemical cycles. Microwave activation allows for a drastic reduction in the operation conditions of the reduction reaction, leading to unprecedentedly rapid absorption-desorption cycles (<3 min per cycle). For CaTi_0.8Mn_0.2O_3-δ, we achieved a cycle-averaged O₂ production of 2.6 mL g^-1 min^-1 at 800 °C, surpassing conventional values of materials operating in the high-temperature regime. This method could significantly impact thermochemical air separation by enabling a faster oxygen absorption-desorption cycle at more moderate temperatures than those of conventionally heated processes.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":"69324-69332"},"PeriodicalIF":8.3,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778717","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}