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Proteins for Applied and Functional Materials. 用于应用和功能材料的蛋白质。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-18 DOI: 10.1021/acs.biomac.4c00884
Antonio J Capezza, Raffaele Mezzenga

Shifting from a petroleum-based plastic society to a newer one built on circular economy principles requires maximizing the use of renewable resources and resolving the challenges that come with their use. Biopolymers have taken an important role in the design of biobased materials with functional properties, especially those derived from biomass available at a large scale. A number of recent studies have shown how proteins have a new dimension in developing functional materials, taking a step forward from their traditional use in food and biomedicine. Correlating the amino acidic profile of proteins at the nanoscale with their thermomechanical properties at the macroscale enables us to translate these precision polymers into a versatile design of materials, targeting large-scale applications such as foams and food packaging. Moreover, the advances in understanding proteins from a bottom-up perspective reached promising achievements for their use in applications that were not foreseen before, including biosensors, optoelectronics, and semiconductors.

要从以石油为基础的塑料社会转向以循环经济原则为基础的新型社会,就必须最大限度地利用可再生资源,并解决使用这些资源所带来的挑战。生物聚合物在设计具有功能特性的生物基材料方面发挥了重要作用,特别是那些从可大规模获得的生物质中提取的材料。最近的一些研究表明,蛋白质在开发功能材料方面有了新的发展,比其在食品和生物医学方面的传统用途向前迈进了一步。在纳米尺度上将蛋白质的氨基酸谱与它们在宏观尺度上的热力学特性联系起来,使我们能够将这些精密聚合物转化为多用途的材料设计,瞄准泡沫和食品包装等大规模应用。此外,从自下而上的角度理解蛋白质所取得的进展,为蛋白质在生物传感器、光电子学和半导体等前所未见的应用领域的应用带来了希望。
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引用次数: 0
Glycoside Phosphorylase Catalyzed Cellulose and β-1,3-Glucan Synthesis Using Chromophoric Glycosyl Acceptors. 糖苷磷酸化酶催化的纤维素和 β-1,3-葡聚糖合成(使用色素糖基受体)。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-18 DOI: 10.1021/acs.biomac.4c00455
Robert Pylkkänen, Hannu Maaheimo, Ville Liljeström, Pezhman Mohammadi, Merja Penttilä

Glycoside phosphorylases are enzymes that are frequently used for polysaccharide synthesis. Some of these enzymes have broad substrate specificity, enabling the synthesis of reducing-end-functionalized glucan chains. Here, we explore the potential of glycoside phosphorylases in synthesizing chromophore-conjugated polysaccharides using commercially available chromophoric model compounds as glycosyl acceptors. Specifically, we report cellulose and β-1,3-glucan synthesis using 2-nitrophenyl β-d-glucopyranoside, 4-nitrophenyl β-d-glucopyranoside, and 2-methoxy-4-(2-nitrovinyl)phenyl β-d-glucopyranoside with Clostridium thermocellum cellodextrin phosphorylase and Thermosipho africanus β-1,3-glucan phosphorylase as catalysts. We demonstrate activity for both enzymes with all assayed chromophoric acceptors and report the crystallization-driven precipitation and detailed structural characterization of the synthesized polysaccharides, i.e., their molar mass distributions and various structural parameters, such as morphology, fibril diameter, lamellar thickness, and crystal form. Our results provide insights for the studies of chromophore-conjugated low molecular weight polysaccharides, glycoside phosphorylases, and the hierarchical assembly of crystalline cellulose and β-1,3-glucan.

