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Biodegradable photocatalytic film based on chia seed mucilage (xylose, glucose, and methyl glucuronic acid polysaccharides) containing barberry extract and SnO2 nanoparticles 基于奇异籽粘液(木糖、葡萄糖和甲基葡萄糖醛酸多糖)的可生物降解光催化薄膜,其中含有巴桑提取物和二氧化硒纳米颗粒
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-29 DOI: 10.1016/j.carpta.2024.100592
Shirin Forouzan , Sajad Pirsa , Abolfazl Alirezalu
In this study, chia seed mucilage (CSM) was extracted and used to prepare biodegradable film. The prepared film was modified with barberry extract (Ex) and tin oxide (SnO2) nanoparticles (NPs). According to the obtained results, barberry extract significantly increased the thickness of the film, while tin oxide nanoparticles affected the thickness very little. Adding nanoparticles to the film decreased both the tensile strength and flexibility of the film. Barberry extract increased the tensile strength and flexibility of the film. Barberry extract and tin oxide nanoparticles decreased the permeability to water vapor in the films. Barberry extract and tin oxide nanoparticles both increased the antioxidant property of the film. The addition of barberry extract and tin oxide nanoparticles significantly increased the antibacterial properties of the film against both Staphylococcus aureus and Escherichia coli bacteria. Physical connections and electrostatic interactions between composite components were confirmed by Fourier transform infrared (FTIR) spectra. The X-ray diffraction (XRD) results showed the positive effect of tin oxide nanoparticles in the formation of the crystal structure of the composite film. Additives of extract and nanoparticle increased the thermal stability of the film. The mucilage film with the highest percentage of tin oxide nanoparticles up to 50 % caused the photocatalytic degradation of methylene blue.
本研究提取了奇异籽粘液(CSM)并用于制备生物降解薄膜。在制备的薄膜上添加了巴桑子提取物(Ex)和氧化锡纳米颗粒(NPs)。结果表明,桑葚提取物明显增加了薄膜的厚度,而纳米氧化锡颗粒对薄膜厚度的影响很小。在薄膜中添加纳米粒子会降低薄膜的拉伸强度和柔韧性。桑葚提取物提高了薄膜的拉伸强度和柔韧性。桑葚提取物和纳米氧化锡粒子降低了薄膜的水蒸气渗透性。桑葚提取物和纳米氧化锡粒子都提高了薄膜的抗氧化性。添加了桑葚提取物和纳米氧化锡颗粒后,薄膜对金黄色葡萄球菌和大肠杆菌的抗菌性能明显提高。傅立叶变换红外光谱(FTIR)证实了复合成分之间的物理连接和静电作用。X 射线衍射(XRD)结果表明,氧化锡纳米粒子对复合薄膜晶体结构的形成具有积极作用。提取物和纳米颗粒的添加增加了薄膜的热稳定性。纳米氧化锡颗粒比例最高的粘液膜达到了 50%,可对亚甲蓝进行光催化降解。
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引用次数: 0
A computational probe into the physicochemical properties of cyclodextrin-based deep eutectic solvents for extraction processes 基于环糊精的深共晶溶剂在萃取过程中的物理化学特性计算探究
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-29 DOI: 10.1016/j.carpta.2024.100596
Parisa Jahanbakhsh-Bonab , Zahra Khoshnazar , Jaber Jahanbin Sardroodi , Ehsan Heidaryan
The use of deep eutectic solvents (DESs) as environmentally friendly alternatives to traditional volatile organic solvents has attracted significant attention in the industrial sector. In this study, molecular dynamics simulations were utilized to examine the physicochemical and structural characteristics of novel DESs—specifically DES1, DES2, and DES3—comprising methyl-β-cyclodextrin (MBCD) mixed with formic acid (FA), propionic acid (PA), and acetic acid (AA), respectively, in a 1:3 molar ratio. Structural analysis, as revealed by the combined distribution function and radial distribution function, indicated that the dominant interactions within the DESs occur between the hydroxyl hydrogen of the acids and the hydroxyl oxygen of MBCD, as well as between the hydroxyl hydrogen of MBCD and the carbonyl oxygen of the acids. Furthermore, it was observed that MBCD forms more hydrogen bonds and non-bonded interactions with PA than with FA or AA. As a result, PA exhibits a lower self-diffusion coefficient compared to FA and AA. The findings also demonstrate that the influence of the acid type on the density and isothermal compressibility of the DESs follows the order: DES2 > DES1 > DES3 for density and DES3 > DES2 > DES1 for compressibility. Overall, this study provides valuable insights into the behavior of novel MBCD-based DESs, offering predictive insights for their potential applications in extraction processes.
