large-scale synthesis

大规模合成
  • 文章类型: Journal Article
    本文介绍了将实验室规模的合成(1g)过渡到大规模(400g)合成3-5-二氨基-1H-吡唑的工作。一种治疗抗生素耐药铜绿假单胞菌生物膜感染的新药。将实验室规模合成中潜在危险的重氮化步骤转变为安全且易于处理的流动化学步骤。此外,本文介绍了OSHA推荐的活性化合物E的安全性评估,由Fauske和Associates表演,LLC,伯尔岭,IL,美国。
    This paper presents the work performed to transition a lab-scale synthesis (1 g) to a large-scale (400 g) synthesis of the 3-5-diamino-1H-Pyrazole Disperazol, a new pharmaceutical for treatment of antibiotic-resistant Pseudomonas aeruginosa biofilm infections. The potentially hazardous diazotisation step in the lab-scale synthesis was transformed to a safe and easy-to-handle flow chemistry step. Additionally, the paper presents an OSHA-recommended safety assessment of active compound E, as performed by Fauske and Associates, LLC, Burr Ridge, IL, USA.
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  • 文章类型: Journal Article
    异鸟苷(isoG)是鸟苷(G)的天然结构异构体,具有在离子载体中应用的巨大潜力,遗传学,凝胶形成,和癌症治疗。然而,市售isoG的克级成本相对较高。迄今为止,尚未报道大规模制备高纯度isoG的详细方法。这项研究为通过在室温下用亚硝酸钠和乙酸重氮化2,6-二氨基嘌呤核苷进行大规模合成isoG提供了一种简单方便的方法。Further,该方法可以使用重氮化法从2,6-二氨基嘌呤核苷衍生物合成isoG衍生物(2'-氟-异鸟苷(1)和2'-脱氧-异鸟苷(2))。天然和修饰核苷的结构信息对于DNA/RNA的修饰和取代至关重要。这项研究首次获得了isoG的单晶结构,并使用微晶电子衍射对其进行了详细分析。isoG的三维超分子结构采用了来自不同层的π-π堆叠相互作用的类似碱基对基序,分子内氢键,和糖残基的独特氢键相互作用。这项研究有助于进一步的isoG修饰及其在药物化学和材料中的应用。
    Isoguanosine (isoG) is a natural structural isomer of guanosine (G) with significant potential for applications in ionophores, genetics, gel formation, and cancer therapy. However, the cost of commercially available isoG on a gram scale is relatively high. To date, a detailed method for the large-scale preparation of high-purity isoG has not been reported. This study presented a simple and convenient approach for the large-scale synthesis of isoG through the diazotization of 2,6-diaminopurine riboside with sodium nitrite and acetic acid at room temperature. Further, this method could synthesize isoG derivatives (2\'-fluoro-isoguanosine (1) and 2\'-deoxy-isoguanosine (2)) from 2,6-diaminopurine nucleoside derivatives using diazotization. The structural information of natural and modified nucleosides is crucial for the modification and substitution of DNA/RNA. This study obtained the single-crystal structure of isoG for the first time and analyzed it in detail using microcrystal electron diffraction. The three-dimensional supramolecular structure of isoG adopted similarly base-pair motifs from π-π stacking interaction of diverse layers, intramolecular hydrogen bonding, and distinct hydrogen bonding interactions from sugar residues. This study has contributed to further isoG modification and its applications in medicinal chemistry and materials.
