Sakti Prasanna Muduli, Rama Chandra Muduli, Paresh Kale
Solid-state hydrogen storage outperforms conventional storage methods in terms of safety and on-board applications. Porous Si (PS) is the optimized Si nanostructure with ample surface area (∼400 m2 g–1) and maximum dangling sites for hydrogenation. Though solid-state hydrogen storage in Si nanostructures, especially in porous Si, is extensively studied, the thermal desorption of hydrogen is rarely reported. This work investigates and analyzes the thermal desorption of a hydrogen-terminated PS surface using attenuated total reflectance–Fourier transform infrared spectroscopy (ATR-FTIR) to optimize the temperature for efficient desorption, as FTIR is sensitive to identifying the presence of Si hydride species (SiHx). The relative peak intensities in the spectra estimate the relative hydrogen retention (γ) for the analysis of the desorption kinetics. The desorption curves are divided into two zones on the time scale: the excitation zone and the recombination zone, separated by the recombination threshold point. The initially absorbed energy breaks the Si–Hx bonds in the excitation zone to reach the recombination threshold for H2 formation. The recombination zone is further divided into two subzones: the avalanche subzone (a sudden decrease in γ indicating molecular desorption) and the saturation subzone (almost constant γ with minimal desorption). The time constant from the first-order reaction kinetic fitting of the desorption curves explores the time–temperature correlation and the barrier energy estimation for the excitation and recombination zones. The analysis identifies the critical operating point for desorption as 100 °C and 4 min, with the optimized temperature of 250 °C. This article applies an analogous electrical circuit to compare the thermal hydrogen desorption and capacitor discharge circuit for analytical convenience.
{"title":"Decoding Hydrogen Desorption Kinetics in Porous Silicon: An Electrical Circuit Modeling Approach","authors":"Sakti Prasanna Muduli, Rama Chandra Muduli, Paresh Kale","doi":"10.1021/acsami.4c11255","DOIUrl":"https://doi.org/10.1021/acsami.4c11255","url":null,"abstract":"Solid-state hydrogen storage outperforms conventional storage methods in terms of safety and on-board applications. Porous Si (PS) is the optimized Si nanostructure with ample surface area (∼400 m<sup>2</sup> g<sup>–1</sup>) and maximum dangling sites for hydrogenation. Though solid-state hydrogen storage in Si nanostructures, especially in porous Si, is extensively studied, the thermal desorption of hydrogen is rarely reported. This work investigates and analyzes the thermal desorption of a hydrogen-terminated PS surface using attenuated total reflectance–Fourier transform infrared spectroscopy (ATR-FTIR) to optimize the temperature for efficient desorption, as FTIR is sensitive to identifying the presence of Si hydride species (SiH<sub><i>x</i></sub>). The relative peak intensities in the spectra estimate the relative hydrogen retention (γ) for the analysis of the desorption kinetics. The desorption curves are divided into two zones on the time scale: the excitation zone and the recombination zone, separated by the recombination threshold point. The initially absorbed energy breaks the Si–H<sub><i>x</i></sub> bonds in the excitation zone to reach the recombination threshold for H<sub>2</sub> formation. The recombination zone is further divided into two subzones: the avalanche subzone (a sudden decrease in γ indicating molecular desorption) and the saturation subzone (almost constant γ with minimal desorption). The time constant from the first-order reaction kinetic fitting of the desorption curves explores the time–temperature correlation and the barrier energy estimation for the excitation and recombination zones. The analysis identifies the critical operating point for desorption as 100 °C and 4 min, with the optimized temperature of 250 °C. This article applies an analogous electrical circuit to compare the thermal hydrogen desorption and capacitor discharge circuit for analytical convenience.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486688","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}
Isabella A. Kalluvila Justin, David O. Tiede, Manuel Piot, Michele Forzatti, Cristina Roldán-Carmona, Juan F. Galisteo-López, Hernán Míguez, Henk J. Bolink
Herein, we demonstrate that coevaporated dopants provide a means to passivate buried interfacial defects occurring at perovskite grain boundaries in evaporated perovskite thin films, thus giving rise to an enhanced photoluminescence. By means of an extensive photophysical characterization, we provide experimental evidence that indicate that the codopant acts mainly at the grain boundaries. They passivate interfacial traps and prevent the formation of photoinduced deep traps. On the other hand, the presence of an excessive amount of organic dopant can lead to a barrier for carrier diffusion. Hence, the passivation process demands a proper balance between the two effects. Our analysis on the role of the dopant, performed under different excitation regimes, permits evaluation of the performance of the material under conditions more adapted to photovoltaic or light emitting applications. In this context, the approach taken herein provides a screening method to evaluate the suitability of a passivating strategy prior to its incorporation into a device.