深共晶溶剂(DES)作为传统挥发性有机溶剂的环保型替代品,在工业领域备受关注。本研究利用分子动力学模拟研究了新型 DES 的物理化学和结构特征,特别是 DES1、DES2 和 DES3,它们分别由甲基-β-环糊精(MBCD)与甲酸(FA)、丙酸(PA)和乙酸(AA)以 1:3 的摩尔比混合而成。综合分布函数和径向分布函数显示的结构分析表明,DES 内部的主要相互作用发生在酸的羟基氢和 MBCD 的羟基氧之间,以及 MBCD 的羟基氢和酸的羰基氧之间。此外,还观察到 MBCD 与 PA 形成的氢键和非键相互作用多于与 FA 或 AA 形成的氢键和非键相互作用。因此,与 FA 和 AA 相比,PA 的自扩散系数较低。研究结果还表明,酸类型对 DES 的密度和等温压缩性的影响遵循以下顺序:密度为 DES2 > DES1 > DES3,压缩性为 DES3 > DES2 > DES1。总之,这项研究为了解基于 MBCD 的新型 DES 的行为提供了宝贵的见解,为其在萃取过程中的潜在应用提供了预测性的见解。
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引用次数: 0
A structural investigation on the interactions of cotton fabric cellulose with olive oil and water 棉织物纤维素与橄榄油和水相互作用的结构研究
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-19 DOI: 10.1016/j.carpta.2024.100590
Andriani Tsompou , Peter Falkman , Ann Terry , Vitaly Kocherbitov
The cotton fabric consists of cellulose arranged in a complex structure with multiple levels of organization at different length scales. Understanding this structure and its interactions with water and oil is essential for developing efficient and environmentally friendly methods of cotton washing. In this study, the structure of raw cotton fabric cellulose and the effects of water and oil were examined across a broad range of length scales using spatially resolved synchrotron small-angle X-ray scattering (SAXS) and auxiliary techniques.
Water was observed to penetrate the cotton fabric and interact across nearly all length scales. Although a certain amount of the material was not affected by water as seen by intact distance between microfibrils, fractal analysis of the scattering data indicated a loosening of the microfibril arrangement after contact with water. This process was hindered if the material had been pre-treated with oil and was not seen after subsequent washing with water or surfactant solution. Analyzing spatially resolved SAXS data using a bi-sinusoidal model and 2D maps of the oil-to-cotton ratio facilitates understanding the structure of the material and its interactions with oil on the molecular, nano and macrolevels.
棉织物由纤维素组成,其结构复杂,在不同长度尺度上具有多层次的组织结构。了解这种结构及其与水和油的相互作用对于开发高效、环保的棉布洗涤方法至关重要。在这项研究中,利用空间分辨同步加速器小角 X 射线散射(SAXS)和辅助技术,在广泛的长度尺度范围内研究了原棉织物纤维素的结构以及水和油的影响。虽然从微纤维之间的完整距离可以看出,一定量的材料不受水的影响,但对散射数据的分形分析表明,微纤维的排列在与水接触后会变得松散。如果材料预先用油处理过,这一过程就会受到阻碍,而且在随后用水或表面活性剂溶液清洗后也不会出现这种情况。使用双正弦曲线模型和油棉比二维图分析空间分辨 SAXS 数据有助于了解材料的结构及其与油在分子、纳米和宏观层面上的相互作用。
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引用次数: 0
Cellulose-based photocatalytic membranes for dye degradation: A review 用于染料降解的纤维素基光催化膜:综述
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-15 DOI: 10.1016/j.carpta.2024.100589
Medhanit Tefera Yifira , Anteneh Kindu Mersha , Gebrehiwot Gebreslassie , Kebede Nigussie Mekonnen
Clean drinking water has been a challenge due to the pollution from industrialization, urbanization, the growing global population, and lack of infrastructure. Textile industry waste has become a major problem due to wastewater that contains dyes commonly discharged into the water bodies. Wastewater-containing dye should be treated to avoid undesired environmental effects. Among the various water treatment methods, photocatalysis has been getting growing attention in mitigating water pollution issues, particularly in removing organic contaminants (such as organic dyes) due to their good efficiency, low cost, and environmental friendliness. Organic-inorganic composites such as combinations of cellulose and semiconductors can produce unique functional hybrid materials with tailored characteristics. Cellulose has been used as a carrier material due to its superfine network structure, reactive surface groups, and good compatibility with metal oxides. In addition to increasing the catalyst surface area, it improves the photocatalytic effectiveness of nanocomposites by acting as electron acceptors and transporters resulting in a better charge carrier separation. Therefore, cellulose-based photocatalytic membranes are environmentally friendly, fully biodegradable, and biocompatible with efficient applications in wastewater management for the degradation of organic dyes. In this review work, the applications of cellulose-based photocatalytic membranes for the removal of cationic and anionic organic dyes have been reviewed.