糖苷磷酸化酶是一种常用于多糖合成的酶。其中一些酶具有广泛的底物特异性,能够合成还原端功能化的葡聚糖链。在此,我们探讨了糖苷磷酸化酶在使用市售的发色团模型化合物作为糖基受体合成发色团共轭多糖方面的潜力。具体来说,我们以热梭菌纤维糊精磷酸化酶和非洲嗜热菌β-1,3-葡聚糖磷酸化酶为催化剂,使用 2-硝基苯基β-d-吡喃葡萄糖苷、4-硝基苯基β-d-吡喃葡萄糖苷和 2-甲氧基-4-(2-硝基乙烯基)苯基β-d-吡喃葡萄糖苷合成纤维素和β-1,3-葡聚糖。我们证明了这两种酶在所有检测的发色受体上的活性,并报告了结晶驱动的沉淀和合成多糖的详细结构特征,即它们的摩尔质量分布和各种结构参数,如形态、纤维直径、薄片厚度和晶形。我们的研究结果为研究发色团共轭低分子量多糖、糖苷磷酸化酶以及结晶纤维素和β-1,3-葡聚糖的分层组装提供了启示。
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引用次数: 0
Nanoassemblies of Chitosan-Based Polyelectrolyte Complexes as Nucleic Acid Delivery Systems. 壳聚糖聚电解质复合物的纳米组合作为核酸输送系统。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-18 DOI: 10.1021/acs.biomac.4c00054
Hussein H Genedy, Thierry Delair, Pierre Alcouffe, Agnès Crépet, Elodie Chatre, Khair Alhareth, Alexandra Montembault

Nucleic acid delivery requires vectorization for protection from nucleases, preventing clearance by the reticuloendothelial system, and targeting to allow cellular uptake. Nanovectors meeting the above specifications should be safe for the patient, simple to manufacture, and display long-term stability. Our nanovectors were obtained via the green process of polyelectrolyte complexation, carried out at 25 °C in water at a low shear rate using chitosan (a polycationic biocompatible polysaccharide of specific molar mass and acetylation degree) and dextran sulfate as a polyanionic biocompatible polysaccharide. These complexes formed nanoassemblies of primary nanoparticles (20-35 nm) and maintained their colloidal stability for over 1 year at 25 °C. They could be steam sterilized, and a model nucleic acid could be either encapsulated or surface adsorbed. A targeting agent was finally bound to their surface. This work serves as a proof of concept of the suitability of chitosan-based polyelectrolyte complexes as nanovectors by sequential multilayered adsorption of various biomacromolecules.

核酸递送需要载体化,以防止核酸酶的破坏,防止被网状内皮系统清除,并具有靶向性,使细胞能够吸收。符合上述规格的纳米载体应该对患者安全、制造简单并具有长期稳定性。我们的纳米载体是通过多电解质复合物的绿色工艺获得的,该工艺在 25 °C 的水中以低剪切速率进行,使用壳聚糖(一种具有特定摩尔质量和乙酰化程度的多阳离子生物相容性多糖)和硫酸葡聚糖(一种多阴离子生物相容性多糖)。这些复合物形成了原生纳米颗粒(20-35 纳米)的纳米集合体,并在 25 °C 下保持胶体稳定性超过 1 年。它们可以进行蒸汽灭菌,模型核酸可以被包裹或表面吸附。最终,一种靶向药剂被结合到了它们的表面。这项工作证明了壳聚糖基聚电解质复合物通过多层顺序吸附各种生物大分子作为纳米载体的适用性。
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引用次数: 0
Electrophoretically Snagging Viral Genomes in Wormlike Micelle Networks Using Peptide Nucleic Acid Amphiphiles and dsDNA Oligomers. 利用多肽核酸虹吸体和 dsDNA 寡聚体在蠕虫状胶束网络中电泳捕捉病毒基因组
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-17 DOI: 10.1021/acs.biomac.4c00332
Kimberly Hui, Lingxiao Yan, James W Schneider

We demonstrate that the attachment of 30-170 bp dsDNA oligomers to ssDNA viral genomes gives a significant additional mobility shift in micelle-tagging electrophoresis (MTE). In MTE, a modified peptide nucleic acid amphiphile is attached to the viral genome to bind drag-inducing micelles present in capillary electrophoresis running buffers. Further attachment of 30-170 bp dsDNA oligomers drastically shifts the mobility of the 5.1 kB ssDNA genome of mouse minute virus (MMV), providing a new mechanism to improve resolution in CE-based analysis of kilobase nucleic acids. A model based on biased-reptation electrophoresis, end-labeled free-solution electrophoresis, and Ferguson gel-filtration theory is presented to describe the observed mobility shifts.

