scalable fabrication

  • 文章类型: Journal Article
    有效的局部药物递送仍然是青光眼管理中的重大挑战。虽然纳米颗粒配方提供了相当大的前景,他们复杂的准备过程,共同交付问题,和批量一致性阻碍了它们的潜力。这里开发了一种可扩展的制造策略,用于制备具有增强的药物递送效率的固体药物纳米颗粒(SDN)。使用疏水性抗青光眼药物溴莫尼定(BM)和倍他洛尔(BX),通过连续工艺制造均匀固定组合BM/BXSDN,改善青光眼联合治疗的批次间一致性。海藻糖被用作冻干保护剂,BM/BXSDN可以作为干粉储存并容易地在磷酸盐缓冲盐水中重构。重要的是,重组的BM/BXSDN形式清晰,均匀溶液,并表现出微不足道的细胞毒性和刺激性,使它们非常适合作为眼药水的局部给药。离体和体内研究表明,与亲水对应物相比,局部施用的BM/BXSDN可显着(约2倍至3倍)渗透通过角膜。即,酒石酸溴莫尼定,和盐酸倍他洛尔.值得注意的是,BM/BXSDN在正常血压大鼠和青光眼小鼠体内均表现出一致的眼内压降低作用。总的来说,这项研究证明了可扩展制造策略和所得BM/BXSDN通过滴眼液改善青光眼管理的潜力。
    Efficient topical drug delivery remains a significant challenge in glaucoma management. Although nanoparticle formulations offer considerable promise, their complex preparation processes, co-delivery issues, and batch consistency have hindered their potential. A scalable fabrication strategy is developed here for preparing solid drug nanoparticles (SDNs) with enhanced drug delivery efficiency. Utilizing hydrophobic antiglaucoma drugs brimonidine (BM) and betaxolol (BX), uniform fixed combination BM/BX SDNs are fabricated through a continuous process, improving batch-to-batch consistency for combined glaucoma treatment. With trehalose being used as a lyoprotectant, BM/BX SDNs can be stored as dry powder and easily reconstituted in phosphate buffered saline. Importantly, reconstituted BM/BX SDNs form clear, homogenous solutions, and exhibit negligible cytotoxicity and irritation, making them well-suited for topical administration as eyedrops. Ex vivo and in vivo studies demonstrated that topically applied BM/BX SDNs permeate through the cornea significantly (about two fold to three fold) compared to their hydrophilic counterparts, i.e., brimonidine tartrate, and betaxolol hydrogen chloride. Notably, BM/BX SDNs displayed consistent intraocular pressure lowering effects in vivo in both normotensive rats and glaucoma mice. Collectively, this study demonstrates the potential of the scalable fabrication strategy and the resultant BM/BX SDNs for improving glaucoma management through eyedrops.
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  • 文章类型: Journal Article
    高性能和稳定的钙钛矿太阳能电池(PSC)的可升级打印是商业化的高度期望。然而,由于缺乏对钙钛矿结晶动力学的系统理解和控制,印刷PSC的效率落后于实验室规模的旋涂对应物。这里,我们报告了使用添加剂1-丁基吡啶四氟硼酸酯(BPyBF4)用于高质量环境印刷的α-甲酰胺三碘化铅(FAPbI3)钙钛矿薄膜的受控结晶动力学。使用原位掠入射广角X射线散射和光学诊断,我们证明了在没有δ-FAPbI3参与的情况下,印刷过程中前体自发形成α-FAPbI3和溶胶-凝胶。BPyBF4的加入延迟了α-FAPbI3的结晶开始,增强了从溶胶-凝胶到钙钛矿的转化,并减少印刷过程中的堆叠缺陷。因此,改变的结晶导致更少的空隙,较大的颗粒,和较少的陷阱诱导的重组损失在印刷薄膜。对于0.09cm2面积的器件和5cm×5cm面积的模块,印刷的PSC产生23.50%和21.60%的高功率转换效率,分别。进一步证明了设备稳定性的提高,即,大约94%的初始效率在环境条件下保持超过2400h而不封装。本研究为大面积高性能PSC的环境印刷制造提供了一种有效的结晶控制方法。本文受版权保护。保留所有权利。
    Upscalable printing of high-performance and stable perovskite solar cells (PSCs) is highly desired for commercialization. However, the efficiencies of printed PSCs lag behind those of their lab-scale spin-coated counterparts owing to the lack of systematic understanding and control over perovskite crystallization dynamics. Here, the controlled crystallization dynamics achieved using an additive 1-butylpyridine tetrafluoroborate (BPyBF4 ) for high-quality ambient printed α-formamidinium lead triiodide (FAPbI3 ) perovskite films are reported. Using in situ grazing-incidence wide-angle X-ray scattering and optical diagnostics, the spontaneous formation of α-FAPbI3 from precursors during printing without the involvement of  δ-FAPbI3 is demonstrated. The addition of BPyBF4 delays the crystallization onset of α-FAPbI3 , enhances the conversion from sol-gel to perovskite, and reduces stacking defects during printing. Therefore, the altered crystallization results in fewer voids, larger grains, and less trap-induced recombination loss within printed films. The printed PSCs yield high power conversion efficiencies of 23.50% and 21.60% for a 0.09 cm-2 area device and a 5 cm × 5 cm-area module, respectively. Improved device stability is further demonstrated, i.e., approximately 94% of the initial efficiency is retained for over 2400 h under ambient conditions without encapsulation. This study provides an effective crystallization control method for the ambient printing manufacture of large-area high-performance PSCs.