由于工业化、城市化、全球人口增长和基础设施缺乏造成的污染,清洁饮用水一直是一个挑战。由于含有染料的废水通常被排放到水体中,纺织业废物已成为一个主要问题。含染料的废水应加以处理,以避免对环境造成不良影响。在各种水处理方法中,光催化技术因其高效、低成本和环保性,在缓解水污染问题,特别是去除有机污染物(如有机染料)方面日益受到关注。有机-无机复合材料,如纤维素和半导体的组合,可以产生具有定制特性的独特功能性混合材料。纤维素因其超细网络结构、活性表面基团以及与金属氧化物的良好兼容性而被用作载体材料。除了增加催化剂的表面积外,纤维素还可作为电子受体和传输体,改善电荷载体的分离,从而提高纳米复合材料的光催化效果。因此,纤维素基光催化膜对环境友好,可完全生物降解,且具有生物相容性,可有效应用于废水管理中有机染料的降解。本综述综述了纤维素基光催化膜在去除阳离子和阴离子有机染料方面的应用。
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引用次数: 0
Three-dimensional bioprinted materials in alginate-hyaluronic acid complex based hydrogel based bio-ink as absorbents for heavy metal ions removal 海藻酸-透明质酸复合水凝胶生物墨水中的三维生物打印材料作为重金属离子去除吸收剂
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-15 DOI: 10.1016/j.carpta.2024.100588
A.E. Swathe Sriee , Vijayalakshmi Shankar
Major environmental and health effects arise from the presence of heavy metals in water, including lead (Pb²⁺), mercury (Hg²⁺), chromium (Cr⁶⁺), cadmium (Cd²⁺), and arsenic (As³⁺), which contribute significantly to water pollution and pose severe risks to ecosystems and human health. This study demonstrates the fabrication of 3D printed self-regenerative functional living materials, a fungi, by using mixture of sodium alginate and hyaluronic acid hydrogel as absorbents to remove the heavy metals from the environment. Bioprinting has emerged as a transformative technology for fabricating complex biological constructs. The bioprinting experiments, conducted with optimized parameters, revealed the viscoelastic behavior of the hydrogel, suitable for 3D bioprinting applications. MicroCT analysis indicated that the hydrogel's porosity and structural properties support fungal growth in a controlled three-dimensional setting. Microscopic analyses, including phase contrast microscopy, FESEM, and HRTEM, provided insights into the cellular morphology of the bioprinted constructs. Cell viability was assessed using flow cytometry with FDA and PI staining, showing a significant population of live cells, affirming the biocompatibility of the hydrogel. Additionally, the study explored the hydrogel's potential for heavy metal removal from water samples. Multi-element standard solutions containing Copper (Cu²⁺), Cadmium (Cd²⁺), Nickel (Ni²⁺), Cobalt (Co²⁺), and Ferrous (Fe³⁺) ions at different concentrations were incubated with hydrogel patches embedded with Aspergillus flavus. Atomic absorption spectrophotometry analysis showed rapid initial removal rates of metal ions, with maximum removal efficiency achieved around the 12th hour. Comparisons with a control hydrogel without the fungal strain demonstrated significantly enhanced removal efficiency due to the presence of Aspergillus flavus. This study highlights the dual functionality of sodium alginate with hyaluronic acid -based hydrogels for bioprinting fungi and for environmental remediation of heavy metals, offering promising applications in environmental cleanup.