我们证明,在胶束标记电泳(MTE)中,30-170 bp dsDNA 寡聚体附着在 ssDNA 病毒基因组上会产生显著的额外迁移率变化。在胶束标记电泳(MTE)中,病毒基因组上附有改良的肽核酸双亲化合物,可与毛细管电泳运行缓冲液中的拖曳诱导胶束结合。30-170 bp dsDNA 寡聚体的进一步附着极大地改变了小鼠细小病毒(MMV)5.1 kB ssDNA 基因组的迁移率,为提高基于 CE 的千碱基核酸分析的分辨率提供了一种新机制。该研究提出了一个基于偏倚回复电泳、末端标记自由溶液电泳和弗格森凝胶过滤理论的模型,用以描述观察到的迁移率变化。
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引用次数: 0
Permselectivity of Silk Fibroin Hydrogels for Advanced Drug Delivery Neurotherapies. 蚕丝纤维素水凝胶用于先进给药神经疗法的选择性。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-17 DOI: 10.1021/acs.biomac.4c00629
Rocío Fernández-Serra, Amira Lekouaghet, Lorena Peracho, Mahdi Yonesi, Alberto Alcázar, Mourad Chioua, José Marco-Contelles, José Pérez-Rigueiro, Francisco J Rojo, Fivos Panetsos, Gustavo V Guinea, Daniel González-Nieto

A promising trend in tissue engineering is using biomaterials to improve the control of drug concentration in targeted tissue. These vehicular systems are of specific interest when the required treatment time window is higher than the stability of therapeutic molecules in the body. Herein, the capacity of silk fibroin hydrogels to release different molecules and drugs in a sustained manner was evaluated. We found that a biomaterial format, obtained by an entirely aqueous-based process, could release molecules of variable molecular weight and charge with a preferential delivery of negatively charged molecules. Although the theoretical modeling suggested that drug delivery was more likely to be driven by Fickian diffusion, the external media had a considerable influence on the release, with lipophilic organic solvents such as acetonitrile-methanol (ACN-MeOH) intensifying the release of hydrophobic molecules. Second, we found that silk fibroin could be used as a vehicular system to treat a variety of brain disorders as this biomaterial sustained the release of different factors with neurotrophic (brain-derived neurotrophic factor) (BDNF), chemoattractant (C-X-C motif chemokine 12) (CXCL12), anti-inflammatory (TGF-β-1), and angiogenic (VEGF) capacities. Finally, we demonstrated that this biomaterial hydrogel could release cholesteronitrone ISQ201, a nitrone with antioxidant capacity, showing neuroprotective activity in an in vitro model of ischemia-reoxygenation. Given the slow degradation rate shown by silk fibroin in many biological tissues, including the nervous system, our study expands the restricted list of drug delivery-based biomaterial systems with therapeutic capacity for both short- and especially long-term treatment windows and has merit for use with brain pathologies.

组织工程学中一个很有前途的趋势是利用生物材料来改善靶组织中药物浓度的控制。当所需的治疗时间窗口高于治疗分子在体内的稳定性时,这些载体系统就会受到特别关注。在这里,我们评估了丝纤维水凝胶持续释放不同分子和药物的能力。我们发现,通过完全基于水的工艺获得的生物材料形式可以释放不同分子量和电荷的分子,并优先释放带负电荷的分子。虽然理论建模表明药物释放更可能是由菲氏扩散驱动的,但外部介质对释放有相当大的影响,乙腈-甲醇(ACN-MeOH)等亲油性有机溶剂会加强疏水性分子的释放。其次,我们发现丝纤维素可用作治疗各种脑部疾病的载体系统,因为这种生物材料能持续释放不同的因子,包括神经营养因子(脑源性神经营养因子)(BDNF)、趋化吸引因子(C-X-C motif趋化因子12)(CXCL12)、抗炎因子(TGF-β-1)和血管生成因子(VEGF)。最后,我们证明这种生物材料水凝胶可以释放胆固醇硝酮 ISQ201,这是一种具有抗氧化能力的硝酮,在体外缺血缺氧模型中显示出神经保护活性。鉴于蚕丝纤维素在包括神经系统在内的许多生物组织中降解速度较慢,我们的研究扩大了具有短期、特别是长期治疗能力的药物输送型生物材料系统的范围,并有望用于脑部病变。
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引用次数: 0
Mechanism of Cationic Lipid Induced DNA Condensation: Lipid-DNA Coordination and Divalent Cation Charge Fluctuations. 阳离子脂质诱导 DNA 缩合的机理:脂质-DNA配位和二价阳离子电荷波动。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-16 DOI: 10.1021/acs.biomac.4c00192
Weiwei He, Serdal Kirmizialtin

