functionalization

Functionalization
  • 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
    可见光介导的反应最近已成为在温和反应条件下合成多种有机分子的有力策略。通常,反应在室温下进行,因此敏感官能团保持不受影响。因此,该协议受到了学术界和工业界的强烈兴趣。杂环,总的来说,由于它们的生物活性和在治疗中的应用而引起了极大的兴趣。含氧和含硫杂环化合物最近引起了人们的关注,因为这些化合物显示出作为抗癌药物的有希望的活性,抗生素,抗真菌和抗炎药在其他应用。通过有效和更绿色的途径合成这类化合物已成为重要的目标。这篇综述强调了在可见光诱导的反应下合成这些化合物及其衍生物的各种程序。讨论了每个程序的绿色方面和机制。
    Visible-light-mediated reactions have recently emerged as a powerful strategy for the synthesis of diverse organic molecules under mild reaction conditions. Usually, the reactions are performed at room temperature and thus sensitive functional groups remain unaffected. Thus, this protocol has received intense interest from academia as well as industries. The heterocycles, in general, are of much interest because of their biological activities and application in therapeutics. The Oxygen- and Sulfur-containing heterocyclic compounds have recently attracted attention as these compounds showed promising activities as anti-cancer drugs, antibiotics, antifungal and anti-inflammatory agents among other applications. The synthesis of this class of compounds by efficient and greener routes has become an important target. This review highlights the various procedures for the synthesis of these compounds and their derivatives under visible light-induced reactions. The green aspects and mechanism of each procedure have been discussed.
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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
    两亲性嵌段共聚物是制造具有同孔整体不对称结构的超滤膜的有希望的候选物。膜通常通过嵌段共聚物自组装和非溶剂诱导的相分离(SNIPS)方法的组合来制造,从而产生同孔整体不对称膜。当然,所有这些膜缺乏热和化学稳定性,限制了这些材料的使用。在这项研究中,完全交联的多孔整体不对称嵌段共聚物膜的制造通过UV交联得到化学和热稳定的超滤膜证明。PVBCB-b-P4VP(聚(4-乙烯基苯并环丁烯)-b-聚(4-乙烯基吡啶))嵌段共聚物膜的UV交联过程取决于辐照时间,强度,膜和紫外线源之间的距离和波长进行了研究。此外,表明,在进行紫外线交联之前,可以通过将膜浸入波导溶液中来增加渗透深度。此外,一种全新的和容易的交联策略是基于等折变溶剂开发的热和化学稳定的膜,通过整个膜厚度交联。最后,等折变溶液中的新交联策略被转移到商业PVDF和PAN-co-PVC聚合物膜,为更稳定和可持续的超滤膜铺平了道路。
    Amphiphilic block copolymers are promising candidates for the fabrication of ultrafiltration membranes with an isoporous integral asymmetric structure. The membranes are typically fabricated by the combination of block copolymer self-assembly and the non-solvent-induced phase separation (SNIPS) process resulting in isoporous integral asymmetric membranes. Certainly, all these membranes lack thermal and chemical stability limiting the usage of such materials. Within this study, the fabrication of completely cross-linked isoporous integral asymmetric block copolymer membranes is demonstrated by UV cross-linking resulting in chemical and thermal stable ultrafiltration membranes. The UV cross-linking process of PVBCB-b-P4VP (poly(4-vinylbenzocyclobutene)-b-poly(4vinylpyridine)) block copolymer membranes in dependency of irradiation time, intensity, distance between membrane and UV source and the wavelength is investigated. Furthermore, it is shown that the penetration depths can be increased by soaking the membranes in wave-guiding solutions before UV cross-linking is carried out. Moreover, a completely new and easy cross-linking strategy is developed based on isorefractive solvents resulting in thermal and chemically stable membranes that are cross-linked through the whole membrane thickness. Finally, the new cross-linking strategy in isorefractive solutions is transferred to commercial PVDF and PAN-co-PVC polymer membranes paving the way for more stable and sustainable ultrafiltration membranes.
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  • 文章类型: Journal Article
    这项研究调查了垂直排列的二硫化钼纳米结构(VA-MoS2)与Ag纳米颗粒(NP)和氮官能化的同时装饰。使用氮气作为反应气体,通过物理气相沉积(PVD)直流磁控溅射实现氮气功能化,旨在诱导MoS2中的p型行为。利用反应溅射导致MoS2表面上三维银结构的生长,促进银纳米颗粒的形成。进行了全面表征以评估表面改性并分析化学和结构变化。X射线光电子能谱(XPS)显示在MoS2表面上存在银。扫描电子显微镜(SEM)证实了银纳米颗粒的成功装饰,表明沉积时间影响银在MoS2表面上的尺寸和分布。
    This study investigates the simultaneous decoration of vertically aligned molybdenum disulfide nanostructure (VA-MoS2) with Ag nanoparticles (NPs) and nitrogen functionalization. Nitrogen functionalization was achieved through physical vapor deposition (PVD) DC-magnetron sputtering using nitrogen as a reactive gas, aiming to induce p-type behavior in MoS2. The utilization of reactive sputtering resulted in the growth of three-dimensional silver structures on the surface of MoS2, promoting the formation of silver nanoparticles. A comprehensive characterization was conducted to assess surface modifications and analyze chemical and structural changes. X-ray photoelectron spectroscopy (XPS) showed the presence of silver on the MoS2 surface. Scanning electron microscopy (SEM) confirmed successful decoration with silver nanoparticles, showing that deposition time affects the size and distribution of the silver on the MoS2 surface.