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  • 文章类型: Journal Article
    超疏水涂层在自清洁和油水分离方面具有巨大的应用前景,但通过简单的方法大规模制备坚固且耐候的超疏水涂层仍然具有挑战性。在这里,这项工作报告了通过在各种基材上喷涂含有超疏水二氧化硅纳米颗粒和工业涂料清漆的悬浮液,从而可扩展地制造具有多尺度粗糙珊瑚礁状结构的耐候性超疏水涂层。珊瑚礁状结构有效地提高了表面粗糙度和耐磨性。快速老化实验(3000h)和室外建筑项目应用(3000m2)表明,喷涂的超疏水涂层表现出优异的自清洁性能,耐候性,和环境适应性。此外,组合的二氧化硅涂层清漆-聚氨酯(CSCP)超疏水海绵具有出色的油水分离能力,选择性地从水中吸收油达到其自身重量的39倍。此外,分子动力学(MD)模拟表明,较高的表面粗糙度的综合作用,较小的水分子扩散系数,水和表面之间较弱的静电相互作用共同决定了所制备涂层的超疏水性。这项工作从能量和动力学性质的角度加深了对超疏水表面抗润湿机理的理解,从而为超疏水材料的合理设计及其大规模应用铺平了道路。
    Superhydrophobic coating has a great application prospect in self-cleaning and oil-water separation but remains challenging for large-scale preparation of robust and weather-resistant superhydrophobic coatings via facile approaches. Herein, this work reports a scalable fabrication of weather-resistant superhydrophobic coating with multiscale rough coral reef-like structures by spraying the suspension containing superhydrophobic silica nanoparticles and industrial coating varnish on various substrates. The coral reef-like structures effectively improves the surface roughness and abrasion resistance. Rapid aging experiments (3000 h) and the outdoor building project application (3000 m2 ) show that the sprayed superhydrophobic coating exhibits excellent self-cleaning properties, weather resistance, and environmental adaptability. Moreover, the combined silica-coating varnish-polyurethane (CSCP) superhydrophobic sponge exhibits exceptional oil-water separation capabilities, selectively absorbing the oils from water up to 39 times of its own weight. Furthermore, the molecular dynamics (MD) simulation reveals that the combined effect of higher surface roughness, smaller diffusion coefficient of water molecules, and weaker electrostatic interactions between water and the surface jointly determines the superhydrophobicity of the prepared coating. This work deepens the understanding of the anti-wetting mechanism of superhydrophobic surfaces from the perspective of energetic and kinetic properties, thereby paving the way for the rational design of superhydrophobic materials and their large-scale applications.