The condensation of nucleic acids by lipids is a widespread phenomenon in biology with crucial implications for drug delivery. However, the mechanisms of DNA assembly in lipid bilayers remain insufficiently understood due to challenges in measuring and assessing each component's contribution in the lipid-DNA-cation system. This study uses all-atom molecular dynamics simulations to investigate DNA condensation in cationic lipid bilayers. Our exhaustive exploration of the thermodynamic factors reveals unique roles for phospholipid head groups and cations. We observed that bridging cations between lipid and DNA drastically reduce charges, while mobile magnesium cations "ping-ponging" between double strands create charge fluctuations. While the first factor stabilizes the DNA-lipid complex, the latter creates attractive forces to induce the spontaneous condensation of DNAs. This novel mechanism not only sheds light on the current data regarding cationic lipid-induced DNA condensation but also provides potential design strategies for creating efficient gene delivery vectors for drug delivery.

核酸被脂质凝结是生物学中的一种普遍现象,对药物输送具有重要影响。然而,由于难以测量和评估脂质-DNA-阳离子系统中每种成分的贡献,人们对 DNA 在脂质双分子层中的组装机制仍然了解不足。本研究利用全原子分子动力学模拟来研究阳离子脂质双分子层中的 DNA 凝聚。我们对热力学因素的详尽探索揭示了磷脂头基和阳离子的独特作用。我们观察到,脂质和 DNA 之间的桥接阳离子会大幅降低电荷,而在双链之间 "乒乓 "作响的移动镁阳离子则会产生电荷波动。前一个因素稳定了 DNA 脂质复合物,而后一个因素则产生了吸引力,诱导 DNA 自发凝结。这一新机制不仅揭示了目前有关阳离子脂质诱导 DNA 凝聚的数据,还为创建高效的基因递送载体提供了潜在的药物递送设计策略。
{"title":"Mechanism of Cationic Lipid Induced DNA Condensation: Lipid-DNA Coordination and Divalent Cation Charge Fluctuations.","authors":"Weiwei He, Serdal Kirmizialtin","doi":"10.1021/acs.biomac.4c00192","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c00192","url":null,"abstract":"<p><p>The condensation of nucleic acids by lipids is a widespread phenomenon in biology with crucial implications for drug delivery. However, the mechanisms of DNA assembly in lipid bilayers remain insufficiently understood due to challenges in measuring and assessing each component's contribution in the lipid-DNA-cation system. This study uses all-atom molecular dynamics simulations to investigate DNA condensation in cationic lipid bilayers. Our exhaustive exploration of the thermodynamic factors reveals unique roles for phospholipid head groups and cations. We observed that bridging cations between lipid and DNA drastically reduce charges, while mobile magnesium cations \"ping-ponging\" between double strands create charge fluctuations. While the first factor stabilizes the DNA-lipid complex, the latter creates attractive forces to induce the spontaneous condensation of DNAs. This novel mechanism not only sheds light on the current data regarding cationic lipid-induced DNA condensation but also provides potential design strategies for creating efficient gene delivery vectors for drug delivery.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":null,"pages":null},"PeriodicalIF":5.5,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Experimental Correlation between Apparent pKa and Gelation Propensity in Amphiphilic Hydrogelators Derived from l-Dopa. 由 l-Dopa 制成的两性水凝胶的表观 pKa 与凝胶倾向之间的实验相关性。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-16 DOI: 10.1021/acs.biomac.4c00470
Fabia Cenciarelli, Silvia Pieraccini, Stefano Masiero, Giuseppe Falini, Demetra Giuri, Claudia Tomasini

