Microgels

微凝胶
  • 文章类型: Journal Article
    基于刺激响应性聚(N-乙烯基己内酰胺)(PVCL)的微凝胶,可以对微小的外部环境变化做出反应,在生物医学和纳米技术领域引起了极大的兴趣。然而,由于其低的掺入效率和热响应性钝化,此类微凝胶的制备遇到了严峻的挑战。为了解决这些问题,我们选择3-(叔丁氧羰基)-N-乙烯基己内酰胺(TBVCL),羧基官能化的VCL衍生物,作为共聚单体开发pH/温度双响应微凝胶。TBVCL,具有类似于VCL的结构,提高掺入效率和胶体稳定性,同时减少热响应性钝化。微凝胶的体积相变温度(VPTT)可以在宽范围(19.0-49.5°C)内调节。值得注意的是,微凝胶的径向溶胀率可以通过pH调节,实现3的最大溶胀比。在不同温度或pH条件下溶解-沉淀行为的不同变化使得这些微凝胶适用于诸如智能窗户和传感器的应用。此外,这种制造具有pH可调相变温度的微凝胶的新方法证明了纳米颗粒控释的重要潜力(例如,毒品,催化剂,和量子点)以及智能纳米晶体-聚合物复合传感器的开发。
    Stimuli-responsive poly(N-vinylcaprolactam) (PVCL)-based microgels, which could response to small external environmental changes, have attracted great interests in the fields of biomedicine and nanotechnology. However, the preparation of such microgels meets severe challenge due to their low incorporation efficiency and thermoresponsivity passivation. To address these issues, we select 3-(tert-butoxycarbonyl)-N-vinylcaprolactam (TBVCL), a carboxyl-functionalized VCL derivative, as a comonomer to develop pH/temperature dual-responsive microgels. TBVCL, with a structure similar to VCL, enhances incorporation efficiency and colloidal stability, while reducing thermoresponsivity passivation. The volume phase transition temperature (VPTT) of the microgels can be adjusted over a broad range (19.0-49.5 °C). Notably, the radial swelling ratios of the microgels can be modulated by pH, achieving a maximum swelling ratio of 3. The distinct changes in dissolution-precipitation behavior under different temperatures or pH conditions make these microgels suitable for applications such as smart windows and sensors. Furthermore, this novel approach for fabricating microgels with pH-tunable phase-transition temperatures demonstrates significant potential for the controlled release of nanoparticles (e.g., drugs, catalysts, and quantum dots) and the development of smart nanocrystal-polymer composite sensors.
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  • 文章类型: Journal Article
    微凝胶递送系统在功能性物质包封方面具有巨大的潜力,保护,释放,精准分娩和营养干预。微凝胶是生物聚合物通过物理或化学交联形成的三维网络结构,其特征包括分散和溶胀,结构稳定,小体积和高比表面积,是一种特殊的胶体。在这一章中,制备食品级微凝胶的常用墙体材料,以及主要的准备原则,方法,首先综述了负载功能物质的微凝胶的优缺点。然后分析了微凝胶作为给药系统的主要特点,例如可变形性,高封装,刺激响应释放和靶向递送,并总结了其在干预慢性病方面的潜在益处。最后,讨论了功能物质微凝胶缓释系统在精准营养领域的应用。本章将有助于设计下一代先进的靶向微凝胶给药系统,实现食品功能性物质对机体健康的精准营养干预。
    Microgels delivery system have great potential in functional substances encapsulation, protection, release, precise delivery and nutritional intervention. Microgel is a three-dimensional network structure formed by physical or chemical crosslinking of biopolymers, whose characteristics include dispersion and swelling, stable structure, small volume and high specific surface area, and is a special kind of colloid. In this chapter, the common wall materials for preparing food grade microgels, and the main preparation principles, methods, advantages and disadvantages of microgels loaded with functional substances were firstly reviewed. Then the main characteristics of microgel as delivery system, such as deformability, high encapsulation, stimulus-responsive release and targeted delivery, and its potential benefits in intervening chronic diseases were summarized. Finally, the applications of microgel delivery system for functional substance in the field of precision nutrition were discussed. This chapter will help to design of next-generation advanced targeting microgel delivery system, and realize precision nutrition intervention of food functional substances on body health.