水中重金属(包括铅(Pb²⁺)、汞(Hg²⁺)、铬(Cr⁶⁺)、镉(Cd²⁺)和砷(As³⁺))对环境和健康产生重大影响,严重加剧了水污染,对生态系统和人类健康构成严重威胁。本研究展示了利用海藻酸钠和透明质酸水凝胶的混合物作为吸附剂,制造三维打印的自再生功能性活体材料--真菌,以去除环境中的重金属。生物打印已成为制造复杂生物构造物的变革性技术。采用优化参数进行的生物打印实验揭示了水凝胶的粘弹性行为,适合三维生物打印应用。显微 CT 分析表明,水凝胶的孔隙率和结构特性支持真菌在受控三维环境中生长。相衬显微镜、FESEM 和 HRTEM 等显微分析有助于深入了解生物打印构建体的细胞形态。使用 FDA 和 PI 染色流式细胞仪对细胞存活率进行了评估,结果显示有大量的活细胞,这肯定了水凝胶的生物相容性。此外,研究还探讨了水凝胶去除水样中重金属的潜力。将含有不同浓度的铜(Cu²⁺)、镉(Cd²⁺)、镍(Ni²⁺)、钴(Co²⁺)和亚铁(Fe³⁺)离子的多元素标准溶液与嵌入黄曲霉的水凝胶贴片一起培养。原子吸收分光光度法分析表明,金属离子的初始去除率很快,在第 12 小时左右达到最高去除效率。与不含真菌菌株的对照水凝胶相比,由于黄曲霉的存在,去除效率明显提高。这项研究强调了海藻酸钠与透明质酸水凝胶的双重功能,既可用于真菌的生物打印,也可用于重金属的环境修复,在环境净化方面具有广阔的应用前景。
{"title":"Three-dimensional bioprinted materials in alginate-hyaluronic acid complex based hydrogel based bio-ink as absorbents for heavy metal ions removal","authors":"A.E. Swathe Sriee ,&nbsp;Vijayalakshmi Shankar","doi":"10.1016/j.carpta.2024.100588","DOIUrl":"10.1016/j.carpta.2024.100588","url":null,"abstract":"<div><div>Major environmental and health effects arise from the presence of heavy metals in water, including lead (Pb²⁺), mercury (Hg²⁺), chromium (Cr⁶⁺), cadmium (Cd²⁺), and arsenic (As³⁺), which contribute significantly to water pollution and pose severe risks to ecosystems and human health. This study demonstrates the fabrication of 3D printed self-regenerative functional living materials, a fungi, by using mixture of sodium alginate and hyaluronic acid hydrogel as absorbents to remove the heavy metals from the environment. Bioprinting has emerged as a transformative technology for fabricating complex biological constructs. The bioprinting experiments, conducted with optimized parameters, revealed the viscoelastic behavior of the hydrogel, suitable for 3D bioprinting applications. MicroCT analysis indicated that the hydrogel's porosity and structural properties support fungal growth in a controlled three-dimensional setting. Microscopic analyses, including phase contrast microscopy, FESEM, and HRTEM, provided insights into the cellular morphology of the bioprinted constructs. Cell viability was assessed using flow cytometry with FDA and PI staining, showing a significant population of live cells, affirming the biocompatibility of the hydrogel. Additionally, the study explored the hydrogel's potential for heavy metal removal from water samples. Multi-element standard solutions containing Copper (Cu²⁺), Cadmium (Cd²⁺), Nickel (Ni²⁺), Cobalt (Co²⁺), and Ferrous (Fe³⁺) ions at different concentrations were incubated with hydrogel patches embedded with <em>Aspergillus flavus</em>. Atomic absorption spectrophotometry analysis showed rapid initial removal rates of metal ions, with maximum removal efficiency achieved around the 12th hour. Comparisons with a control hydrogel without the fungal strain demonstrated significantly enhanced removal efficiency due to the presence of <em>Aspergillus flavus</em>. This study highlights the dual functionality of sodium alginate with hyaluronic acid -based hydrogels for bioprinting fungi and for environmental remediation of heavy metals, offering promising applications in environmental cleanup.</div></div>","PeriodicalId":100213,"journal":{"name":"Carbohydrate Polymer Technologies and Applications","volume":"8 ","pages":"Article 100588"},"PeriodicalIF":6.2,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142538687","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polyethylenimine functionalized graphene oxide and cellulose nanofibril composite hydrogels: Synthesis, characterization and water pollutants adsorption 聚乙烯亚胺功能化氧化石墨烯和纤维素纳米纤维复合水凝胶:合成、表征和水污染物吸附
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-11 DOI: 10.1016/j.carpta.2024.100585
Yufei Nan , Diego Gomez-Maldonado , Kailong Zhang , Haishun Du , Daniel C. Whitehead , Mi Li , Xinyu Zhang , Maria Soledad Peresin
A stable 2,2,6,6-tetramethylpiperidine-1-yl)oxyl (TEMPO)-oxidized cellulose nanofibril (TCNF)/graphene oxide (GO)/polyethylenimine (PEI) composite hydrogel was synthesized by self-assembly instead of chemical crosslinking. Their chemical, morphology, surface, and mechanical properties were characterized and adsorption behavior for methyl blue (–) was systematically investigated in terms of the optimal GO content, pH effect, kinetics, and isotherm models. Additionally, to assess the adsorption capability of the TCNF/GO/PEI hydrogel for various contaminants, its effectiveness was also tested for methylene blue (+), Cu (II), and soybean oils. The maximum adsorption capability for the methyl blue (−) dyes increased from 3125 to 3962 mg/g when 13.3 % of GO was added. The adsorption capability for Cu (II) and soybean oils rose from 205.3 to 218.5 and 2.1 to 7.2 mg/g, respectively. The adsorption capability of optimized TCNF/GO/PEI hydrogel for a variety of contaminants was improved overall based on the increase of surface area, electrostatic interactions, and hydrophobic domains. Moreover, adding GO did not impact the adsorption mechanism but increased the external diffusion rate in the intraparticle diffusion model. This work provides a self-assembling route to TCNF/GO/PEI hydrogels with great potential for the removal of multiple water pollutants.