We report the gelation propensity of three gelators derived from l-dihydroxyphenylalanine (l-Dopa), where the amino group is derivatized with three different fatty acids (lauric acid, palmitic acid, and azelaic acid). The long aliphatic side chains should introduce additional van der Waals interactions among the molecules, contributing to the self-assembly process. The hydrogels have been prepared with the pH change method, and both the hydrogels and the corresponding aerogels have been analyzed using several techniques. In any case, Lau-Dopa provides stronger hydrogels compared with the other gelators. This property may be ascribed to its tendency to efficiently form supramolecular β-sheet structures, as outlined by the ECD, IR, and SEM analyses. Moreover, the preliminary measurement of the apparent pKa displays for Lau-Dopa two plateaux, as previously observed for, one at about pH 12 and a second one at pH 7.5. Thus, its pKa results in two apparent pKa shifts of ∼8.5 and ∼4 pH units above the theoretical pKa, as a consequence of a multistep self-assembly pathway that correlates, in the final β-sheet-based hydrogel, with a high degree of order and stability.

我们报告了从 l-二羟基苯丙氨酸(l-Dopa)中提取的三种凝胶剂的凝胶化倾向,其中氨基被三种不同的脂肪酸(月桂酸、棕榈酸和壬二酸)衍生。长的脂肪族侧链会在分子间引入额外的范德华相互作用,从而促进自组装过程。水凝胶是用改变 pH 值的方法制备的,水凝胶和相应的气凝胶都使用了多种技术进行分析。无论如何,与其他凝胶剂相比,Lau-Dopa 能提供更强的水凝胶。正如 ECD、红外和扫描电镜分析所显示的那样,这种特性可能是由于它能有效地形成超分子 β 片状结构。此外,对表观 pKa 的初步测量显示,Lau-Dopa 具有两个高原,正如以前观察到的那样,一个在 pH 值约为 12 时,另一个在 pH 值为 7.5 时。因此,它的表观 pKa 比理论 pKa 分别高出 8.5 和 4 个 pH 单位,这是多步自组装途径的结果,在最终的 β 片基水凝胶中,这与高度的有序性和稳定性相关。
{"title":"Experimental Correlation between Apparent p<i>K</i><sub>a</sub> and Gelation Propensity in Amphiphilic Hydrogelators Derived from l-Dopa.","authors":"Fabia Cenciarelli, Silvia Pieraccini, Stefano Masiero, Giuseppe Falini, Demetra Giuri, Claudia Tomasini","doi":"10.1021/acs.biomac.4c00470","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c00470","url":null,"abstract":"<p><p>We report the gelation propensity of three gelators derived from l-dihydroxyphenylalanine (l-Dopa), where the amino group is derivatized with three different fatty acids (lauric acid, palmitic acid, and azelaic acid). The long aliphatic side chains should introduce additional van der Waals interactions among the molecules, contributing to the self-assembly process. The hydrogels have been prepared with the pH change method, and both the hydrogels and the corresponding aerogels have been analyzed using several techniques. In any case, Lau-Dopa provides stronger hydrogels compared with the other gelators. This property may be ascribed to its tendency to efficiently form supramolecular β-sheet structures, as outlined by the ECD, IR, and SEM analyses. Moreover, the preliminary measurement of the apparent p<i>K</i><sub>a</sub> displays for Lau-Dopa two plateaux, as previously observed for, one at about pH 12 and a second one at pH 7.5. Thus, its p<i>K</i><sub>a</sub> results in two apparent p<i>K</i><sub>a</sub> shifts of ∼8.5 and ∼4 pH units above the theoretical p<i>K</i><sub>a</sub>, as a consequence of a multistep self-assembly pathway that correlates, in the final β-sheet-based hydrogel, with a high degree of order and stability.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":null,"pages":null},"PeriodicalIF":5.5,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141625311","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modulating the Thermoresponsive Characteristics of PLGA-PEG-PLGA Hydrogels via Manipulation of PLGA Monomer Sequences. 通过操纵 PLGA 单体序列调节 PLGA-PEG-PLGA 水凝胶的热致伸缩特性。
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-16 DOI: 10.1021/acs.biomac.4c00817
SeongHoon Jo, Soonjong Roh, Jaemin Shim, Ji Woong Yu, Youngmee Jung, Woo Young Jang, Bumjoon Seo, You-Yeon Won, Jin Yoo