{"title":"Strong Grain Boundary Passivation Effect of Coevaporated Dopants Enhances the Photoemission of Lead Halide Perovskites","authors":"Isabella A. Kalluvila Justin, David O. Tiede, Manuel Piot, Michele Forzatti, Cristina Roldán-Carmona, Juan F. Galisteo-López, Hernán Míguez, Henk J. Bolink","doi":"10.1021/acsami.4c13434","DOIUrl":"https://doi.org/10.1021/acsami.4c13434","url":null,"abstract":"Herein, we demonstrate that coevaporated dopants provide a means to passivate buried interfacial defects occurring at perovskite grain boundaries in evaporated perovskite thin films, thus giving rise to an enhanced photoluminescence. By means of an extensive photophysical characterization, we provide experimental evidence that indicate that the codopant acts mainly at the grain boundaries. They passivate interfacial traps and prevent the formation of photoinduced deep traps. On the other hand, the presence of an excessive amount of organic dopant can lead to a barrier for carrier diffusion. Hence, the passivation process demands a proper balance between the two effects. Our analysis on the role of the dopant, performed under different excitation regimes, permits evaluation of the performance of the material under conditions more adapted to photovoltaic or light emitting applications. In this context, the approach taken herein provides a screening method to evaluate the suitability of a passivating strategy prior to its incorporation into a device.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486821","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}
Xinyan Yue, Xiaohu Wang, Jianbo Shao, Huabing Wang, Yu Chen, Kun Zhang, Xiao Han, Jianhan Hong
Flexible capacitive sensors have attracted the attention of researchers owing to their simple structure, ease of realization, and wearability. Currently, flexible capacitive sensors mainly have three-dimensional and two-dimensional structures, which are subject to several limitations in their applications. A low-cost, high-efficiency, and continuously processable process was used to wrap nylon DTY (PA) filaments on the surface of silver-coated nylon (SCN) core yarns and impregnate them with waterborne polyurethane (WPU) to obtain SCN/PA/WPU composite yarns, which were then utilized in the design of SCN/PA/WPU for the preparation of one-dimensionally structured flexible capacitive sensors. The morphology and mechanical properties of the SCN core yarn, SCN/PA wrapped yarn, and SCN/PA/WPU composite yarn were characterized. The strain-sensing performance of the sensor was analyzed, and the sensor was used to monitor human physiological activities. The sensor exhibited excellent strain capacitance sensing performance with a strain range of up to 140%. With a gauge factor of 0.66 at 10% tensile strain, it can detect strains as low as 1% and has good repeatability, withstanding more than 3200 tensile-unload cycles at 80% strain. The one-dimensional structure sensor can be used to monitor the large-scale movements of joints and muscles in various parts of the human body and the physiological signals of tiny human movements, such as breathing, coughing, and facial expressions, which have potential applications in the fields of sports monitoring and smart wearable.
