functionalization

Functionalization
  • 文章类型: Journal Article
    在环境污染和资源枯竭的情况下,开发和利用生物质资源作为石油的替代品是一个突出的研究重点。在环境保护和可持续发展的推动下,从石油基聚氨酯向生物基聚氨酯的转变是聚氨酯材料发展的主流趋势。生物质来源,如植物油,多糖,木质素在生物基聚氨酯生产中具有广泛的应用前景。这些聚氨酯的功能改性可以进一步扩大其应用范围。本文探讨了各种生物基聚氨酯的制备,它们在不同领域的应用,以及它们预期的未来发展和用途。
    Amid environmental pollution and resource depletion, developing and utilizing biomass resources as alternatives to petroleum is a prominent research focus. Driven by environmental protection and sustainable development, the shift from petroleum-based to bio-based polyurethane is a prevailing trend in polyurethane material development. Biomass sources such as vegetable oil, polysaccharides, and lignin offer extensive application prospects in bio-based polyurethane production. Functional modifications of these polyurethanes can further expand their application range. This article explores the preparation of various bio-based polyurethanes, their applications across different fields, and their anticipated future development and uses.
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  • 文章类型: Journal Article
    由SARS-CoV-2产生的COVID-19已经严重影响了全球的医疗保健系统。这一流行病凸显了疫苗开发的迫切需要。除了传统的疫苗接种模型,其中包括活减毒,重组蛋白,和灭活疫苗,纳米疫苗为推进疫苗研究和提供方便的替代品提供了一个独特的机会。这篇综述重点介绍了许多广泛使用的纳米颗粒疫苗载体,概述了它们的优点和缺点,并研究了预防SARS-CoV-2的纳米颗粒疫苗的最新进展。它还全面概述了纳米颗粒疫苗的许多优点,包括增强的宿主免疫反应,多价抗原递送,和有效的药物输送。主要目的是为创新抗病毒疫苗的开发提供参考。
    COVID-19, generated by SARS-CoV-2, has significantly affected healthcare systems worldwide. The epidemic has highlighted the urgent need for vaccine development. Besides the conventional vaccination models, which include live-attenuated, recombinant protein, and inactivated vaccines, nanovaccines present a distinct opportunity to progress vaccine research and offer convenient alternatives. This review highlights the many widely used nanoparticle vaccine vectors, outlines their benefits and drawbacks, and examines recent developments in nanoparticle vaccines to prevent SARS-CoV-2. It also offers a thorough overview of the many advantages of nanoparticle vaccines, including an enhanced host immune response, multivalent antigen delivery, and efficient drug delivery. The main objective is to provide a reference for the development of innovative antiviral vaccines.
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  • 文章类型: Journal Article
    木质素光催化转化为增值化学品,尤其是那些官能化分子代表了可持续和环境友好发展的最重要策略之一。在温和的光催化条件下将木质素中的C-C键裂解以将木质素精制成有用的分子是有意义的但具有挑战性的。同时,在解聚过程中,将各种官能团组装成活性木质素片段具有很大的挑战性。在这里,在可见光照射下使用廉价的铁催化剂,木质素中Cα-Cβ键的高选择性和有效裂解是通过配体到金属的电荷转移(LMCT)和氢原子转移(HAT)过程实现的。所产生的基于木质素片段的自由基中间体的随后的发散官能化使得能够有效地形成不同的官能化分子。该方法对于天然木质素中的Cα-Cβ键的裂解也是有效的,产生两种确定的苯甲醛单体,总收率为8.7wt%。
    The photocatalytic conversion of lignin into value-added chemicals especially those functionalized molecules represent one of the most important strategies for sustainable and environmental-friendly development. Cleavage of C-C bonds in lignin under mild photocatalytic conditions for refining lignin into useful molecules is meaningful but challenging. Meanwhile, the assembly of diverse functional groups into active lignin fragments during the depolymerization is of great challenging. Herein, using cheap iron catalysts under visible light irradiation, the highly selective and efficient cleavage of Cα-Cβ bond in lignin is realized via ligand-to-metal charge transfer (LMCT) and hydrogen atom transfer (HAT) processes. The subsequent divergent functionalization of generated lignin fragment-based radical intermediates enables an efficient formation of diverse functionalized molecules. This method is also effective for cleavage of Cα-Cβ bond in native lignin, yielding two identified benzaldehyde monomers in a total yield of 8.7 wt%.