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  • 文章类型: Journal Article
    尽管钙钛矿发光二极管(PeLED)取得了快速进展,大面积钙钛矿器件的电致发光性能远远落后于实验室规模的器件。这里,我们通过在钙钛矿层和底层空穴传输层(HTL)之间创建甜菜碱柠檬酸(BC)的两亲分子界面修饰剂,报告了3.5cm×3.5cm的大面积PeLED,具有创纪录的高外部量子效率12.1%。已发现,由于BC分子中甲基和羧基的共存,使有利的基团选择性地与HTL表面接触并增加表面自由能,因此可以有效地改善各种HTL的表面润湿性。这极大地促进了溶液处理钙钛矿薄膜的可扩展过程。此外,通过羧基中的C=O与Pb悬空键之间的配位,钙钛矿发光体的发光性能同时得到增强。
    Despite the rapid progress in perovskite light-emitting diodes (PeLEDs), the electroluminescence performance of large-area perovskite devices lags far behind that of laboratory-size ones. Here, we report a 3.5 cm × 3.5 cm large-area PeLED with a record-high external quantum efficiency of 12.1% by creating an amphipathic molecular interface modifier of betaine citrate (BC) between the perovskite layer and the underlying hole transport layer (HTL). It is found that the surface wettability for various HTLs can be efficiently improved as a result of the coexistence of methyl and carboxyl groups in the BC molecules that makes favorable groups to selectively contact with the HTL surface and increases the surface free energy, which greatly facilitates the scalable process of solution-processed perovskite films. Moreover, the luminous performance of perovskite emitters is simultaneously enhanced through the coordination between C═O in the carboxyl groups and Pb dangling bonds.
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  • 文章类型: Journal Article
    用于气体分离的大面积沸石膜的可再现制造仍然是巨大的挑战。我们首次报告了通过在19通道氧化铝整料上进行单步二次生长的高性能沸石MFI膜的可扩展制造。这些整体膜的堆积密度和机械强度远高于管状膜。使用真空和Wicke-Kallenbach模式可比较地评估整体式膜对丁烷异构体混合物的分离性能。有效面积为~84cm2的三种膜的正丁烷渗透和正丁烷/异丁烷分离因子>1.0×10-7mol(m2sPa)-1,并且在343K时>50等摩尔正丁烷/异丁烷混合物,分别。我们成功地扩大了膜合成的规模,迄今为止最大的面积为270cm2,是工业1m长的管状膜面积的1.3倍。整料负载的沸石MFI膜显示出工业正丁烷/异丁烷分离的巨大潜力。
    The reproducible fabrication of large-area zeolite membranes for gas separation is still a great challenge. We report the scalable fabrication of high-performance zeolite MFI membranes by single-step secondary growth on the 19-channel alumina monoliths for the first time. The packing density and mechanical strength of the monolithic membranes are much higher for these than for tubular ones. Separation performance of the monolithic membranes toward the butane isomer mixture was comparably evaluated using the vacuum and Wicke-Kallenbach modes. The n-butane permeances and n-butane/i-butane separation factors for the three membranes with an effective area of ∼84 cm2 were >1.0 × 10-7 mol (m2 s Pa)-1 and >50 at 343 K for an equimolar n-butane/i-butane mixture, respectively. We succeeded in scaling up the membrane synthesis with the largest area of 270 cm2 to date which has 1.3 times the area of an industrial 1 m long tubular membrane. Monolith supported zeolite MFI membranes show great potential for industrial n-butane/i-butane separation.
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  • 文章类型: Journal Article
    Developing manufacturing methods that are scalable and compatible with a roll-to-roll process with low waste of material has become a pressing need to transfer organic photovoltaics (OPVs) to a viable renewable energy source. For this purpose, various spray printing methods have been proposed. Among them, electrospray (ES) is an attractive option due to its negligible material waste, tunable droplet size, and tolerance to the substrate defects and roughness. Conventional ES with a circular spray footprint often makes the droplets well separated and unlikely to merge, giving rise to \"coffee rings\" which cause a rough and flawed film morphology. Here, a quadrupole electrode is introduced to generate a compressing electric field that squeezes the conical ES profile into the shape of a thin sheet. The numerical simulation and experimental data of the trajectories of sprayed droplets show that the quadrupole apparatus can effectively increase the long axis to short axis ratio of the oval spray footprint and hence bring droplets closer to each other and make the merging more likely for the deposited droplets. By promoting the merging of droplets, individual coffee rings are also suppressed. Thus, the quadrupole ES offers untapped opportunities for effectively reducing voids and improving the flatness of the ES-printed active layer. The devices with a PM6:N3 active layer printed by the sheet ES exhibited the highest power conversion efficiency (PCE) of up to 15.98%, which is a noticeable improvement over that (14.85%) of counterparts fabricated by a conventional conical ES. This is the highest PCE reported for ES-printed OPVs and is one of the most efficient spray-deposited OPVs so far. In addition, the all-spray-printed devices reached a PCE of 14.55%, which is also among the most efficient all-spray-printed OPVs.