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  • 文章类型: Journal Article
    氧化铝负载的PtSn是一种工业化的丙烷脱氢催化剂。在催化剂浸渍过程中,以氯铂酸为前驱体的酸性浸渍溶液不可避免地导致两性氧化铝载体表面的部分溶解,最终改变催化性能。在这里,活动相的结构演变,由浸渍的酸性溶液诱导,被特别小心地研究。根据扩散双层理论,我们提出了浸渍过程中微凝胶的模型。通过在干燥和煅烧过程中的再沉淀,在催化剂表面上具有合适酸度的溶液中形成的微凝胶演变成Al2O3包覆的氧化Pt的结构。覆盖的Pt物质可以通过Ar+溅射暴露或在还原过程中迁移到表面以用作丙烷脱氢的活性位点。值得注意的是,当浸渍溶液的pH为约0.56时,产生表面Sn0物质,这对于存在于Sn-Al2O3载体表面上的SnOx物质上的PtSn合金存在的独特活性相是坚实的证明。合成的催化剂具有高的丙烯选择性(99.4%)和优异的稳定性(kd=0.002h-1)。本研究为Pt/Sn-Al2O3催化剂的精确制备提供了新的思路。
    Alumina-supported PtSn is an industrialized catalyst for propane dehydrogenation. During the catalyst impregnation, the acidic impregnation solution with chloroplatinic acid as a precursor inevitably leads to the partial dissolution of the surface of amphoteric alumina support and finally varies catalytic performance. Herein, the structure evolution of the active phase, induced by an impregnated acidic solution, was studied with special care. According to the diffused double layer theory, we proposed a model of microgels during impregnation. The microgels formed in the solution with suitable acidity on the surface of the catalysts evolved into a structure of Al2O3-coated oxidized Pt by reprecipitation during drying and calcination. The covered Pt species could be exposed by Ar+ sputtering or migrate to the surface during reduction to serve as active sites for propane dehydrogenation. Noticeably, the surface Sn0 species was generated when the pH of the impregnated solution was around 0.56, which is solid proof for the unique active phase with the PtSn alloy present on SnOx species existing on the surface of the Sn-Al2O3 support. The synthesized catalyst exhibited high propylene selectivity (99.4%) and superior stability (kd = 0.002 h-1). This study provides new insight for the precise preparation of Pt/Sn-Al2O3 catalysts.
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  • 文章类型: Journal Article
    本研究旨在研究界面层组成和结构对形成的影响,Pickering乳液的理化性质和稳定性。使用豌豆蛋白分离物(PPI)形成界面层,PPI微凝胶颗粒(PPIMP),PPIMP和海藻酸钠(PPIMP-SA)的混合物,或PPIMP-SA缀合物。然后在这些Pickering乳液中评估对不同疏水性生物活性物质的包封和保护作用。结果表明,PPIMP-SA结合物在油滴表面周围形成了厚而坚固的界面层,这增加了乳液对聚结的抵抗力,乳化液,和环境压力,包括加热,曝光,和冻融循环。此外,通过PPIMP-SA缀合物稳定的乳液显着提高了疏水性生物活性物质的光热稳定性,与非封装形式相比,保留了较高百分比的原始含量。总的来说,本研究开发的新型蛋白质微凝胶和缀合物具有提高乳化食品理化稳定性的巨大潜力。
    This study aims to investigate the effects of interfacial layer composition and structure on the formation, physicochemical properties and stability of Pickering emulsions. Interfacial layers were formed using pea protein isolate (PPI), PPI microgel particles (PPIMP), a mixture of PPIMP and sodium alginate (PPIMP-SA), or PPIMP-SA conjugate. The encapsulation and protective effects on different hydrophobic bioactives were then evaluated within these Pickering emulsions. The results demonstrated that the PPIMP-SA conjugate formed thick and robust interfacial layers around the oil droplet surfaces, which increased the resistance of the emulsion to coalescence, creaming, and environmental stresses, including heating, light exposure, and freezing-thawing cycle. Additionally, the emulsion stabilized by the PPIMP-SA conjugate significantly improved the photothermal stability of hydrophobic bioactives, retaining a higher percentage of their original content compared to those in non-encapsulated forms. Overall, the novel protein microgels and the conjugate developed in this study have great potential for improving the physicochemical stability of emulsified foods.