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  • 文章类型: Journal Article
    尽管物联网(IoT)和便携式设备取得了进步,光和气体双重检测的零偏置传感系统的发展仍然是一个挑战。作为一项新兴技术,由二维(2D)材料的有趣的物理性质驱动的直接能量转换可以在纳米器件或零偏置集成系统中实现。在这项研究中,我们前所未有地尝试利用二维SnSe的光刺激热热电耦合,用于零偏置多模态换能器,以对光和气体进行双重检测。我们合成了均匀的,基于溶液处理的单源前体的热分解,通过合理的合成路线在SnSe多层膜中大面积6。通过利用SnSe的光刺激热电效应和热电效应的协同耦合,实现了用于光和气体双重监测的零偏置SnSe换能器。基于SnSe的换能器在532nm处的提取光响应度和NO2气体响应度对应于1.07×10-6A/W和0V时的13263.6%,分别。为了实现零偏置SnSe换能器的普遍适用性,系统评估了宽工作带宽的光电特性(对NIR可见)和对两种NO2/NH3气体的动态电流响应。
    Despite the advancement of the Internet of Things (IoT) and portable devices, the development of zero-biased sensing systems for the dual detection of light and gases remains a challenge. As an emerging technology, direct energy conversion driven by intriguing physical properties of two-dimensional (2D) materials can be realized in nanodevices or a zero-biased integrated system. In this study, we unprecedentedly attempted to exploit the photostimulated pyrothermoelectric coupling of two-dimensional SnSe for use in zero-biased multimodal transducers for the dual detection of light and gases. We synthesized homogeneous, large-area 6 in SnSe multilayers via a rational synthetic route based on the thermal decomposition of a solution-processed single-source precursor. Zero-biased SnSe transducers for the dual monitoring of light and gases were realized by exploiting the synergistic coupling of the photostimulated pyroelectric and thermoelectric effects of SnSe. The extracted photoresponsivity at 532 nm and NO2 gas responsivity of the SnSe-based transducers corresponded to 1.07 × 10-6 A/W and 13263.6% at 0 V, respectively. To bring universal applicability of the zero-biased SnSe transducers, the wide operation bandwidth photoelectrical properties (visible to NIR) and dynamic current responses toward two NO2/NH3 gases were systematically evaluated.
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  • 文章类型: Journal Article
    通过使用环境友好的前驱体,通过溶解-沉淀法以显著的效率合成了镁钙铁矿(Mg-WH)粉末,石膏。在优化条件下,每5.00g初始石膏在单个批次中产生令人印象深刻的量的3.00g(89%产率)的Mg-WH。值得注意的是,未观察到归因于杂质相的XRD峰,表明样品的单相性质。FT-IR分析证实在获得的Mg-WH相中存在PO43-和HPO42-基团。SEM-EDX结果证实Mg-WH晶体具有均匀的Ca,Mg,P,得到了O分布。在以前发表的研究论文中,由于在窄的pH和温度范围内形成材料,Mg-WH的合成一直被描述为高度复杂的过程。我们提出的合成方法特别引人注目,因为它消除了细致监测的需要,在寻求更方便,更有效的Mg-WH合成方面取得了显着进步。拟议的程序不仅强调程序的有效性,但也强调了它满足重大需求的潜力,为各种有前途的应用中的大规模生产需求提供可靠的解决方案。
    Magnesium whitlockite (Mg-WH) powders were synthesized with remarkable efficiency via the dissolution-precipitation method by employing an environmentally benign precursor, gypsum. Under optimized conditions, each 5.00 g of initial gypsum yielded an impressive amount of 3.00 g (89% yield) of Mg-WH in a single batch. Remarkably, no XRD peaks attributable to impurity phases were observed, indicating the single-phase nature of the sample. FT-IR analysis confirmed the presence of the PO43- and HPO42- groups in the obtained Mg-WH phase. The SEM-EDX results confirmed that Mg-WH crystals with homogeneous Ca, Mg, P, and O distributions were obtained. In previously published research papers, the synthesis of Mg-WH has been consistently described as a highly intricate process due to material formation within a narrow pH and temperature range. Our proposed synthesis method is particularly compelling as it eliminates the need for meticulous monitoring, presenting a notable improvement in the quest for a more convenient and efficient Mg-WH synthesis. The proposed procedure not only emphasizes the effectiveness of the process, but also highlights its potential to meet significant demands, providing a reliable solution for large-scale production needs in various promising applications.