{"title":"One-Dimensional Flexible Capacitive Sensor with Large Strain and High Stability for Human Motion Monitoring.","authors":"Xinyan Yue, Xiaohu Wang, Jianbo Shao, Huabing Wang, Yu Chen, Kun Zhang, Xiao Han, Jianhan Hong","doi":"10.1021/acsami.4c14974","DOIUrl":"https://doi.org/10.1021/acsami.4c14974","url":null,"abstract":"<p><p>Flexible capacitive sensors have attracted the attention of researchers owing to their simple structure, ease of realization, and wearability. Currently, flexible capacitive sensors mainly have three-dimensional and two-dimensional structures, which are subject to several limitations in their applications. A low-cost, high-efficiency, and continuously processable process was used to wrap nylon DTY (PA) filaments on the surface of silver-coated nylon (SCN) core yarns and impregnate them with waterborne polyurethane (WPU) to obtain SCN/PA/WPU composite yarns, which were then utilized in the design of SCN/PA/WPU for the preparation of one-dimensionally structured flexible capacitive sensors. The morphology and mechanical properties of the SCN core yarn, SCN/PA wrapped yarn, and SCN/PA/WPU composite yarn were characterized. The strain-sensing performance of the sensor was analyzed, and the sensor was used to monitor human physiological activities. The sensor exhibited excellent strain capacitance sensing performance with a strain range of up to 140%. With a gauge factor of 0.66 at 10% tensile strain, it can detect strains as low as 1% and has good repeatability, withstanding more than 3200 tensile-unload cycles at 80% strain. The one-dimensional structure sensor can be used to monitor the large-scale movements of joints and muscles in various parts of the human body and the physiological signals of tiny human movements, such as breathing, coughing, and facial expressions, which have potential applications in the fields of sports monitoring and smart wearable.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453173","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}
Chao Yin, Yue Zhang, Cong Fan, Jun Zheng, Yu Yang, Yi Zhang, Jian Jiang
Posterior capsular opacification (PCO) is a common complication following cataract surgery, which can lead to a significant vision loss. This study introduces a facile method for developing a metformin-derived hydrogel (HCM6) stabilized by dynamic covalent bonds among natural polymers. This hydrogel demonstrates antifibrotic properties, on-demand drug release, pH responsiveness, injectability, and self-healing capabilities. Our in vitro experiments confirmed that the HCM6 hydrogel exhibits excellent biocompatibility, inhibiting lens epithelial cell migration, and transforming growth factor-2β (TGFβ2)-induced α-smooth muscle actin (α-SMA) expression in lens epithelial cells. In vivo studies conducted in a rat extracapsular lens extraction (ECLE) model revealed that HCM6 significantly suppressed PCO after 21 days of implantation with no observed pathological effects on surrounding tissues or the optic nerve. According to our experimental results, the inhibitory mechanism of PCO may be attributed to metformin’s suppressive effect on lens cell migration, epithelial–mesenchymal transition (EMT), and lens fiber formation. In summary, the long-acting, controllable, and on-demand release characteristics of the HCM6 hydrogel not only provide an effective strategy for preventing PCO but also offer new avenues for treating undesirable proliferative conditions in ophthalmology and beyond.
{"title":"Injectable and pH-Responsive Metformin-Loaded Hydrogel for Active Inhibition of Posterior Capsular Opacification","authors":"Chao Yin, Yue Zhang, Cong Fan, Jun Zheng, Yu Yang, Yi Zhang, Jian Jiang","doi":"10.1021/acsami.4c13318","DOIUrl":"https://doi.org/10.1021/acsami.4c13318","url":null,"abstract":"Posterior capsular opacification (PCO) is a common complication following cataract surgery, which can lead to a significant vision loss. This study introduces a facile method for developing a metformin-derived hydrogel (HCM<sub>6</sub>) stabilized by dynamic covalent bonds among natural polymers. This hydrogel demonstrates antifibrotic properties, on-demand drug release, pH responsiveness, injectability, and self-healing capabilities. Our in vitro experiments confirmed that the HCM<sub>6</sub> hydrogel exhibits excellent biocompatibility, inhibiting lens epithelial cell migration, and transforming growth factor-2β (TGFβ2)-induced α-smooth muscle actin (α-SMA) expression in lens epithelial cells. In vivo studies conducted in a rat extracapsular lens extraction (ECLE) model revealed that HCM<sub>6</sub> significantly suppressed PCO after 21 days of implantation with no observed pathological effects on surrounding tissues or the optic nerve. According to our experimental results, the inhibitory mechanism of PCO may be attributed to metformin’s suppressive effect on lens cell migration, epithelial–mesenchymal transition (EMT), and lens fiber formation. In summary, the long-acting, controllable, and on-demand release characteristics of the HCM<sub>6</sub> hydrogel not only provide an effective strategy for preventing PCO but also offer new avenues for treating undesirable proliferative conditions in ophthalmology and beyond.