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  • 文章类型: Journal Article
    基于肿瘤球体的以往癌症研究的精度,特别是包裹微凝胶的肿瘤球体,受到肿瘤球体大小和形状高度异质性的限制。这里,我们报道了一种用户友好的基于电磁阀的分选器,以减少这种异质性。采用人工智能算法对肿瘤球体进行实时检测和分割,进行大小和形状计算。提出了一种简单的基于芯片外电磁阀的分选驱动模块,用于分选具有所需尺寸和形状的目标肿瘤球体。利用开发的分拣机,我们成功地发现了相同人群但不同大小和形状的肺肿瘤球状体对顺铂的药物反应变化。此外,有了这个分拣机,球体群体水平的药物测试精度提高到与精确但复杂的单个球体分析相当的水平。开发的分选机还具有用于精密医学研究的类器官形态学和分选的巨大潜力。
    The precision of previous cancer research based on tumor spheroids, especially the microgel-encapsulating tumor spheroids, was limited by the high heterogeneity in the tumor spheroid size and shape. Here, we reported a user-friendly solenoid valve-based sorter to reduce this heterogeneity. The artificial intelligence algorithm was employed to detect and segmentate the tumor spheroids in real-time for the size and shape calculation. A simple off-chip solenoid valve-based sorting actuation module was proposed to sort out target tumor spheroids with the desired size and shape. Utilizing the developed sorter, we successfully uncovered the drug response variations on cisplatin of lung tumor spheroids in the same population but with different sizes and shapes. Moreover, with this sorter, the precision of drug testing on the spheroid population level was improved to a level comparable to the precise but complex single spheroid analysis. The developed sorter also exhibits significant potential for organoid morphology and sorting for precision medicine research.
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  • 文章类型: Journal Article
    大豆壳多糖(SHP)表现出优异的界面活性,并具有作为乳液乳化剂的潜力。为了揭示SHP在水/油(W/O)界面的原位行为,在这项研究中使用了分子动力学(MD)模拟和粒子跟踪微流变。MD的结果表明,SHP分子自发地向界面移动,鼠李糖半乳糖醛酸-I启动这种运动,而其上的半乳糖醛酸作为锚将SHP分子固定在W/O界面。微流变学结果表明,SHP在W/O界面形成微凝胶,微凝胶的晶格不断发生动态变化。在低浓度的SHP和短的界面形成时间,微凝胶的网络是弱的并且由粘性性质主导。然而,当SHP达到0.75%,界面形成时间约为60分钟时,微凝胶显示出完美的弹性,这有利于稳定乳液。
    The soy hull polysaccharide (SHP) exhibits excellent interfacial activity and holds potential as an emulsifier for emulsions. To reveal the behavior of SHP at the water/oil (W/O) interface in situ, molecular dynamics (MD) simulations and particle tracking microrheology were used in this study. The results of MD reveal that SHP molecular spontaneously move toward the interface and rhamnogalacturonan-I initiates this movement, while its galacturonic acids on it act as anchors to immobilize the SHP molecules at the W/O interface. Microrheology results suggest that SHP forms microgels at the W/O interface, with the lattices of the microgels continually undergoing dynamic changes. At low concentrations of SHP and short interfacial formation time, the network of the microgels is weak and dominated by viscous properties. However, when SHP reaches 0.75 % and the interfacial formation time is about 60 min, the microgels show perfect elasticity, which is beneficial for stabilizing emulsions.