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  • 文章类型: Journal Article
    HgTe纳米晶体(NCs)具有红外吸收光谱可调等优点,溶液可加工性,和低制造成本,为下一代红外探测器的发展提供了新的途径。尽管合成技术取得了巨大进展,在工业应用方面,实现HgTeNCs的定制合成仍然至关重要。在这里,通过利用HgTeNC的高临界成核浓度,证明了一种连续逐滴(CD)合成方法,其特征是以可行的逐滴方式添加阴离子前体。缓慢的反应动力学使HgTeNCs的尺寸定制合成具有尖锐的带尾和宽吸收范围,完全覆盖短和中红外区域。更重要的是,CD工艺的固有优点确保了从批次到批次的高均匀性和放大合成,而不损害激子特征。所得的HgTe纳米晶体光电探测器在1.7µm的截止吸收边缘处显示出8.1×1011Jones的高室温探测率。这种CD方法验证了用于HgTeNC的受控合成的稳健方法,并且可能对其他纳米晶体材料的放大合成具有重要意义。
    HgTe nanocrystals (NCs) possess advantages including tunable infrared absorption spectra, solution processability, and low fabrication costs, offering new avenues for the advancement of next-generation infrared detectors. In spite of great synthetic advances, it remains essential to achieve customized synthesis of HgTe NCs in terms of industrial applications. Herein, by taking advantage of a high critical nucleation concentration of HgTe NCs, a continuous-dropwise (CD) synthetic approach that features the addition of the anion precursors in a feasible drop-by-drop fashion is demonstrated. The slow reaction dynamics enable size-customized synthesis of HgTe NCs with sharp band tails and wide absorption range fully covering the short- and mid-infrared regions. More importantly, the intrinsic advantages of CD process ensure high-uniformity and scale-up synthesis from batch to batch without compromising the excitonic features. The resultant HgTe nanocrystal photodetectors show a high room-temperature detectivity of 8.1 × 1011 Jones at 1.7 µm cutoff absorption edge. This CD approach verifies a robust method for controlled synthesis of HgTe NCs and might have important implications for scale-up synthesis of other nanocrystal materials.
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  • 文章类型: Journal Article
    在电子器件的基底上构建均匀的共价有机骨架(COF)膜是非常需要的。这里,开发了一种简单而温和的策略,通过在固液界面上聚合来制备它们。成功制备了五种具有不同微观结构的COF薄膜,证实了该方法的普遍性。这些薄膜有很大的横向尺寸,可控厚度,和高结晶质量。而且COF图案也可以通过亲水和疏水界面工程直接在基底上实现,这有利于准备器件阵列。对于应用研究,PyTTA-TPA(PyTTA:4,4\',4″,4-(1,3,6,8-四(4-氨基苯基)芘和TPA:对苯二甲醛)COF膜在420nm处具有59.79μAW-1的高光响应度,用于光电化学(PEC)检测。当首次尝试用作光电突触设备的活性材料时,它显示出优异的光刺激突触可塑性特性,如短期可塑性(STP),长期塑性(LTP),以及STP到LTP的转换,可用于模拟生物突触功能。
    Constructing uniform covalent organic framework (COF) film on substrates for electronic devices is highly desirable. Here, a simple and mild strategy is developed to prepare them by polymerization on a solid-liquid interface. The universality of the method is confirmed by the successful preparation of five COF films with different microstructures. These films have large lateral size, controllable thickness, and high crystalline quality. And COF patterns can also be directly achieved on substrates via hydrophilic and hydrophobic interface engineering, which is in favor of preparing device array. For application studies, the PyTTA-TPA (PyTTA: 4,4\',4\'\',4\'\'\'-(1,3,6,8-Tetrakis(4-aminophenyl)pyrene and TPA: terephthalaldehyde) COF film has a high photoresponsivity of 59.79 μA W-1 at 420 nm for photoelectrochemical (PEC) detection. When employed as an active material for optoelectronic synaptic devices for the first attempt, it shows excellent light-stimulated synaptic plasticity properties such as short-term plasticity (STP), long-term plasticity (LTP), and the conversion of STP to LTP, which can be used to simulate biological synaptic functions.
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  • 文章类型: Journal Article
    二氢喹唑啉酮(DHQZ)最近已被用作酮衍生的前芳族试剂,广泛用于(金属)光氧化还原反应中,作为通用的基团转移剂。在这项工作中,我们概述了一种无柱色谱的方案,用于多克规模合成的前芳香族DHQZs及其在单批次中的克规模镍/光氧化还原双催化交叉偶联中的用途,photoflow,和同时多个小批量。虽然单批次方法杠杆化了适度的收益率,尽管使用了异质碱,但简单的塞流式光反应器也表现出了良好的生产率(高达45%的产率)。同时,在简易光反应器中以多个较小批量进行金属光氧化还原催化反应,促进了高达59%的高产率和良好的重现性,暗示在没有photoflow设置的情况下是一个方便的替代方案。
    Dihydroquinazolinone (DHQZ) has recently been harnessed as a ketone-derived pro-aromatic reagent extensively employed in (metalla)photoredox reactions as versatile group transfer agents. In this work, we outline a column chromatography-free protocol for the multigram-scale synthesis of pro-aromatic DHQZs as well as its use in a gram-scale nickel/photoredox dual-catalyzed cross-coupling in single-batch, photoflow, and simultaneous multiple smaller batches. While the single-batch approach leveraged moderate yields, a simple plug-flow photoreactor also exhibited amenable productivity (up to 45 % yield) despite the use of a heterogeneous base. Meanwhile, performing the metallaphotoredox-catalyzed reaction in multiple smaller batches in an improvised photoreactor facilitated high yields of up to 59 % and good reproducibility, implying a convenient alternative in the absence of photoflow setups.