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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
    成功开发了来自Lehensis芽孢杆菌G1(Combi-CLEAs-CM)的环糊精葡聚糖转移酶(CGTase)和麦芽糖淀粉酶(Mag1)的组合交联酶聚集体,以合成麦芽寡糖(MOS)。然而,壳聚糖(交联剂)和酶之间的交联性能差,导致活性恢复和催化效率低。在这项研究中,我们提出了结合计算分析的交联剂的功能化,以研究不同官能团对combi-CLEA开发中交联剂的影响。从硅分析来看,选择对两种酶具有最高结合亲和力的O-羧甲基壳聚糖(OCMCS),并显示与实验结果一致。其中合成了OCMCS作为交联剂,以提高Combi-CLEAs-CM-ocmcs的活性回收率(74%)。发现Combi-CLEAs-CM-ocmcs的热稳定性和失活能(205.86kJ/mol)高于Combi-CLEAs-CM(192.59kJ/mol)。羧甲基基团的较长侧链的引入导致Combi-CLEAs-CM-ocmcs的更灵活的结构。与Combi-CLEAs-CM相比,这种改变使Combi-CLEAs-CM-ocmcs的Km值显着降低了约3.64倍,并导致更高的Kcat/Km(高3.63倍)。此外,Combi-CLEAs-CM-ocmcs提高了可重用性,保留了>50%的活性,而Combi-CLEAs-CM在五个周期后仅占36.18%。最后,使用响应面法优化后,Combi-CLEAs-CM-ocmcs获得了最大MOS产量(777.46mg/g)。
    Combined cross-linked enzyme aggregates of cyclodextrin glucanotransferase (CGTase) and maltogenic amylase (Mag1) from Bacillus lehensis G1 (Combi-CLEAs-CM) were successfully developed to synthesis maltooligosaccharides (MOS). Yet, the poor cross-linking performance between chitosan (cross-linker) and enzymes resulting low activity recovery and catalytic efficiency. In this study, we proposed the functionalization of cross-linkers with the integration of computational analysis to study the influences of different functional group on cross-linkers in combi-CLEAs development. From in-silico analysis, O-carboxymethyl chitosan (OCMCS) with the highest binding affinity toward both enzymes was chosen and showed alignment with the experimental result, in which OCMCS was synthesized as cross-linker to develop improved activity recovery of Combi-CLEAs-CM-ocmcs (74 %). The thermal stability and deactivation energy (205.86 kJ/mol) of Combi-CLEAs-CM-ocmcs were found to be higher than Combi-CLEAs-CM (192.59 kJ/mol). The introduction of longer side chain of carboxymethyl group led to a more flexible structure of Combi-CLEAs-CM-ocmcs. This alteration significantly reduced the Km value of Combi-CLEAs-CM-ocmcs by about 3.64-fold and resulted in a greater Kcat/Km (3.63-fold higher) as compared to Combi-CLEAs-CM. Moreover, Combi-CLEAs-CM-ocmcs improved the reusability with retained >50 % of activity while Combi-CLEAs-CM only 36.18 % after five cycles. Finally, maximum MOS production (777.46 mg/g) was obtained by Combi-CLEAs-CM-ocmcs after optimization using response surface methodology.
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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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  • 文章类型: Journal Article
    吸附是去除持久性有机污染物(POPs)的一种有前途的方法,一个重大的环境问题。它们的高孔隙率和广阔的表面积,MOF由于其优异的吸附能力而适合于POP去除。这篇综述讨论了MOF介导的吸附的复杂原理,并有助于将来减轻有机水污染的尝试。这篇综述探讨了MOF介导的吸附的复杂概念,包括MOF合成方法,吸附机制,以及材料的可调性和适应性。MOFs通过静电力吸附POPs的能力,酸碱相互作用,氢键,并详细阐述了pi-pi相互作用。这篇综述证明了它在消除许多类型的污染物方面的多功能性。Functionalizing,添加金属纳米颗粒,或在创建后更改MOF可以提高其性能并去除污染物。本文还讨论了基于MOF的污染物去除问题和未来前景,包括吸附能力,选择性,扩大实际应用,稳定性,和恢复。这些障碍可以通过合理设计MOFs来克服,开发复合材料,并改善材料的生产和表征。总的来说,MOF技术研究和创新为环境污染解决方案和可持续修复带来了巨大的希望。MOFs中的解吸和再生也包括在审查中,以及提高污染物去除效率和可持续性的方法。讨论了有效的MOF再生和扩大实际部署的案例研究,以及解决这些障碍的未来想法。
    Adsorption is a promising way to remove persistent organic pollutants (POPs), a major environmental issue. With their high porosity and vast surface areas, MOFs are suited for POP removal due to their excellent adsorption capabilities. This review addresses the intricate principles of MOF-mediated adsorption and helps to future attempts to mitigate organic water pollution. This review examines the complicated concepts of MOF-mediated adsorption, including MOF synthesis methodologies, adsorption mechanisms, and material tunability and adaptability. MOFs\' ability to adsorb POPs via electrostatic forces, acid-base interactions, hydrogen bonds, and pi-pi interactions is elaborated. This review demonstrates its versatility in eliminating many types of contaminants. Functionalizing, adding metal nanoparticles, or changing MOFs after they are created can improve their performance and remove contaminants. This paper also discusses MOF-based pollutant removal issues and future prospects, including adsorption capacity, selectivity, scale-up for practical application, stability, and recovery. These obstacles can be overcome by rationally designing MOFs, developing composite materials, and improving material production and characterization. Overall, MOF technology research and innovation hold considerable promise for environmental pollution solutions and sustainable remediation. Desorption and regeneration in MOFs are also included in the review, along with methods for improving pollutant removal efficiency and sustainability. Case studies of effective MOF regeneration and scaling up for practical deployment are discussed, along with future ideas for addressing these hurdles.
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