通过自组装而非化学交联合成了一种稳定的 2,2,6,6-四甲基哌啶-1-基)氧化(TEMPO)-氧化纤维素纳米纤维(TCNF)/氧化石墨烯(GO)/聚乙烯亚胺(PEI)复合水凝胶。对它们的化学、形态、表面和机械性能进行了表征,并从最佳 GO 含量、pH 值效应、动力学和等温线模型等方面对甲基蓝(-)的吸附行为进行了系统研究。此外,为了评估 TCNF/GO/PEI 水凝胶对各种污染物的吸附能力,还测试了它对亚甲蓝(+)、铜(II)和大豆油的吸附效果。当添加 13.3 % 的 GO 时,甲基蓝(-)染料的最大吸附能力从 3125 mg/g 增加到 3962 mg/g。铜(II)和大豆油的吸附能力分别从 205.3 毫克/克上升到 218.5 毫克/克和 2.1 毫克/克上升到 7.2 毫克/克。基于表面积、静电相互作用和疏水域的增加,优化的 TCNF/GO/PEI 水凝胶对多种污染物的吸附能力得到了全面提高。此外,添加 GO 不会影响吸附机制,但会增加粒子内扩散模型中的外部扩散速率。这项研究为 TCNF/GO/PEI 水凝胶的自组装提供了一条途径,具有去除多种水污染物的巨大潜力。
{"title":"Polyethylenimine functionalized graphene oxide and cellulose nanofibril composite hydrogels: Synthesis, characterization and water pollutants adsorption","authors":"Yufei Nan ,&nbsp;Diego Gomez-Maldonado ,&nbsp;Kailong Zhang ,&nbsp;Haishun Du ,&nbsp;Daniel C. Whitehead ,&nbsp;Mi Li ,&nbsp;Xinyu Zhang ,&nbsp;Maria Soledad Peresin","doi":"10.1016/j.carpta.2024.100585","DOIUrl":"10.1016/j.carpta.2024.100585","url":null,"abstract":"<div><div>A stable 2,2,6,6-tetramethylpiperidine-1-yl)oxyl (TEMPO)-oxidized cellulose nanofibril (TCNF)/graphene oxide (GO)/polyethylenimine (PEI) composite hydrogel was synthesized by self-assembly instead of chemical crosslinking. Their chemical, morphology, surface, and mechanical properties were characterized and adsorption behavior for methyl blue (–) was systematically investigated in terms of the optimal GO content, pH effect, kinetics, and isotherm models. Additionally, to assess the adsorption capability of the TCNF/GO/PEI hydrogel for various contaminants, its effectiveness was also tested for methylene blue (+), Cu (II), and soybean oils. The maximum adsorption capability for the methyl blue (−) dyes increased from 3125 to 3962 mg/g when 13.3 % of GO was added. The adsorption capability for Cu (II) and soybean oils rose from 205.3 to 218.5 and 2.1 to 7.2 mg/g, respectively. The adsorption capability of optimized TCNF/GO/PEI hydrogel for a variety of contaminants was improved overall based on the increase of surface area, electrostatic interactions, and hydrophobic domains. Moreover, adding GO did not impact the adsorption mechanism but increased the external diffusion rate in the intraparticle diffusion model. This work provides a self-assembling route to TCNF/GO/PEI hydrogels with great potential for the removal of multiple water pollutants.</div></div>","PeriodicalId":100213,"journal":{"name":"Carbohydrate Polymer Technologies and Applications","volume":"8 ","pages":"Article 100585"},"PeriodicalIF":6.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142418595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Creation of 3D chitin/chitosan composite scaffold from naturally pre-structured verongiid sponge skeleton 利用天然预结构疣状海绵骨架创建甲壳素/壳聚糖三维复合支架
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-10 DOI: 10.1016/j.carpta.2024.100587
Izabela Dziedzic , Kamil Dydek , Jakub Trzciński , Anna Boczkowska , Alona Voronkina , Teofil Jesionowski , Hermann Ehrlich