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  • 文章类型: Journal Article
    2D薄膜,具有原子薄的厚度,正在成为下一代电子设备的有希望的候选人,由于其新颖的性能和高性能。早年,使用几种方法(机械/液体剥离,化学气相沉积,等。).然而,二维薄片的有限尺寸阻碍了它们的基础研究和设备应用,因此,有效的大规模制备2D薄膜仍然具有挑战性。最近,脉冲激光沉积(PLD)似乎是一种有效的二维薄膜晶圆级生长方法,由于目标保持的化学计量,高增长率,和效率。在这次审查中,综述了近年来二维薄膜PLD制备的研究进展,包括增长机制,战略,和材料分类。首先,重点介绍了PLD生长的有效策略。然后,增长,表征,介绍了各种2D薄膜的器件应用,比如石墨烯,h-BN,MoS2,BP,氧化物,钙钛矿,半金属,等。最后,展望了PLD技术的潜在挑战和进一步的研究方向。
    2D thin films, possessing atomically thin thickness, are emerging as promising candidates for next-generation electronic devices, due to their novel properties and high performance. In the early years, a wide variety of 2D materials are prepared using several methods (mechanical/liquid exfoliation, chemical vapor deposition, etc.). However, the limited size of 2D flakes hinders their fundamental research and device applications, and hence the effective large-scale preparation of 2D films is still challenging. Recently, pulsed laser deposition (PLD) has appeared to be an impactful method for wafer-scale growth of 2D films, owing to target-maintained stoichiometry, high growth rate, and efficiency. In this review, the recent advances on the PLD preparation of 2D films are summarized, including the growth mechanisms, strategies, and materials classification. First, efficacious strategies of PLD growth are highlighted. Then, the growth, characterization, and device applications of various 2D films are presented, such as graphene, h-BN, MoS2 , BP, oxide, perovskite, semi-metal, etc. Finally, the potential challenges and further research directions of PLD technique is envisioned.
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  • 文章类型: Journal Article
    植物化学共轭银纳米颗粒(AgNP)被认为是纳米技术和治疗之间的桥梁。由于此类材料的广泛应用,因此非常需要绿色和大量生产。尤其是在生物医学领域。在这项研究中,使用一锅法固态技术大规模合成了莫林稳定的银纳米颗粒(莫林/AgNPs)。该反应通过在环境温度下球磨桑色素和硝酸银粉末而不使用任何溶剂或有毒试剂来实现。制备的morin/AgNP表现出半六边形形状,尺寸范围为21至43nm。X射线衍射结果阐明了高度结晶的AgNP的形成。傅里叶变换红外和X射线光电子能谱分析证明,羰基,桑林中的芳香官能团在AgNP的还原和稳定中起着重要作用。利用2,2-二苯基-1-甲基酰基-肼基(DPPH)测定来评估莫林/AgNP的抗氧化潜力。Morin/AgNP表现出比Morin(IC50=14.8μg/mL)更好的自由基清除活性(IC50=11.7μg/mL)。此外,合成的AgNPs对大肠杆菌具有良好的抗菌活性,肺炎克雷伯菌,金黄色葡萄球菌,变形链球菌,和白色念珠菌.观察到针对金黄色葡萄球菌(21.2±0.6mm)和肺炎克雷伯菌(20.3±0.5mm)的最大抑制区。上述结果强调了桑林/AgNP作为有前途的抗氧化剂和抗微生物材料用于安全医疗应用的预期应用。研究重点:开发了大规模生产AgNPs的简单绿色路线。Morin在AgNP的固态合成中充当还原剂/稳定剂。Morin/AgNPs具有良好的抗菌和抗氧化活性。
    Phytochemical-conjugated silver nanoparticles (AgNPs) are believed to act as a bridge between nanotechnology and therapy. There is a significant need for green and mass production of such materials due to their extensive applications, especially in the biomedical sector. In this study, morin-stabilized silver nanoparticles (morin/AgNPs) were synthesized on a massive scale using a one-pot solid-state technique. The reaction is achieved by ball milling of morin and silver nitrate powders at ambient temperature without any solvent or toxic reagent. The prepared morin/AgNPs exhibited a semi-hexagonal shape and ranged in size from 21 to 43 nm. The x-ray diffraction results elucidated the formation of highly crystalline AgNPs. Fourier transform infrared and