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  • 文章类型: Journal Article
    熟练处理糖尿病伤口,随着糖尿病病例的全球升级,造成重大的临床困难。已经设计并生产了一系列生物功能敷料以加快糖尿病伤口的愈合过程。这项研究提出了一种用于糖尿病伤口愈合的多功能水凝胶敷料,由聚乙烯醇(PVA)和N1-(4-硼苄基)-N3-(4-硼苯基)-N1,N1,N3,N3-三甲基丙烷-1,3-二胺(TSPBA)组成,和双载药明胶甲基丙烯酰基(GM)微凝胶。GM微凝胶装载有夫西酸钠(SF)和含有盐酸二甲双胍(MH)的纳米脂质体(LP)。值得注意的是,水凝胶的粘附性和自修复性增强了它们的治疗潜力和易于应用。体外评估表明,注入SF的水凝胶可以在24小时内消除98%以上的细菌,并在15天内保持持续释放。此外,在超过15天的持续时间内,在水凝胶内掺入的MH已经证明了有效的葡萄糖水平调节。水凝胶在整个愈合过程中表现出中和ROS的持续能力,主要通过电子捐赠和隔离。这种多功能水凝胶敷料,整合了对MSSA和MRSA菌株的有效杀菌活性的生物学功能,血糖调节,控制活性氧水平,在14天内成功促进了大鼠糖尿病伤口的愈合。水凝胶敷料在促进糖尿病伤口的愈合过程中表现出显著的有效性,突出了其临床翻译的巨大前景。
    The proficient handling of diabetic wounds, a rising issue coinciding with the global escalation of diabetes cases, poses significant clinical difficulties. A range of biofunctional dressings have been engineered and produced to expedite the healing process of diabetic wounds. This study proposes a multifunctional hydrogel dressing for diabetic wound healing, which is composed of Polyvinyl Alcohol (PVA) and N1-(4-boronobenzyl)-N3-(4-boronophenyl)-N1, N1, N3, N3-teramethylpropane-1, 3-diaminium (TSPBA), and a dual-drug loaded Gelatin methacryloyl (GM) microgel. The GM microgel is loaded with sodium fusidate (SF) and nanoliposomes (LP) that contain metformin hydrochloride (MH). Notably, adhesive and self-healing properties the hydrogel enhance their therapeutic potential and ease of application. In vitro assessments indicate that SF-infused hydrogel can eliminate more than 98% of bacteria within 24 h and maintain a sustained release over 15 days. Additionally, MH incorporated within the hydrogel has demonstrated effective glucose level regulation for a duration exceeding 15 days. The hydrogel demonstrates a sustained ability to neutralize ROS throughout the entire healing process, predominantly by electron donation and sequestration. This multifunctional hydrogel dressing, which integrated biological functions of efficient bactericidal activity against both MSSA and MRSA strains, blood glucose modulation, and control of active oxygen levels, has successfully promoted the healing of diabetic wounds in rats in 14 days. The hydrogel dressing exhibited significant effectiveness in facilitating the healing process of diabetic wounds, highlighting its considerable promise for clinical translation.