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486690","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}
We report the solvent-evaporation and ionic cross-linking mediated self-assembly of the shell cross-linked micelles of the amphiphilic triblock copolymer containing middle poly(methyl methacrylate) block (hydrophobic) and poly(2-dimethylamino)ethyl methacrylate end blocks (hydrophilic) on the membrane substrate to create molecular selective channels. The formation of selective channels on the substrate is attributed to the local increase of micelle concentration upon solvent evaporation, which leads to the core–core hydrophobic interaction. The post-ionic cross-linking of the shell part further reduces the intermicelle distance, thereby creating interstices for selective separation. The TUF-1:1 membrane prepared by the self-assembly of the cross-linked micelles (triblock copolymer:halide-terminated PEG-based = 1:1 w w–1) and by the post-ionic cross-linking shows molecular weight cutoff of 3000 g mol–1 and pure water permeance of 52 L m–2 h–1 bar–1. The membrane shows 99.5–99.9% rejection of Congo red and Direct red-80 in the presence or absence of salts and Na2SO4 to dye separation factor of about 900. The added functionality (PEG) in the micelle structure provides good fouling-resistant properties toward dye and bovine serum albumin. This work provides the membrane formation mechanism and the advantages of the membrane for fractionation and resource recovery applications.
我们报告了在溶剂蒸发和离子交联介导下，含有聚（甲基丙烯酸甲酯）中间嵌段（疏水性）和聚（2-二甲基氨基）乙基甲基丙烯酸酯末端嵌段（亲水性）的两亲性三嵌段共聚物的壳交联胶束在膜基底上的自组装，从而形成分子选择性通道。基底上选择性通道的形成归因于溶剂蒸发时胶束浓度的局部增加，这导致了核心与核心之间的疏水相互作用。外壳部分的后离子交联进一步缩小了胶束间的距离，从而形成了选择性分离的间隙。通过交联胶束（三嵌段共聚物：卤化物端基 PEG = 1:1 w w-1）的自组装和后离子交联制备的 TUF-1:1 膜的分子量截止值为 3000 g mol-1，纯水渗透率为 52 L m-2 h-1 bar-1。在盐和 Na2SO4 存在或不存在的情况下，该膜对刚果红和直接红-80 的抑制率为 99.5-99.9%，染料分离系数约为 900。胶束结构中添加的功能性物质（PEG）对染料和牛血清白蛋白具有良好的抗污性能。这项研究提供了膜的形成机理以及该膜在分馏和资源回收应用方面的优势。
{"title":"Low Fouling Molecular Selective Channels through Self-assembly of Cross-linked Block Copolymer Micelles for Selective Separation of Dye and Salt","authors":"Anuradha, Urvashi S. Joshi, Suresh K. Jewrajka","doi":"10.1021/acsami.4c14085","DOIUrl":"https://doi.org/10.1021/acsami.4c14085","url":null,"abstract":"We report the solvent-evaporation and ionic cross-linking mediated self-assembly of the shell cross-linked micelles of the amphiphilic triblock copolymer containing middle poly(methyl methacrylate) block (hydrophobic) and poly(2-dimethylamino)ethyl methacrylate end blocks (hydrophilic) on the membrane substrate to create molecular selective channels. The formation of selective channels on the substrate is attributed to the local increase of micelle concentration upon solvent evaporation, which leads to the core–core hydrophobic interaction. The post-ionic cross-linking of the shell part further reduces the intermicelle distance, thereby creating interstices for selective separation. The TUF-1:1 membrane prepared by the self-assembly of the cross-linked micelles (triblock copolymer:halide-terminated PEG-based = 1:1 w w<sup>–1</sup>) and by the post-ionic cross-linking shows molecular weight cutoff of 3000 g mol<sup>–1</sup> and pure water permeance of 52 L m<sup>–</sup><sup>2</sup> h<sup>–1</sup> bar<sup>–1</sup>. The membrane shows 99.5–99.9% rejection of Congo red and Direct red-80 in the presence or absence of salts and Na<sub>2</sub>SO<sub>4</sub> to dye separation factor of about 900. The added functionality (PEG) in the micelle structure provides good fouling-resistant properties toward dye and bovine serum albumin. This work provides the membrane formation mechanism and the advantages of the membrane for fractionation and resource recovery applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486822","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}
Yongjing Zhang, Ying Lin, Yanlong Ma, Qibin Yuan, Haibo Yang