This study represents the first creation and characterization of a 3D chitin/chitosan composite scaffold derived from the naturally pre-structured skeleton of the cultivated marine demosponge Aplysina aerophoba, aiming to preserve the intricate architecture of the unique tube-like chitin while incorporating chitosan layers. Advanced staining methods, including the use of iodine and Cibacron Brilliant Red (CBR), were employed to distinguish these polysaccharides. ATR-FTIR spectroscopy confirmed the system's structural integrity and identified the optimal chitin/chitosan balance, achieved after 60-minute treatment in 38 % NaOH at 95 °C. Fluorescent microscopy using fluorescein isothiocyanate (FITC) effectively confirmed the presence of chitosan layers in the created chitin/chitosan scaffolds. Scanning electron microscopy analysis further elucidated significant morphological distinctions, where chitin fibers displayed a smooth, uniform surface, contrasting with the ragged and irregular texture of chitosan-containing fibers, indicating significant surface modifications. Zeta potential measurements confirmed the partial transformation of chitin into chitosan. The dual-layer configuration, consisting of a resilient chitin core and a versatile chitosan exterior, not only provides structural support, but also enhances the scaffold's functionality for potential technological and biomedical applications. The preferential metallization of the chitosan phase by copper nanoparticles in the created 3D chitin/chitosan composite opens the way to the potential use of such scaffolds in catalysis.
本研究首次创建并表征了一种三维甲壳素/壳聚糖复合支架,该支架来自于养殖的海洋底层海绵 Aplysina aerophoba 的天然预结构骨架,旨在保留独特的管状甲壳素的复杂结构,同时结合壳聚糖层。为了区分这些多糖,我们采用了先进的染色方法,包括使用碘和 Cibacron 亮红(CBR)。ATR-FTIR 光谱证实了该系统的结构完整性,并确定了在 95 °C 下用 38 % NaOH 处理 60 分钟后达到的甲壳素/壳聚糖最佳平衡。使用异硫氰酸荧光素(FITC)进行的荧光显微镜检查有效地证实了壳聚糖层存在于所创建的甲壳素/壳聚糖支架中。扫描电子显微镜分析进一步阐明了形态上的显著区别,甲壳素纤维表面光滑、均匀,与含壳聚糖纤维的粗糙、不规则纹理形成鲜明对比,表明表面发生了显著的改性。Zeta 电位测量证实甲壳素部分转化为壳聚糖。由弹性甲壳素内核和多功能壳聚糖外层组成的双层结构不仅提供了结构支撑,还增强了支架的功能,具有潜在的技术和生物医学应用价值。在所创建的三维甲壳素/壳聚糖复合材料中,铜纳米粒子对壳聚糖相的优先金属化为此类支架在催化领域的潜在应用开辟了道路。
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引用次数: 0
An injectable supramolecular antimicrobial hydrogel based on hyaluronic acid with dynamic borate bond and hydrogen bond crosslinking for sinusitis treatment 一种基于透明质酸的动态硼酸键和氢键交联的可注射超分子抗菌水凝胶,用于治疗鼻窦炎
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-10 DOI: 10.1016/j.carpta.2024.100584
Qianqian Zhao , Datao Hu , Ting Wang , Hanchao Zhou , Jinli Gao , Ke Wang , Daqing Zhao , Leping Liang
In this study, chlorogenic acid-modified hyaluronic acid (HA-CGA) and phenylboric acid-modified ciprofloxacin (Cip-BPA) were synthesized and their structures were analyzed by 1HNMR and 13CNMR. Following, a dynamic borate and hydrogen bond crosslinked HCCB hydrogel was prepared by mixing HA-CGA and Cip-BPA solution. Its properties and gel formation mechanism were studied by means of ratio optimization, scanning electron microscopy, rheology, 11B-NMR and temperature-changing infrared spectroscopy. The basic properties and bioactivity of HCCB hydrogel were investigated by in vitro antibacterial experiment, in vitro anti-inflammatory oxidation experiment and biocompatibility test. We found that borate ester bond and hydrogen bond are important driving forces for the formation of HCCB hydrogels, and when the molar ratio of chlorogenic acid in HA-CGA and phenylboronic acid in Cip-BPA is 2:1, the properties of HCCB hydrogels formed are the best. It has excellent antibacterial properties, anti-inflammatory and antioxidant properties, good biocompatibility and pH/ROS response. The successful preparation of the gel and its excellent properties indicate that it has great potential in the treatment of some inflammation treatment.