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  • 文章类型: Journal Article
    目的:在分子尺度上工程化基于植物的微凝胶颗粒(MPs)对于制备功能性脂肪类似物是有意义的。我们假设燕麦分离蛋白(OPI)和κ-角叉菜胶(CA)在MPs形成中具有协同作用,使用具有可控结构的MP,进一步制备具有可调节特性的脂肪类似物是可行的。它们的消化命运也可能受到界面涂层的调节。
    方法:设计了基于OPI的共轭MPs,通过改变交联密度具有可调的刚度。微凝胶结构之间的关系,并通过光谱学研究了乳液凝胶的性质,微观结构,流变学和摩擦学。交付番茄红素,在模拟胃肠道中评估了脂肪类似物的抑制消化行为。
    结果:可以调整共轭MPs的刚性以优化脂肪类似物的性能。OPI-1%CAMPs可以稳定乳液高达95%的油分,质地细腻。摩擦学行为依赖于微凝胶弹性和界面涂层,口服后,中等硬MP稳定的乳剂破裂较少,没有聚结。通过软化界面颗粒层或限制脂肪酶的可及性,较致密和较硬的MP延迟了消化。较软的共轭MP具有更好的柔韧性,并且更容易分解,从而导致更高的脂质消化率。
    OBJECTIVE: Engineering plant-based microgel particles (MPs) at a molecular scale is meaningful to prepare functional fat analogues. We hypothesize that oat protein isolate (OPI) and κ-carrageenan (CA) have synergy in MPs formation, using MPs with controllable structure, and further to fabricate fat analogues with adjustable characteristics is feasible. Their digestion fate will also be possibly modulated by interfacial coatings.
    METHODS: OPI-based conjugated MPs with tunable rigidities by changing crosslinking densities were designed. The relationship between microgel structures, and emulsion gel properties was explored through spectroscopy, microstructure, rheology and tribology. The delivery to lycopene, as well as inhibiting digestion behaviors of fat analogues was evaluated in a simulated gastro-intestinal tract.
    RESULTS: The rigidity of conjugated MPs could be tailored to optimize the performance of fat analogues. OPI-1 %CA MPs could stabilize emulsions up to 95 % oil fraction with fine texture. Tribological behaviors had a dependence on microgel elasticity and interfacial coatings, medium hard MP-stabilized emulsion was less disrupted without coalescence after oral processing. Digestion was delayed by denser and harder MPs by softening the interfacial particle layer or limiting lipase accessibility. Softer conjugated MPs possessed better flexibility and were broken down more easily leading to a higher rate of lipid digestion.
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  • 文章类型: Journal Article
    通过顺序促进止血的综合伤口护理,密封,治疗在临床实践中有着巨大的希望。然而,由于难以适应动态机械和湿伤口环境,常规生物粘合剂实现动态伤口的综合护理仍然具有挑战性。在这里,我们报道了一种脱水,物理双交联微凝胶(DPDMs)能够原位形成高度可拉伸,用于动态伤口综合护理的可压缩和组织粘附水凝胶。通过将可逆交联和双交联合理地整合到微粉化凝胶中来设计DPDM。可逆的物理交联使DPDM能够集成在一起,和双重交联特性进一步加强形成的宏观网络(DPDM-凝胶)。我们证明了DPDM凝胶同时具有出色的拉伸(~940kJ/m3)和压缩(~270kJ/m3)韧性,商业生物粘合剂-可比的组织粘附强度,在数百种变形下性能稳定。体内实验结果进一步表明,DPDM-Gels在各种出血模型中均能有效止血,即使在实际的动态环境中,并实现动态皮肤伤口的综合护理。基于卓越的机械性能和适当的粘合性能,加上令人印象深刻的综合护理能力,DPDM凝胶可以为动态伤口的智能护理提供新的方法。重要声明:动态伤口的综合护理在临床实践中具有重要意义。然而,动态和潮湿的伤口环境对现有的水凝胶实现它提出了巨大的挑战。这项工作开发了强大的粘合剂水凝胶,用于通过设计脱水来综合护理动态伤口,物理双交联微凝胶(DPDMs)。可逆和双交联使DPDMs能够整合到具有高机械性能的宏观水凝胶中,适当的粘合强度和稳定的性能在数百种外部变形。在受伤部位申请时,DPDM凝胶有效止血,即使在实际的动态环境中,在动态伤口的综合护理中也显示出有效性。有了迷人的特性,DPDMs可能成为智能伤口护理的有效工具。
    Integrated wound care through sequentially promoting hemostasis, sealing, and healing holds great promise in clinical practice. However, it remains challenging for regular bioadhesives to achieve integrated care of dynamic wounds due to the difficulties in adapting to dynamic mechanical and wet wound environments. Herein, we reported a type of dehydrated, physical double crosslinked microgels (DPDMs) which were capable of in situ forming highly stretchable, compressible and tissue-adhesive hydrogels for integrated care of dynamic wounds. The DPDMs were designed by the rational integration of the reversible