Dielectric capacitors play a crucial role in the field of energy storage; however, the low discharged energy density (Ue) of existing commercial dielectrics limits their future applications. Currently, further improvement in the Ue of dielectrics is constrained by the challenge of simultaneously achieving high permittivity (εr) and high breakdown electric field strength (Eb). To address this issue, we designed a series of four-layer poly(vinylidene fluoride) (PVDF)-based composite films comprising three functional layers: a sodium bismuth titanate (NBT) plus PVDF composite (NBT&PVDF) layer to achieve high εr values and a pure PVDF layer and a boron nitride (BN) plus PVDF composite (BN&PVDF) layer to achieve high Eb values. This design synergistically enhanced the εr and Eb values of the composite films by exploiting low-loss macrointerface polarization via adjustment of the functional layer stacking order, as supported by simulation analyses. Ultimately, the composite film with a topmost layer of pure PVDF, followed by an NBT&PVDF layer, another pure PVDF layer, and a BN&PVDF layer achieved an enhanced Ue value of 26.42 J·cm–3 and excellent efficiency of 80.03% at an ultrahigh Eb value of 770 MV·m–1. This approach offers an innovative pathway for developing advanced energy storage composite dielectrics via macrointerface manipulation.
{"title":"Enhanced Energy Storage Properties of Four-Layer Composite Films via Strategic Macrointerface Modulation","authors":"Yongjing Zhang, Ying Lin, Yanlong Ma, Qibin Yuan, Haibo Yang","doi":"10.1021/acsami.4c12142","DOIUrl":"https://doi.org/10.1021/acsami.4c12142","url":null,"abstract":"Dielectric capacitors play a crucial role in the field of energy storage; however, the low discharged energy density (<i>U</i><sub>e</sub>) of existing commercial dielectrics limits their future applications. Currently, further improvement in the <i>U</i><sub>e</sub> of dielectrics is constrained by the challenge of simultaneously achieving high permittivity (ε<sub>r</sub>) and high breakdown electric field strength (<i>E</i><sub>b</sub>). To address this issue, we designed a series of four-layer poly(vinylidene fluoride) (PVDF)-based composite films comprising three functional layers: a sodium bismuth titanate (NBT) plus PVDF composite (NBT&PVDF) layer to achieve high ε<sub>r</sub> values and a pure PVDF layer and a boron nitride (BN) plus PVDF composite (BN&PVDF) layer to achieve high <i>E</i><sub>b</sub> values. This design synergistically enhanced the ε<sub>r</sub> and <i>E</i><sub>b</sub> values of the composite films by exploiting low-loss macrointerface polarization via adjustment of the functional layer stacking order, as supported by simulation analyses. Ultimately, the composite film with a topmost layer of pure PVDF, followed by an NBT&PVDF layer, another pure PVDF layer, and a BN&PVDF layer achieved an enhanced <i>U</i><sub>e</sub> value of 26.42 J·cm<sup>–3</sup> and excellent efficiency of 80.03% at an ultrahigh <i>E</i><sub>b</sub> value of 770 MV·m<sup>–1</sup>. This approach offers an innovative pathway for developing advanced energy storage composite dielectrics via macrointerface manipulation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486689","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}
Apurva Jaiswal, Neha Kaushik, Tirtha Raj Acharya, Han Sup Uhm, Eun Ha Choi, Nagendra Kumar Kaushik
Nitric oxide (NO), a potential therapeutic antiaging molecule, modulates various physiological and cellular processes. However, alterations in endogenous NO levels brought on by aging impact multiple organ systems and heighten susceptibility to age-related skin diseases. This correlation underscores the importance of investigating NO-based antiaging interventions. Nonthermal plasma-generated NO is a promising avenue for cosmetic and regenerative medicine due to its capacity to stimulate cellular growth. Herein, we examine the potential of plasma-generated nitric oxide water (NOW) as a bioactive agent in human dermal fibroblasts, emphasizing gene expression patterns linked to extracellular matrix (ECM) breakdown and cellular senescence. The findings of our study indicate that administering NOW at lower dosages enhances cell migration and proliferation. Moreover, the genetic signatures associated with ECM synthesis, antioxidant defense, and antisenescence pathways have been analyzed in NOW-exposed cells. Notably, the downregulation of ECM-degrading enzyme transcripts─collagenase, elastase, and hyaluronidase─suggests NOW’s potential in mitigating the intrinsic skin aging phenomena, emphasizing the promise of NO-based interventions in advancing antiaging strategies within regenerative medicine.