本研究合成了绿原酸改性透明质酸(HA-CGA)和苯硼酸改性环丙沙星(Cip-BPA),并通过 1HNMR 和 13CNMR 分析了它们的结构。随后,通过混合 HA-CGA 和 Cip-BPA 溶液制备了动态硼酸盐和氢键交联的 HCCB 水凝胶。通过优化配比、扫描电子显微镜、流变学、11B-NMR 和变温红外光谱等方法研究了其性质和凝胶形成机理。通过体外抗菌实验、体外抗炎氧化实验和生物相容性测试,研究了 HCCB 水凝胶的基本性质和生物活性。我们发现,硼酸酯键和氢键是 HCCB 水凝胶形成的重要驱动力,当 HA-CGA 中的绿原酸和 Cip-BPA 中的苯硼酸的摩尔比为 2:1 时,形成的 HCCB 水凝胶性能最好。它具有优异的抗菌性、抗炎性和抗氧化性,良好的生物相容性和 pH/ROS 反应。该凝胶的成功制备及其优良特性表明,它在治疗某些炎症方面具有很大的潜力。
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引用次数: 0
Disulfide stoppered polyrotaxanes with enhanced cellular uptake and intracellular cyclodextrin release 具有增强细胞摄取能力和细胞内环糊精释放能力的二硫键封端聚罗他赛
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-10 DOI: 10.1016/j.carpta.2024.100586
Gergely Kali , Alexander H. Mayer , Dennis To , Martyna Truszkowska , Raphael Plangger , Markus Gallei , Andreas Bernkop-Schnürch

Background and Aim

Polyrotaxanes are molecular necklaces composed of polymers, threaded macrocycles, and bulky stopper molecules to inhibit the decomposition of the first two. These supramolecular assemblies are promising active ingredients for treating lysosomal storage disorders. This study aimed to synthesize such polyrotaxanes with a novel, simple method, resulting in high threading efficacy, enhanced cellular uptake, and intracellular cyclodextrin (CD) release.

Methods

In this study, we developed two novel poly(ethylene glycol) (PEG) based polyrotaxanes, with threaded α-cyclodextrin (α-CD) or its mixture with 2-hydroxypropyl-α-CD (HP-α-CD) and glutathione sensitive disulfide connected stopper molecules. The structure and composition of these polyrotaxanes were determined by 1H NMR spectroscopy and gel permeation chromatography, while the cellular uptake was investigated by flow cytometry and confocal microscopy.

Results

High threading efficacy, as well as molar mass of 17.9 and 13.1 kDa, was found for the polymeric supramolecules with threaded α-CD and α-CD/HP-α-CD, respectively. Glutathion-triggered reductive removal of the stopper molecules showed potential decomposition of these polyrotaxanes in target cells. Flow cytometry revealed an up to 52-fold enhancement in cellular uptake of α- and HP-α-CD by the polyrotaxanes compared to free CD, which was also visualized by confocal microscopy.

Conclusion and scope of application

Polyrotaxanes based on α-CD and its derivative were tested in vitro for application in the treatment of lysosomal storage disease for the first time. Based on these results, polyrotaxanes with disulfide stopper molecules might be promising supramolecular excipients for cellular delivery of α-CDs.
