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Phage endolysin–polyphosphate/alginate nanocomplexes inhibit staphylococcal biofilms for implant protection 噬菌体内溶素-多磷酸/海藻酸盐纳米复合物抑制葡萄球菌生物膜对植入物的保护作用
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-15 DOI: 10.1016/j.carpta.2026.101089
Mariana Blanco Massani , Dennis To , David Gintsburg , Lana Molnar , Ilaria Polidori , Susanne Meile , Anna Seybold , Burak Ünalan , Débora C. Coraça-Huber , Florentine Marx , Martin J. Loessner , Mathias Schmelcher , Szczepan Zapotoczny , Andreas Bernkop-Schnürch
Implant-associated infections caused by Staphylococcus epidermidis and Staphylococcus aureus remain a major challenge in orthopedic surgery due to their robust biofilm formation and resistance to conventional antibiotics.
We aimed to develop an alginate-based delivery system for peptidoglycan hydrolase–polyphosphate (PGH-PP) nanoparticles to prevent staphylococcal biofilm formation on implant surfaces. These nanoparticles incorporated two chimeric phage-derived endolysins, GH15 and M23. Formulations were screened for antimicrobial and antibiofilm activity against staphylococcal species using low- and very low-viscosity alginate. The nanostructure of the delivery systems was analyzed via transmission electron microscopy and phosphate release assays. Biocompatibility with MC3T3 preosteoblasts and the formulation´s impact on bone development were evaluated. Efficacy in inhibiting biofilm formation by S. epidermidis 9142 and S. aureus ATCC 25923 was assessed both on orthopedic implant surrogates and in co-culture experiments with MC3T3 preosteoblasts.
Very low-viscosity alginate (0.625% w/v), in conjunction with a synergistic combination of M23-PP and GH15-PP, formed well-defined complex coacervates of approximately 350 nm (M23-PP/GH15-PP/VL alginate). The developed nanocomplexes effectively eradicated both bacterial species and further inhibited biofilm formation on implants, as confirmed by scanning electron microscopy. M23-PP/GH15-PP/VL alginate was biocompatible with MC3T3 preosteoblasts supporting its potential use in orthopedic applications. When MC3T3 cells were co-cultured with S. epidermidis or S. aureus, M23-PP/GH15-PP/VL alginate treatment led to an 8 log reduction in bacterial counts, with healthy mammalian cells proliferating in the absence of bacteria.
These results highlight the potential of M23-PP/GH15-PP/VL alginate as a biocompatible approach to preventing staphylococcal biofilm formation, mitigating the risk of implant-related bone infections.
表皮葡萄球菌和金黄色葡萄球菌引起的植入物相关感染由于其强大的生物膜形成和对常规抗生素的耐药性,仍然是骨科手术的主要挑战。我们的目标是开发一种基于海藻酸盐的肽聚糖水解酶-聚磷酸(PGH-PP)纳米颗粒递送系统,以防止葡萄球菌在植入物表面形成生物膜。这些纳米颗粒含有两种嵌合噬菌体衍生的内溶素GH15和M23。使用低粘度和极低粘度海藻酸盐对葡萄球菌进行抗菌和抗生物膜活性筛选。通过透射电子显微镜和磷酸盐释放实验分析了递送系统的纳米结构。评估其与MC3T3成骨前细胞的生物相容性以及对骨发育的影响。在骨科假体和MC3T3成骨前细胞共培养实验中,研究了表皮葡萄球菌9142和金黄色葡萄球菌ATCC 25923抑制生物膜形成的效果。非常低粘度的海藻酸盐(0.625% w/v),与M23-PP和GH15-PP的协同组合一起,形成了约350 nm的清晰的复杂凝聚体(M23-PP/GH15-PP/VL海藻酸盐)。扫描电镜证实,所开发的纳米复合物有效地根除了这两种细菌,并进一步抑制了植入物上生物膜的形成。M23-PP/GH15-PP/VL海藻酸盐与MC3T3成骨前细胞具有生物相容性,支持其在骨科应用中的潜在应用。当MC3T3细胞与表皮葡萄球菌或金黄色葡萄球菌共培养时,M23-PP/GH15-PP/VL海藻酸盐处理导致细菌计数减少8倍,健康哺乳动物细胞在没有细菌的情况下增殖。这些结果强调了M23-PP/GH15-PP/VL海藻酸盐作为一种生物相容性方法的潜力,可以预防葡萄球菌生物膜的形成,降低种植体相关骨感染的风险。
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引用次数: 0
Controllable polysaccharide depolymerization by heparinases for efficient low molecular weight heparin production 可控多糖解聚肝素酶高效低分子量肝素生产
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-09 DOI: 10.1016/j.carpta.2026.101087
Fengling Yang , Ruirui Xu , Hao Huang , Jie Lu , Jiamin Feng , Xiaoyuan Sun , Jianghua Li , Guocheng Du , Zhen Kang
Low molecular weight heparins (LMWHs) are widely used in clinical anticoagulant therapy. Although most commercial LMWHs are still produced through chemical depolymerization, enzymatic depolymerization using heparinases has emerged as a highly attractive alternative due to its environmental friendliness, high selectivity, and superior preservation of native heparin bioactivity. Heparinases selectively cleave specific glycosidic bonds in unfractionated heparin (UFH), enabling precise and controllable depolymerization of polysaccharide chains and thereby generating LMWHs with well-defined structures and favorable anticoagulant properties, typically reflected by anti-Xa/anti-IIa activity ratios. Distinct classes of heparinases differ in substrate specificity and catalytic mechanisms, allowing targeted cleavage guided by sulfation patterns and structural features. This review summarizes the substrate preferences, crystal structures, and catalytic mechanisms of heparinases, highlighting their mechanistic basis for controlled polysaccharide depolymerization. Recent advances in protein engineering and LMWHs production strategies are discussed, along with emerging trends and future directions aimed at enhancing catalytic performance and enabling more tailored, efficient, and sustainable LMWHs manufacturing.