{"title":"Antiaging in a Bottle: Bioactive Competency of Plasma-Generated Nitric Oxide Water for Modulation of Aging-Related Signature in Human Dermal Cells","authors":"Apurva Jaiswal, Neha Kaushik, Tirtha Raj Acharya, Han Sup Uhm, Eun Ha Choi, Nagendra Kumar Kaushik","doi":"10.1021/acsami.4c14051","DOIUrl":"https://doi.org/10.1021/acsami.4c14051","url":null,"abstract":"Nitric oxide (NO), a potential therapeutic antiaging molecule, modulates various physiological and cellular processes. However, alterations in endogenous NO levels brought on by aging impact multiple organ systems and heighten susceptibility to age-related skin diseases. This correlation underscores the importance of investigating NO-based antiaging interventions. Nonthermal plasma-generated NO is a promising avenue for cosmetic and regenerative medicine due to its capacity to stimulate cellular growth. Herein, we examine the potential of plasma-generated nitric oxide water (NOW) as a bioactive agent in human dermal fibroblasts, emphasizing gene expression patterns linked to extracellular matrix (ECM) breakdown and cellular senescence. The findings of our study indicate that administering NOW at lower dosages enhances cell migration and proliferation. Moreover, the genetic signatures associated with ECM synthesis, antioxidant defense, and antisenescence pathways have been analyzed in NOW-exposed cells. Notably, the downregulation of ECM-degrading enzyme transcripts─collagenase, elastase, and hyaluronidase─suggests NOW’s potential in mitigating the intrinsic skin aging phenomena, emphasizing the promise of NO-based interventions in advancing antiaging strategies within regenerative medicine.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486696","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}
Ziyi Qin, Zhenlin Jiang, Lan Zhou, Wenjun Wang, Min Zhu, Jiapeng Chen, Baoxiu Wang, Chaosheng Wang
Zirconia aerogels possess significant applications, including their use catalyst carriers, thermal insulation materials, and thermal barrier coatings. This is due to their ultrahigh temperature resistance, high porosity, and low thermal conductivity. Nonetheless, the inherent challenges associated with ZrO2 aerogels, such as high brittleness, low compressive strength, and inadequate formability, restrict their potential applications. In this paper, with ultralow thermal conductivity and high strength zirconia aerogel composites with inorganic zirconium salt zirconium carbonate as the raw material, acetic acid as the solvent, polyvinylpyrrolidone (PVP) as the viscosity builder to stabilize the structure of the aerogel during the freeze-drying process. Additionally, yttrium nitrate hexahydrate (Y(NO3)3·6H2O) is employed as a phase stabilizer. The sol–gel method, in conjunction with the freeze-drying process, is utilized to fabricate ZrO2 aerogel composites with an optimized microstructure. The findings indicate that optimal process parameters are achieved with a PVP solution concentration of 2.0 wt % and a zirconium carbonate concentration of 20 wt %. The mechanical properties of the resulting composites reach up to 550 kPa, while the thermal insulation performance exhibits a temperature difference of 207 °C/cm and a thermal conductivity of 0.0504 W/(m·K). This advancement addresses the mechanical stability issues commonly associated with traditional ceramic aerogels and widely used elastic insulating materials, thereby enhancing their applicability as thermal insulation and heat preservation materials.