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  • 文章类型: Journal Article
    Although a variety of nanoparticles with better-than-bulk material performances can be synthesized, it remains a challenge to scale the extraordinary properties of individual nanoscale units to the macroscopic level for bulk nanostructured materials. Here, we report a general and scalable biosynthesis strategy that involves simultaneous growth of cellulose nanofibrils through microbial fermentation and co-deposition of various kinds of nanoscale building blocks (NBBs) through aerosol feeding on solid culture substrates. We employ this biosynthesis strategy to assemble a wide range of NBBs into cellulose nanofibril-based bulk nanocomposites. In particular, the biosynthesized carbon nanotubes/bacterial cellulose nanocomposites that consist of integrated 3D cellulose nanofibril networks simultaneously achieve an extremely high mechanical strength and electrical conductivity, and thus exhibit outstanding performance as high-strength lightweight electromagnetic interference shielding materials. The biosynthesis approach represents a general and efficient strategy for large-scale production of functional bulk nanocomposites with enhanced performances for practical applications. Industrial-scale production of these bulk nanocomposite materials for practical applications can be expected in the near future.
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  • 文章类型: Journal Article
    Free-standing silicon nanoprobes (SiNPs) are critical tools for intracellular bioelectrical signal recording, while a scalable fabrication of these tiny SiNPs with ab initio geometry designs has not been possible. In this work, we demonstrate a novel growth shaping of slim Si nanowires (SiNWs) into SiNPs with sharp tips (curvature radii <300 nm), tunable angles of 30°, 60°, to 120° and even programmable triangle/circular shapes. A precise growth integration of orderly single, double, and quadruple SiNPs at prescribed locations enables convenient electrode connection, transferring and mounting these tiny tips onto movable arms to serve as long-protruding (over 4-20 μm) nanoprobes. Mechanical flexibility, resilience, and field-effect sensing functionality of the SiNPs were systematically testified in liquid nanodroplet and cell environments. This highly reliable and economic manufacturing of advanced SiNPs holds a strong potential to boost and open up the market implementations of a wide range of intracellular sensing, monitoring, and editing applications.
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  • 文章类型: Journal Article
    The development of highly conductive electrodes with robust mechanical durability and clear transmittance in the visible to IR spectral range is of great importance for future wearable/flexible electronic applications. In particular, low resistivity, robust flexibility, and wide spectral transparency have a significant impact on optoelectronic performance. Herein, we introduce a new class of covellite copper monosulfide (CuS) nanosheet films as a promising candidate for soft transparent conductive electrodes (TCEs). An atmospheric sulfur adsorption-corrosion phenomenon represents a key approach in our work for the achievement of wafer-scale CuS nanosheet films through systematic control of the neat Cu layer thickness ranging from 2 to 10 nm multilayers at room temperature. These nanosheet films provide outstanding conductivity (∼25 Ω sq-1) and high transparency (> 80%) in the visible to infrared region as well as distinct flexibility and long stability under air exposure, yielding a high figure-of-merit (∼60) that is comparable to that of conventional rigid metal oxide material-based TCEs. Our unique room temperature synthesis process delivers high quality CuS nanosheets on any arbitrary substrates in a short time (< 1 min) scale, thus guaranteeing the widespread use of highly producible and scalable device fabrication.
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  • 文章类型: Journal Article
    Developing scalable processing methods with low material waste is still one of the remaining challenges for organic photovoltaics (OPVs) to become a practical renewable energy source. Here, we report the first study on printing active layers of OPVs containing non-fullerene acceptors (NFAs) by electrospray (ES). The properties of the solvent significantly influence the interfacial morphology of ES-printed organic thin-films, and solvent engineering is essential to facilitate the formation of efficient active-layer films. We introduce low-vapor-pressure non-halogen solvent o-xylene (OXY) into the high vapor pressure solvent of chloroform to form a binary solvent system with appropriate evaporation time, electric conductivity, and solubility. The characteristic times of the ES process using binary solvents are quantified to provide insights into the dynamic formation of thin films. A longer droplet evaporation time with decent solubility collectively decrease the roughness and domain size of the polymer/NFA blend films, thus increase the photocurrent and fill factor of the ES-printed OPV devices. The ES-printed active layers show enhanced crystallinity and phase separation of NFA molecules than the spin-coated films. The champion cell with an ES-printed PTB7-Th:FOIC active layer exhibits a power conversion efficiency of 9.45%, which is on par with the spin-coated cells and is among the highest of spray-deposited organic solar cells to date. This work demonstrates that ES is an effective method to prepare OPVs on NFAs.
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