背景和目的聚对苯二甲酸是一种分子项链,由聚合物、螺纹大环和大块阻遏分子组成,可抑制前两者的分解。这些超分子组合物是治疗溶酶体贮积症的有效成分。本研究旨在用一种新颖、简单的方法合成这种聚二十二烷,从而获得高穿线效能、增强细胞摄取和细胞内环糊精(CD)释放。方法在本研究中,我们开发了两种新型聚乙二醇(PEG)基聚二十二烷,其中含有穿线α-环糊精(α-CD)或其与 2-羟丙基-α-CD(HP-α-CD)的混合物以及谷胱甘肽敏感的二硫连接阻遏分子。结果发现,带螺纹的 α-CD 和 α-CD/HP-α-CD 聚合超分子的穿线效率高,摩尔质量分别为 17.9 和 13.1 kDa。谷胱甘肽触发的还原去除阻遏分子的过程表明,这些聚合高聚物可能会在靶细胞中分解。流式细胞仪显示,与游离 CD 相比,聚糖对 α-CD 和 HP-α-CD 的细胞摄取量最多可提高 52 倍,共聚焦显微镜也可观察到这一点。基于这些结果,带有二硫塞分子的聚二十二烷可能会成为α-CDs细胞递送的有前途的超分子赋形剂。
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引用次数: 0
Development of cellulose-supported Pd-nanocatalyst for the heck coupling and michael addition reactions 开发用于赫克偶联和迈克尔加成反应的纤维素支撑钯纳米催化剂
IF 6.2 Q1 CHEMISTRY, APPLIED Pub Date : 2024-10-09 DOI: 10.1016/j.carpta.2024.100578
Shaheen M. Sarkar , Md Lutfor Rahman , Kamrul Hasan , Md. Maksudur Rahman Khan , Emmet J. O'Reilly , Mohd Hasbi Ab. Rahim
The development of reusable, bio-resource based nanocatalysts with high turnover numbers (TONs) is essential for increased sustainability in the chemical sector. Herein, cellulose-supported bio-resourced poly(hydroxamic acid) is employed as a ligand in the synthesis of a palladium nanocomposite (PdNc-PHA) that exhibits higher TONs that previously reported similar systems for the Mizoroki-Heck and Michael addition reactions. The PdNc-PHA catalyst was characterised using Fourier transform infrared spectroscopy (FTIR), field-emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectrometry (EDX), high-resolution transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma-atomic emission spectroscopy (ICP-AES) analyses. Results showed that the PdNc-PHA catalyst exhibits excellent durability and high catalytic activity in the Mizoroki-Heck and Michael addition reactions, leading to high yields of the desired corresponding products. The Mizoroki-Heck reaction of aryl/heteroaryl chlorides with olefins resulted in the production of cross-coupled products, while the Michael addition reaction of phenol/thiophenol and aliphatic cyclic/alicyclic amines with a variety of olefins synthesised the corresponding O-, S-, and N-alkylated products. The recycle and reusability of the catalyst were tested using 4-nitrochlorobenzene and butyl acrylate. The results demonstrated that the catalyst maintained its catalytic activity effectively for up to ten cycles without any noticeable loss in performance. This research represents a promising strategy for efficient catalysis based on bio-waste as a wealth material.
开发可重复使用的、基于生物资源的、具有高周转次数(TON)的纳米催化剂对于提高化工行业的可持续性至关重要。在此,我们采用纤维素支撑的生物资源聚(羟基氨基甲酸)作为配体,合成了一种钯纳米复合材料(PdNc-PHA),与之前报道的用于 Mizoroki-Heck 和迈克尔加成反应的类似体系相比,这种钯纳米复合材料具有更高的周转次数。傅立叶变换红外光谱(FTIR)、场发射扫描电子显微镜(FE-SEM)、能量色散 X 射线光谱(EDX)、高分辨率透射电子显微镜(HR-TEM)、X 射线光电子能谱(XPS)和电感耦合等离子体原子发射光谱(ICP-AES)分析对 PdNc-PHA 催化剂进行了表征。结果表明,PdNc-PHA 催化剂在 Mizoroki-Heck 反应和迈克尔加成反应中表现出优异的耐久性和高催化活性,并能获得高产率的所需相应产物。芳基/杂芳基氯化物与烯烃的 Mizoroki-Heck 反应生成了交叉耦合产物,而苯酚/噻吩酚和脂肪族环状/脂环族胺与各种烯烃的迈克尔加成反应则合成了相应的 O-、S- 和 N-烷基化产物。使用 4-硝基氯苯和丙烯酸丁酯测试了催化剂的回收和再利用能力。结果表明,该催化剂在长达十次的循环中都能有效地保持其催化活性,而不会出现任何明显的性能损失。这项研究代表了一种以生物废料为富集材料的高效催化战略,前景广阔。
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Carbohydrate Polymer Technologies and Applications
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