{"title":"Construction and Properties of Ultralow Thermal Conductivity and High Strength Zirconia Aerogel Composites by Freeze-Drying","authors":"Ziyi Qin, Zhenlin Jiang, Lan Zhou, Wenjun Wang, Min Zhu, Jiapeng Chen, Baoxiu Wang, Chaosheng Wang","doi":"10.1021/acsami.4c13860","DOIUrl":"https://doi.org/10.1021/acsami.4c13860","url":null,"abstract":"Zirconia aerogels possess significant applications, including their use catalyst carriers, thermal insulation materials, and thermal barrier coatings. This is due to their ultrahigh temperature resistance, high porosity, and low thermal conductivity. Nonetheless, the inherent challenges associated with ZrO<sub>2</sub> aerogels, such as high brittleness, low compressive strength, and inadequate formability, restrict their potential applications. In this paper, with ultralow thermal conductivity and high strength zirconia aerogel composites with inorganic zirconium salt zirconium carbonate as the raw material, acetic acid as the solvent, polyvinylpyrrolidone (PVP) as the viscosity builder to stabilize the structure of the aerogel during the freeze-drying process. Additionally, yttrium nitrate hexahydrate (Y(NO<sub>3</sub>)<sub>3</sub>·6H<sub>2</sub>O) is employed as a phase stabilizer. The sol–gel method, in conjunction with the freeze-drying process, is utilized to fabricate ZrO<sub>2</sub> aerogel composites with an optimized microstructure. The findings indicate that optimal process parameters are achieved with a PVP solution concentration of 2.0 wt % and a zirconium carbonate concentration of 20 wt %. The mechanical properties of the resulting composites reach up to 550 kPa, while the thermal insulation performance exhibits a temperature difference of 207 °C/cm and a thermal conductivity of 0.0504 W/(m·K). This advancement addresses the mechanical stability issues commonly associated with traditional ceramic aerogels and widely used elastic insulating materials, thereby enhancing their applicability as thermal insulation and heat preservation materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486695","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}
Jie Zhang, Jun Jin, Ouwei Sheng, Ya Chen, Yan Lu, Zhaoyin Wen
Li10.35Ge1.35P1.65S12 (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl3. On the one hand, InCl3 induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In3+/Cl– and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li+ flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm2, and a super long cycling stability over 8000 h. Our synergistic interlayer strategy would open an effective avenue for solving interfacial challenges for practical sulfide-based solid-state batteries.
{"title":"Achieving Higher Critical Current Density in LGPS-Based Lithium Metal Batteries via a Synergistic Interlayer for Physical Inhibition and Chemical Scavenging of Lithium Dendrites","authors":"Jie Zhang, Jun Jin, Ouwei Sheng, Ya Chen, Yan Lu, Zhaoyin Wen","doi":"10.1021/acsami.4c14887","DOIUrl":"https://doi.org/10.1021/acsami.4c14887","url":null,"abstract":"Li<sub>10.35</sub>Ge<sub>1.35</sub>P<sub>1.65</sub>S<sub>12</sub> (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl<sub>3</sub>. On the one hand, InCl<sub>3</sub> induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In<sup>3+</sup>/Cl<sup>–</sup> and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li<sup>+</sup> flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm<sup>2</sup>, and a super long cycling stability over 8000 h. Our synergistic interlayer strategy would open an effective avenue for solving interfacial challenges for practical sulfide-based solid-state batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486823","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}
Zhiran Chen, Fangjie Hu, Jingfeng Xiang, Xiaoxiang Zhou, Bo Wu, Baohang Fan, Han Tang, Bin Liu, Longyun Chen
The immunosuppressive nature of the tumor microenvironment (TME) contributes to radioresistance, thereby impairing the effectiveness of radiotherapy as a therapeutic intervention. Activation through the stimulator of interferon genes (STING) pathway shows potential in modulating immunogenicity. However, the therapeutic efficacy of STING agonists might be restricted by off-target effects and potential cytotoxicity. In this work, nanoexosomes (EXOs) loaded within porous microneedles were employed for precise delivery of the STING agonist MSA-2 (MEM) to the tumor site. Leveraging the enhanced tumor penetration enabled by microneedles, EXOs can be continually released and accumulate within deep residual tumors. Once internalized, these EXOs release the encapsulated MSA-2, facilitating the activation of the STING pathway upon exposure to ultrahigh dose-rate (FLASH) irradiation. This strategy elevates the type I interferon level, promotes dendric cell maturation, and modulates the immunosuppressive TME, showing efficient antitumor efficacy in both primary/metastatic tumors. Furthermore, the induction of a potent immune response effectively prevented tumor recurrence. The combination of EXO-loaded microneedles with FLASH radiotherapy resulted in minimal systemic side effects, attributed to precise drug delivery and radioprotection conferred by FLASH. Altogether, the strategic design of EXO-loaded microneedles holds promise for enhancing MSA-2 delivery, thereby mitigating the radioresistant tumor microenvironment through STING cascade activation-mediated immunotherapy, consequently optimizing the outcomes of FLASH radiotherapy.