x-ray photoelectron spectroscopic analyses prove that the hydroxyl, carbonyl, and aromatic functionalities in morin are playing major roles in the reduction and stabilization of AgNPs. The antioxidant potential of morin/AgNPs was evaluated utilizing 2,2-Diphenyl-1-picryl-hydrazyl (DPPH) assay. Morin/AgNPs exhibited better free radical scavenging activity (IC50  = 11.7 μg/mL) than morin (IC50  = 14.8 μg/mL). Furthermore, the synthesized AgNPs showed promising antimicrobial activity against Escherichia coli, Klebsiella pneumonia, Staphylococcus aureus, Streptococcus mutans, and Candida albicans. The largest inhibition zones were observed against S. aureus (21.2 ± 0.6 mm) and K. pneumonia (20.3 ± 0.5 mm) bacteria. The foregoing results highlighted the prospective application of morin/AgNPs as a promising antioxidant and antimicrobial material for safe medical applications. RESEARCH HIGHLIGHTS: A simple green route for the large-scale production of AgNPs was developed. Morin acts as reducing/stabilizing agent in solid-state synthesis of AgNPs. Morin/AgNPs exhibited promising antimicrobial and antioxidant activity.
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  • 文章类型: Journal Article
    碳点的出现和快速发展为光电领域的应用提供了前所未有的机遇,但是它们的实用性仍然受到复杂的合成程序和固态荧光的底物依赖性的影响。在这项研究中,我们设计了一种独特的微波辅助固相合成路线,用于制备具有黄色,橙色,和红色荧光(Y-CD,O-CD,R-CD)通过简单地调整反应物的质量比,一种适用于大规模合成CD的方法。使用物理学和光谱学技术对Y-/O-/R-CD进行了系统表征。基于所提出的荧光CD粉末的完美的固态荧光性能,Y-/O-/R-CD以低成本成功地用于构建多色和白色发光二极管器件。此外,与O-CD和R-CD相比,Y-CD显示出更高的产量和发光效率,并进一步用于玻璃板和锡箔表面的指纹识别。此外,R-CD水溶液荧光对pH敏感,建议将其用作监测细胞内pH波动的pH指示剂。拟议的由CD组成的荧光粉系列可能预示着光学元件和刑事侦查领域应用的新纪元。
    The emergence and fast development of carbon dots (CDs) provide an unprecedented opportunity for applications in the field of photoelectricity, but their practicability still suffers from complicated synthesis procedures and the substrate dependence of solid-state fluorescence. In this study, we design a unique microwave-assisted solid-phase synthesis route for preparing tunable fluorescent CD powders with yellow, orange, and red fluorescence (Y-CDs, O-CDs, R-CDs) by simply adjusting the mass ratio of reactants, a method which is suitable for the large-scale synthesis of CDs. The Y-/O-/R-CDs were systematically characterized using physics and spectroscopy techniques. Based on the perfect solid-state fluorescence performance of the proposed fluorescent CD powders, the Y-/O-/R-CDs were successfully applied for the construction of multi-color and white light-emitting diode devices at low cost. Furthermore, the Y-CDs displayed much higher yield and luminous efficiency than the O-CDs and R-CDs and were further used for fingerprint identification on the surfaces of glass sheets and tinfoil. In addition, the R-CD aqueous solution fluorescence is sensitive to pH, suggesting its use as a pH indicator for monitoring intracellular pH fluctuations. The proposed series of fluorescent powders composed of CDs may herald a new era in the application of optical components and criminal investigation fields.
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