Hydrogels are promising materials for biomedical applications, particularly in drug delivery and tissue engineering. This study highlights thermoresponsive hydrogels, specifically poly(lactic-co-glycolic acid) (PLGA)-poly(ethylene glycol) (PEG)-PLGA triblock copolymers, and introduces a feed rate-controlled polymerization (FRCP) method. By utilizing an organic catalyst and regulating the monomer feed rate, the sequence distribution of PLGA within the triblock copolymer is controlled. Various analyses, including 13C NMR and rheological measurements, were conducted to investigate the impact of sequence distribution. Results show that altering sequence distribution significantly influences the sol-gel transition, hydrophobicity-hydrophilicity balance, and drug release profile. Increased sequence uniformity lowers the glass transition temperature, raises the sol-gel transition temperature due to enhanced hydrophilicity, and promotes a more uniform drug (curcumin) distribution within the PLGA domain, resulting in a slower release rate. This study emphasizes the importance of PLGA sequence distribution in biomedical applications and the potential of FRCP to tailor thermoresponsive hydrogels for biomedical advancements.

水凝胶是一种很有前景的生物医学应用材料,尤其是在药物输送和组织工程方面。本研究重点关注热致伸缩性水凝胶,特别是聚(乳酸-共-乙醇酸)(PLGA)-聚(乙二醇)(PEG)-PLGA 三嵌段共聚物,并介绍了一种进料速率控制聚合(FRCP)方法。通过使用有机催化剂和调节单体进料速率,可以控制 PLGA 在三嵌段共聚物中的序列分布。为了研究序列分布的影响,进行了各种分析,包括 13C NMR 和流变测量。结果表明,改变序列分布会显著影响溶胶-凝胶转变、疏水性-亲水性平衡和药物释放曲线。增加序列的均匀性可降低玻璃化转变温度,由于亲水性增强而提高溶胶-凝胶转变温度,并促进药物(姜黄素)在 PLGA 结构域内更均匀的分布,从而降低释放速率。这项研究强调了 PLGA 序列分布在生物医学应用中的重要性,以及 FRCP 为生物医学进步定制热致伸缩性水凝胶的潜力。
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引用次数: 0
Preparation of Multifunctional Hydrogels with In Situ Dual Network Structure and Promotion of Wound Healing. 制备具有原位双网络结构的多功能水凝胶并促进伤口愈合
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-15 DOI: 10.1021/acs.biomac.4c00403
Yapeng Lu, Maojie Hu, Yikai Huang, Jianwei Liao, Meihui Zhao, Yang Zhou, Guanghua Xia, Qiping Zhan

As an emerging biomedical material, wound dressings play an important therapeutic function in the process of wound healing. It can provide an ideal healing environment while protecting the wound from a complex external environment. A hydrogel wound dressing composed of tilapia skin gelatin (Tsg) and fucoidan (Fuc) was designed in this article to enhance the microenvironment of wound treatment and stimulate wound healing. By mixing horseradish peroxidase (HRP), hydrogen peroxide (H2O2), tilapia skin gelatin-tyramine (Tsg-Tyr), and carboxylated fucoidan-tyramine in agarose (Aga), using the catalytic cross-linking of HRP/H2O2 and the sol-gel transformation of Aga, a novel gelatin-fucoidan (TF) double network hydrogel wound dressing was constructed. The TF hydrogels have a fast and adjustable gelation time, and the addition of Aga further enhances the stability of the hydrogels. Moreover, Tsg and Fuc are coordinated with each other in terms of biological efficacy, and the TF hydrogel demonstrated excellent antioxidant properties and biocompatibility in vitro. Also, in vivo wound healing experiments showed that the TF hydrogel could effectively accelerate wound healing, reduce wound microbial colonization, alleviate inflammation, and promote collagen deposition and angiogenesis. In conclusion, TF hydrogel wound dressings have the potential to replace traditional dressings in wound healing.