肿瘤微环境（TME）的免疫抑制特性会导致放射抗药性，从而损害放疗作为一种治疗干预手段的有效性。通过干扰素基因刺激器（STING）途径进行激活显示了调节免疫原性的潜力。然而，STING 激动剂的疗效可能会受到脱靶效应和潜在细胞毒性的限制。在这项研究中，采用了装载在多孔微针中的纳米外泌体（EXOs），将STING激动剂MSA-2（MEM）精确输送到肿瘤部位。利用微针增强的肿瘤穿透性，EXOs可以不断释放并在深部残留肿瘤内积聚。一旦内化，这些 EXOs 就会释放出封装的 MSA-2，从而在受到超高剂量率（FLASH）照射时促进 STING 通路的激活。这种策略可提高 I 型干扰素水平，促进树突细胞成熟，并调节免疫抑制 TME，从而在原发性/转移性肿瘤中显示出高效的抗肿瘤疗效。此外，诱导的强效免疫反应还能有效防止肿瘤复发。EXO微针与FLASH放疗相结合，全身副作用极小，这归功于FLASH的精确给药和放射保护。总之，EXO负载微针的战略设计有望增强MSA-2的输送，从而通过STING级联激活介导的免疫疗法缓解抗放射肿瘤微环境，进而优化FLASH放疗的效果。
{"title":"Mesoporous Microneedles Enabled Localized Controllable Delivery of Stimulator of Interferon Gene Agonist Nanoexosomes for FLASH Radioimmunotherapy against Breast Cancer","authors":"Zhiran Chen, Fangjie Hu, Jingfeng Xiang, Xiaoxiang Zhou, Bo Wu, Baohang Fan, Han Tang, Bin Liu, Longyun Chen","doi":"10.1021/acsami.4c09833","DOIUrl":"https://doi.org/10.1021/acsami.4c09833","url":null,"abstract":"The immunosuppressive nature of the tumor microenvironment (TME) contributes to radioresistance, thereby impairing the effectiveness of radiotherapy as a therapeutic intervention. Activation through the stimulator of interferon genes (STING) pathway shows potential in modulating immunogenicity. However, the therapeutic efficacy of STING agonists might be restricted by off-target effects and potential cytotoxicity. In this work, nanoexosomes (EXOs) loaded within porous microneedles were employed for precise delivery of the STING agonist MSA-2 (MEM) to the tumor site. Leveraging the enhanced tumor penetration enabled by microneedles, EXOs can be continually released and accumulate within deep residual tumors. Once internalized, these EXOs release the encapsulated MSA-2, facilitating the activation of the STING pathway upon exposure to ultrahigh dose-rate (FLASH) irradiation. This strategy elevates the type I interferon level, promotes dendric cell maturation, and modulates the immunosuppressive TME, showing efficient antitumor efficacy in both primary/metastatic tumors. Furthermore, the induction of a potent immune response effectively prevented tumor recurrence. The combination of EXO-loaded microneedles with FLASH radiotherapy resulted in minimal systemic side effects, attributed to precise drug delivery and radioprotection conferred by FLASH. Altogether, the strategic design of EXO-loaded microneedles holds promise for enhancing MSA-2 delivery, thereby mitigating the radioresistant tumor microenvironment through STING cascade activation-mediated immunotherapy, consequently optimizing the outcomes of FLASH radiotherapy.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":9.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452199","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}
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