crosslinks and double crosslinks into micronized gels. The reversible physical crosslinks enabled the DPDMs to integrate together, and the double crosslinked characteristics further strengthen the formed macroscopical networks (DPDM-Gels). We demonstrated that the DPDM-Gels simultaneously possess outstanding tensile (∼940 kJ/m3) and compressive (∼270 kJ/m3) toughness, commercial bioadhesives-comparable tissue-adhesive strength, together with stable performance under hundreds of deformations. In vivo results further revealed that the DPDM-Gels could effectively stop bleeding in various bleeding models, even in an actual dynamic environment, and enable the integrated care of dynamic skin wounds. On the basis of the remarkable mechanical and appropriate adhesive properties, together with impressive integrated care capacities, the DPDM-Gels may provide a new approach for the smart care of dynamic wounds. STATEMENT OF SIGNIFICANCE: Integrated care of dynamic wounds holds great significance in clinical practice. However, the dynamic and wet wound environments pose great challenges for existing hydrogels to achieve it. This work developed robust adhesive hydrogels for integrated care of dynamic wounds by designing dehydrated, physical double crosslinked microgels (DPDMs). The reversible and double crosslinks enabled DPDMs to integrate into macroscopic hydrogels with high mechanical properties, appropriate adhesive strength and stable performance under hundreds of external deformations. Upon application at the injury site, DPDM-Gels efficiently stopped bleeding, even in an actual dynamic environment and showed effectiveness in integrated care of dynamic wounds. With the fascinating properties, DPDMs may become an effective tool for smart wound care.
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  • 文章类型: Journal Article
    由天然或合成水凝胶材料制备的微凝胶作为多功能细胞或药物载体,这对组织工程和再生医学很有希望。微凝胶也可以聚集成微孔支架,促进细胞浸润和增殖,促进组织修复。本文概述了微凝胶的制造技术和应用的最新进展。一系列常规和新颖的策略,包括乳化,微流体,平版印刷术,电喷射,离心,气体剪切,三维生物打印,等。进行了深入的讨论。阐述了用于细胞培养和递送的微凝胶和基于微凝胶的支架的特性和应用,并强调了这些载体在细胞治疗中的优势。此外,我们阐述了微凝胶及其聚集体在生物医学工程领域中正在进行的和可预见的应用以及当前的局限性。通过激发创新思想,本综述为扩大微凝胶在细胞递送技术中的应用开辟了新的途径。
    Microgels prepared from natural or synthetic hydrogel materials have aroused extensive attention as multifunctional cells or drug carriers, that are promising for tissue engineering and regenerative medicine. Microgels can also be aggregated into microporous scaffolds, promoting cell infiltration and proliferation for tissue repair. This review gives an overview of recent developments in the fabrication techniques and applications of microgels. A series of conventional and novel strategies including emulsification, microfluidic, lithography, electrospray, centrifugation, gas-shearing, three-dimensional bioprinting, etc. are discussed in depth. The characteristics and applications of microgels and microgel-based scaffolds for cell culture and delivery are elaborated with an emphasis on the advantages of these carriers in cell therapy. Additionally, we expound on the ongoing and foreseeable applications and current limitations of microgels and their aggregate in the field of biomedical engineering. Through stimulating innovative ideas, the present review paves new avenues for expanding the application of microgels in cell delivery techniques.
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