低分子量肝素在临床抗凝治疗中有着广泛的应用。尽管大多数商业化的低分子肝素仍是通过化学解聚来生产的,但由于肝素酶的环境友好性、高选择性和天然肝素生物活性的良好保存,酶解聚已成为一种极具吸引力的替代方法。肝素酶选择性地切割未分离肝素(UFH)中特定的糖苷键,实现多糖链的精确和可控解聚,从而产生具有明确结构和良好抗凝性能的lmwh,通常反映在抗xa /抗iia活性比上。不同种类的肝素酶在底物特异性和催化机制上有所不同,允许在硫酸模式和结构特征的指导下进行靶向切割。本文综述了肝素酶的底物偏好、晶体结构和催化机制,重点介绍了其控制多糖解聚的机制基础。本文讨论了蛋白质工程和低分子硫化物生产策略的最新进展,以及旨在提高催化性能和实现更定制、高效和可持续的低分子硫化物制造的新兴趋势和未来方向。
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引用次数: 0
Tunable core water–shell alginate microparticles produced by microfluidics for sustained doxorubicin encapsulation and release 微流体制备的可调核心水壳藻酸盐微颗粒用于阿霉素的持续包封和释放
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-08 DOI: 10.1016/j.carpta.2026.101086
Fatemeh Zarei , Amir Shamloo
Core–shell particles have emerged as a promising platform for drug delivery due to their ability to spatially separate the drug-loaded core from the protective shell, enabling enhanced encapsulation efficiency, protection of sensitive therapeutics, and precise control over release kinetics. This study aimed to develop and optimize a droplet-based microfluidic approach for synthesizing water core–alginate shell particles. To mitigate the limitation of hydrophilic drug retention, these microparticles were designed to encapsulate the anticancer drug doxorubicin, enabling sustained release and reducing adverse side effects. Key parameters—including the flow rate of various phases, the junction width of the flow-focusing device, and the composition of alginate shell solution— were evaluated to achieve stable core–shell microgels with the desired morphology. By adjusting these parameters, monodisperse core-shell droplets (350 µm diameter, 43 µm shell thickness) were successfully tuned to slow drug release and increase resistance to immediate drug diffusion. To prolong the release duration, carboxymethyl cellulose particles and ε-poly-l-lysine were added to the core phase to form interpenetrating networks and electrostatic complexes at the water/alginate interface. This structural modification significantly enhanced drug encapsulation from approximately 67% to over 92%, while simultaneously prolonging the release duration beyond 120 hours under physiological conditions. Finally, the produced core-shell drug carriers were utilized for treating cancer cells, indicating a predictable and sustained cytotoxic effect against cancer cells. Overall, the proposed approach enables reproducible fabrication of tunable core–shell carriers with precise control over structural and functional parameters, offering promise for sustained chemotherapy delivery with reduced side effects.