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  • 文章类型: Journal Article
    膜分离是一种环保的,高渗透性和选择性,低能源需求过程值得科学考察和产业化。为了满足密集的需求,寻求合适的膜材料以超越渗透性和选择性之间的权衡并提高稳定性已成为当务之急。2D材料为研究膜分离过程提供了转型机会和革命性平台。尤其是,具有可控孔隙率和结构的原子薄石墨烯,以及独特的属性,被广泛认为是旨在提供极端稳定性的膜材料的候选物,指数大的选择性与高渗透率相结合。目前,它显示了开发分离膜以解决传统膜瓶颈的有希望的机会,它对分离等用途广泛的应用非常感兴趣,能量收集,和感应。在这次审查中,从分离的运输机制开始,材料选择库缩小到纳米多孔石墨烯。该研究提供了原子薄纳米多孔石墨烯制备的最新发展的启发性概述,并将此类2D纳米多孔材料的表面特性与其在关键分离应用中的性能相关联。最后,还指出了与调制和制造相关的挑战以及性能改进的潜在途径。
    Membrane separation stands as an environmentally friendly, high permeance and selectivity, low energy demand process that deserves scientific investigation and industrialization. To address intensive demand, seeking appropriate membrane materials to surpass trade-off between permeability and selectivity and improve stability is on the schedule. 2D materials offer transformational opportunities and a revolutionary platform for researching membrane separation process. Especially, the atomically thin graphene with controllable porosity and structure, as well as unique properties, is widely considered as a candidate for membrane materials aiming to provide extreme stability, exponentially large selectivity combined with high permeability. Currently, it has shown promising opportunities to develop separation membranes to tackle bottlenecks of traditional membranes, and it has been of great interest for tremendously versatile applications such as separation, energy harvesting, and sensing. In this review, starting from transport mechanisms of separation, the material selection bank is narrowed down to nanoporous graphene. The study presents an enlightening overview of very recent developments in the preparation of atomically thin nanoporous graphene and correlates surface properties of such 2D nanoporous materials to their performance in critical separation applications. Finally, challenges related to modulation and manufacturing as well as potential avenues for performance improvements are also pointed out.
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  • 文章类型: Journal Article
    尽管对分子复杂性的快速访问非常有吸引力,允许结合两个以上官能团的烯烃的多官能化仍然是一个突出的挑战。在这里,我们报告了一种新策略,将偶极环加成与光氧化还原促进的自由基开环远程C(sp3)-H官能化合并,从而实现未活化烯烃的平滑1,2,5-三官能化。高度区域选择性的[32]环加成将反应引发剂锚定在烯烃底物上。随后的卤素原子转移(XAT)选择性地引发开环过程,随后是一系列1,5-氢原子转移(1,5-HAT)和分子间氟原子转移(FAT)事件。使用这种方法,完成了三个不同官能团的位置选择性引入,并从容易获得的末端烯烃合成了广谱的有价值的β-羟基-ε-氟-腈产物。
    Although highly appealing for rapid access of molecular complexity, multi-functionalization of alkenes that allows incorporation of more than two functional groups remains a prominent challenge. Herein, we report a novel strategy that merges dipolar cycloaddition with photoredox promoted radical ring-opening remote C(sp3)-H functionalization, thus enabling a smooth 1,2,5-trifunctionalization of unactivated alkenes. A highly regioselective [3+2] cycloaddition anchors a reaction trigger onto alkene substrates. The subsequent halogen atom transfer (XAT) selectively initiates ring-opening process, which is followed by a series of 1,5-hydrogen atom transfer (1,5-HAT) and intermolecular fluorine atom transfer (FAT) events. With this method, site-selective introduction of three different functional groups is accomplished and a broad spectrum of valuable β-hydroxyl-ε-fluoro-nitrile products are synthesized from readily available terminal alkenes.