作为一种新兴的生物医学材料,伤口敷料在伤口愈合过程中发挥着重要的治疗功能。它既能提供理想的愈合环境,又能保护伤口免受复杂外部环境的影响。本文设计了一种由罗非鱼皮明胶(Tsg)和褐藻糖胶(Fuc)组成的水凝胶伤口敷料,以改善伤口治疗的微环境并刺激伤口愈合。通过将辣根过氧化物酶(HRP)、过氧化氢(H2O2)、罗非鱼皮明胶-酪胺(Tsg-Tyr)和琼脂糖(Aga)中的羧化褐藻糖胶-酪胺混合,利用HRP/H2O2的催化交联和Aga的溶胶-凝胶转化,构建了一种新型明胶-褐藻糖胶(TF)双网络水凝胶伤口敷料。TF 水凝胶的凝胶时间快且可调,加入 Aga 后进一步提高了水凝胶的稳定性。此外,Tsg 和 Fuc 在生物功效方面相互协调,TF 水凝胶在体外表现出优异的抗氧化性和生物相容性。此外,体内伤口愈合实验表明,TF 水凝胶能有效加速伤口愈合,减少伤口微生物定植,缓解炎症,促进胶原沉积和血管生成。总之,TF 水凝胶伤口敷料有望在伤口愈合中取代传统敷料。
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引用次数: 0
Harnessing Cytosine for Tunable Nanoparticle Self-Assembly Behavior Using Orthogonal Stimuli. 利用胞嘧啶,使用正交刺激实现可调控的纳米粒子自组装行为
IF 5.5 2区 化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Pub Date : 2024-07-15 DOI: 10.1021/acs.biomac.4c00352
Sam J Parkinson, Stephen D P Fielden, Marjolaine Thomas, Alisha J Miller, Paul D Topham, Matthew J Derry, Rachel K O'Reilly

Nucleobases control the assembly of DNA, RNA, etc. due to hydrogen bond complementarity. By combining these unique molecules with state-of-the-art synthetic polymers, it is possible to form nanoparticles whose self-assembly behavior could be altered under orthogonal stimuli (pH and temperature). Herein, we report the synthesis of cytosine-containing nanoparticles via aqueous reversible addition-fragmentation chain transfer polymerization-induced self-assembly. A poly(N-acryloylmorpholine) macromolecular chain transfer agent (mCTA) was chain-extended with cytosine acrylamide, and a morphological phase diagram was constructed. By exploiting the ability of cytosine to form dimers via hydrogen bonding, the self-assembly behavior of cytosine-containing polymers was altered when performed under acidic conditions. Under these conditions, stable nanoparticles could be formed at longer polymer chain lengths. Furthermore, the resulting nanoparticles displayed different morphologies compared to those at pH 7. Additionally, particle stability post-assembly could be controlled by varying pH and temperature. Finally, small-angle X-ray scattering was performed to probe their dynamic behavior under thermal cycling.

核碱基通过氢键互补性控制 DNA、RNA 等的组装。通过将这些独特的分子与最先进的合成聚合物相结合,可以形成纳米粒子,其自组装行为可在正交刺激(pH 值和温度)下发生改变。在此,我们报告了通过水性可逆加成-断裂链转移聚合诱导自组装合成含胞嘧啶纳米粒子的情况。我们用胞嘧啶丙烯酰胺对聚(N-丙烯酰吗啉)大分子链转移剂(mCTA)进行了链延伸,并构建了形态相图。利用胞嘧啶通过氢键形成二聚体的能力,含胞嘧啶聚合物在酸性条件下的自组装行为发生了改变。在这些条件下,可以在聚合物链长度较长的情况下形成稳定的纳米颗粒。此外,通过改变 pH 值和温度,还可以控制纳米粒子组装后的稳定性。最后,还进行了小角 X 射线散射,以探测它们在热循环下的动态行为。
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引用次数: 0
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