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  • 文章类型: Journal Article
    两亲性肽由于其高度可设计和自组装行为而引起了极大的关注。自组装肽在生物传感等各个领域都具有出色的潜力,环境监测,和药物输送,由于它们非凡的生物学特性,物理,和化学性质。虽然通过肽自组装形成的纳米材料已经在生物医学应用中发现了广泛的用途,基于两亲性肽的自组装的2D肽纳米片的开发在合理设计和形态调节方面仍然具有挑战性。在这项研究中,合理设计的两亲性肽分子在特定条件下自组装成肽纳米片(PNS)以封装金纳米颗粒(AuNP),导致形成具有高光热转换效率的AuNPs/PNS杂化材料。研究结果表明,2DPNS增强了纳米杂化材料的整体光热治疗效果,因为它们具有更大的AuNP托管面积和更高的生物相容性。本研究中精心设计的两亲性肽提供了对自组装分子的结构设计和功能调节的见解。此外,构建的仿生功能二维无机/有机纳米杂化材料在生物医学工程中具有潜在的应用价值。
    Amphiphilic peptides have garnered significant attention due to their highly designable and self-assembling behaviors. Self-assembled peptides hold excellent potential in various fields such as biosensing, environmental monitoring, and drug delivery, owing to their remarkable biological, physical, and chemical properties. While nanomaterials formed by peptide self-assembly have found widespread use in biomedical applications, the development of 2D peptide nanosheets based on the self-assembly of amphiphilic peptides remains challenging in terms of rational design and morphology modulation. In this study, rationally designed amphiphilic peptide molecules are self-assembled into peptide nanosheets (PNS) under specific conditions to encapsulate gold nanoparticles (AuNPs), resulting in the formation of AuNPs/PNS hybrid materials with high photothermal conversion efficiency. The findings demonstrate that 2D PNS enhances the overall photothermal therapy effect of the nanohybrid materials due to their larger hosting area for AuNPs and higher biocompatibility. The well-designed amphiphilic peptides in this study offer insights into the structural design and functional modulation of self-assembled molecules. In addition, the constructed biomimetic-functional 2D inorganic/organic nanohybrid materials hold potential applications in biomedical engineering.
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  • 文章类型: Journal Article
    银(Ag)的回收对生态保护至关重要,人类健康和经济效益。由于吸附剂的可接近位点不足,从废水中有效捕获Ag(I)仍然具有挑战性。在这里,开发了一种酰氯介导的策略来合成罗丹宁(Rd)修饰的UiO-66衍生物,用于Ag(I)吸附。得益于Rd的高接枝密度,最佳的Rd修饰的UiO-66-NH2(UiO-66-NH2@20Rd)具有超高的吸收能力(最大容量为923.9mg·g-1)和对Ag(I)的选择性(最大选择性系数为1665.52)。在UiO-66-NH2@20Rd上,几乎90%的Ag(I)可以在一分钟内被捕获,并且即使在六个循环之后仍保持98.9%的去除率。此外,固定床柱测试表明,可以有效处理约21,780床体积的Ag(I)模拟废水,表明有很大的实际应用前景。机理研究表明,出色的性能可归因于Ag(I)在致密的罗丹宁位点上的吸附和还原的协同作用。这项研究强调,这种一般策略可以为各种功能吸附材料提供有价值的途径。
    Silver (Ag) recovery is essential for ecological protection, human health and economic benefits. Effective capture of Ag(I) from wastewater is still challenging due to insufficient accessible sites of adsorbents. Herein, an acyl chloride-mediated strategy is developed to synthesize rhodanine (Rd) modified UiO-66 derivatives for Ag(I) adsorption. Benefitting from the high grafting density of Rd, the optimal Rd-modified UiO-66-NH2 (UiO-66-NH2@20Rd) features an ultra-high uptake capacity (maximum capacity of 923.9 mg·g-1) and selectivity (maximum selectivity coefficient of 1665.52) for Ag(I). Almost 90 % of Ag(I) could be captured in one minute over UiO-66-NH2@20Rd and maintained a removal rate of 98.9 % even after six cycles. Moreover, a fixed-bed column test demonstrates that approximately 21,780 bed volumes of Ag(I) simulated wastewater can be effectively treated, indicating great promise for practical application. Mechanism investigation illustrates that outstanding performance can be attributed to the synergistic effect of Ag(I) adsorption and reduction on dense rhodanine sites. This study highlights that such a general strategy can provide a valuable avenue toward various functional adsorption materials.
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  • 文章类型: Journal Article
    作为多种农药常用的合成材料,硫醇化合物,一旦被泄露,会对环境和人类造成严重危害。因此,巯基化合物的高效检测至关重要。在这项研究中,开发了一种开启荧光探针(Cu@Zn-CP)用于高度敏感的巯基化合物的荧光检测。该探针是基于锌配位聚合物(Zn-CP)构建的,其荧光通过Cu2+离子的有效掺杂而猝灭。引入巯基乙酸甲酯(MTC)后,在90s内产生快速的荧光开启响应,低检测限为23ppb。即使重复使用五个周期,该传感器保持优异的检测性能,并表现出良好的可回收性。它还可以检测河水中的MTC,加标回收率在98-103%之间。此外,设计的Cu@Zn-CP对检测多种硫醇化合物具有良好的通用性,包括L-半胱氨酸,谷胱甘肽,单硫代甘油,和2-羟基-1-乙硫醇。该结果为硫醇化合物提供了潜在的可回收荧光传感器。
    As a kind of commonly-used synthetic materials for many pesticides, thiol compounds, once being leaked, can cause serious harm to the environment and humans. Therefore, the efficient detection of thiol compounds is essential. In this study developed a turn-on fluorescent probe (Cu@Zn-CP) for the highly sensitive fluorescence detection of thiol compounds. The probe was constructed based on a zinc coordination polymer (Zn-CP), whose fluorescence was quenched through the effective doping of Cu2+ ions. After the introduction of methyl thioglycolate (MTC), a rapid fluorescence turn-on response was generated within 90 s with a low detection limit of 23 ppb. Even after being reused for five cycles, the sensor maintains excellent detection performance and demonstrates good recyclability. It can also detect MTC in river water, with a spike recovery rate between 98-103 %. Furthermore, the designed Cu@Zn-CP exhibits good universality for detecting multifarious thiol compounds, including L-cysteine, glutathione, monothioglycerol, and 2-hydroxy-1-ethanethiol. This result provides a potential recyclable fluorescent sensor for thiol compounds.
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  • 文章类型: Journal Article
    合成均匀的功能共价有机骨架(COFs)微球是将COFs用作液相色谱的新型固定相的前提。然而,由于在赋予功能时难以维持微球形态,因此官能化COFs微球的合成具有挑战性。这里,我们开发了一种简单而通用的“自限动态接头交换”策略,以实现均匀COFs微球的表面官能化。构造了六种不同类型的COFs微球,显示了该战略的普遍性和优越性。COF微球固定相库可以根据需要通过改变不同的功能构建块来进一步丰富。“自限动态接头交换”归因于反应热力学和分子扩散能垒的微妙平衡。作为一个示范,手性功能性COFs微球作为手性色谱的固定相,实现了有效的对映体分离。本文受版权保护。保留所有权利。
    Synthesizing uniform functional covalent organic framework (COF) microspheres is the prerequisite of applying COFs as novel stationary phases for liquid chromatography. However, the synthesis of functionalized COF microspheres is challenging due to the difficulty in maintaining microspheric morphology when conferring functions. Here, a facile and universal \"self-limited dynamic linker exchange\" strategy is developed to achieve surface functionalization of uniform COF microspheres. Six different types of COF microspheres are constructed, showing the universality and superiority of the strategy. The library of COF microspheres\' stationary phases can be further enriched on demand by varying different functional building blocks. The \"self-limited dynamic linker exchange\" is attributed to the result of a delicate balance of reaction thermodynamics and molecular diffusion energy barrier. As a demonstration, the chiral functional COF microspheres are used as stationary phases of chiral chromatography and realized effective enantioseparation.
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  • 文章类型: Journal Article
    工业排放的有机废水造成的环境污染已经成为一个世界性的问题,对公众和生态系统构成了严重威胁。金属有机骨架(MOFs),包含含金属簇和有机桥接配体,是多孔和结晶材料,拥有迷人的形状和尺寸相关的特性,如高表面积,丰富的活性位点,定义明确的晶体形态,以及表面功能化的巨大潜力。迄今为止,许多精心指定的MOF已经成为关键的功能材料,以解决与水环境问题相关的日益增长的挑战。在这里,我们介绍了MOF基材料的最新进展及其在有机废水处理中的应用。首先,介绍了MOF复合材料的几种传统和新兴的合成策略。然后,提出并分析了MOF复合材料的结构和功能规律。最后,MOF基材料在处理有机废水中的典型应用,包括化学,Pharmaceutical,纺织品,并对农业废水进行了总结。总的来说,这项审查预计将定制设计和监管基于MOF的功能材料,以提高有机废水治理的性能。
    Environmental pollution caused by organic effluents emitted by industry has become a worldwide issue and poses a serious threat to the public and the ecosystem. Metal-organic frameworks (MOFs), comprising metal-containing clusters and organic bridging ligands, are porous and crystalline materials, possessing fascinating shape and size-dependent properties such as high surface area, abundant active sites, well-defined crystal morphologies, and huge potential for surface functionalization. To date, numerous well designated MOFs have emerged as critical functional materials to solve the growing challenges associated with water environmental issues. Here we present the recent progress of MOF-based materials and their applications in the treatment of organic effluents. Firstly, several traditional and emerging synthesis strategies for MOF composites are introduced. Then, the structural and functional regulations of MOF composites are presented and analyzed. Finally, typical applications of MOF-based materials in treating organic effluents, including chemical, pharmaceutical, textile, and agricultural wastewaters are summarized. Overall, this review is anticipated to tailor design and regulation of MOF-based functional materials for boosting the performance of organic effluent remediation.
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