核-壳颗粒已成为一种很有前途的药物递送平台,因为它们能够在空间上将载药的核与保护壳分离,从而提高包封效率,保护敏感疗法,并精确控制释放动力学。本研究旨在开发并优化基于液滴的微流体合成水核-海藻酸盐壳颗粒的方法。为了减轻亲水性药物滞留的限制,这些微颗粒被设计成包封抗癌药物阿霉素,使其能够持续释放并减少不良副作用。评估了关键参数,包括不同相的流速、流动聚焦装置的结宽和海藻酸盐壳溶液的组成,以获得具有所需形态的稳定核-壳微凝胶。通过调节这些参数,单分散的核壳液滴(直径350µm,壳厚43µm)成功地调节到减缓药物释放和增加对药物立即扩散的抵抗力。为了延长释放时间,在核心相中加入羧甲基纤维素颗粒和ε-聚赖氨酸,在水/海藻酸盐界面形成互穿网络和静电配合物。这种结构修饰显著提高了药物包封率,从约67%提高到92%以上,同时延长了生理条件下120小时以上的释放时间。最后,所制备的核壳药物载体被用于治疗癌细胞,表明对癌细胞具有可预测和持续的细胞毒性作用。总的来说,所提出的方法能够重复制造可调核壳载体,精确控制结构和功能参数,为减少副作用的持续化疗提供了希望。
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引用次数: 0
Tailoring mechanical and functional properties of 3D-printed nanocellulose-alginate scaffolds via alternative ionic crosslinkers 通过替代离子交联剂定制3d打印纳米纤维素-海藻酸盐支架的机械和功能特性
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-07 DOI: 10.1016/j.carpta.2026.101084
Ana Peharda , Florian Lackner , Tobias Steindorfer , Julia Fink , Petra Kotzbeck , Rupert Kargl , Karin Stana Kleinscheck , Tamilselvan Mohan
Renewable polysaccharides combined with advanced 3D printing enable precise, biomimetic scaffolds for tissue engineering (TE). Alginate hydrogels offer excellent biocompatibility and rapid gelation but lack mechanical strength and bioactivity. Adding nanofibrillated cellulose (NFC) improves rheological and structural properties, yet research has mostly focused on conventional calcium-based crosslinking. This study evaluates insoluble divalent metal carbonate crosslinkers (Mg²⁺, Ca²⁺, Zn²⁺, Sr²⁺) in NFC–alginate inks printed via direct-ink-writing (DIW) 3D printing. Rheological tests confirmed shear-thinning behavior dominated by the polymer matrix, facilitating extrusion printing. Improved dimensional and mechanical stability resulted from gradual metal ion release and in situ crosslinking triggered by acetic acid in an ethanol–water medium. Sr²⁺-crosslinked scaffolds achieved the highest tensile strength (3.5 MPa) and modulus (16%), outperforming Ca²⁺, Mg²⁺, and Zn²⁺. Sr²⁺ and Ca²⁺ also showed superior ion retention (>75%) and dimensional stability. SEM/EDX analysis confirmed compact matrices with uniform ion distribution. Cytocompatibility assays revealed that Sr²⁺ and Ca²⁺ scaffolds maintained high human cell viability (>80%), while Zn²⁺ was cytotoxic (<30%). These results highlight Sr²⁺ carbonate crosslinking as optimal for mechanical performance and biocompatibility, advancing NFC–alginate bioinks for regenerative and functional biomaterial applications.
可再生多糖与先进的3D打印相结合,为组织工程(TE)提供了精确的仿生支架。海藻酸盐水凝胶具有良好的生物相容性和快速凝胶性,但缺乏机械强度和生物活性。纳米纤化纤维素(NFC)的加入改善了材料的流变学和结构性能,但目前的研究主要集中在传统的钙基交联上。本研究评估了通过直接墨水书写(DIW) 3D打印的nfc -海藻酸盐油墨中不溶性二价金属碳酸盐交联剂(Mg 2 +、Ca 2 +、Zn 2 +、Sr 2 +)的性能。流变试验证实了聚合物基体主导的剪切减薄行为,有利于挤出印刷。在乙醇-水介质中,逐渐释放的金属离子和醋酸引发的原位交联提高了尺寸和机械稳定性。Sr 2 +交联支架获得了最高的抗拉强度(3.5 MPa)和模量(16%),优于Ca 2 +、Mg 2 +和Zn 2 +。Sr 2 +和Ca 2 +也表现出优异的离子保留率(>75%)和尺寸稳定性。SEM/EDX分析证实了致密的基体具有均匀的离子分布。细胞相容性实验表明,Sr 2 +和Ca 2 +支架保持较高的人体细胞活力(>80%),而Zn 2 +具有细胞毒性(<30%)。这些结果强调了Sr 2 +碳酸盐交联是机械性能和生物相容性的最佳选择,推进了nfc -海藻酸盐生物墨水在再生和功能性生物材料中的应用。
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引用次数: 0
Quantitative evaluation of release behavior of synthetic taste-masking drugs using polysaccharide-based carrier with direct analysis in real-time mass spectrometry 实时质谱法直接分析多糖基载体对合成掩味药物释放行为的定量评价
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-07 DOI: 10.1016/j.carpta.2026.101085
Zhao-Liang Hu , Ke Wang , Xiao-Hua Zhou , Xun Zhao , Mei Zhang , Yao-Zuo Yuan , Wen-Yuan Liu , Bao-Cheng Wang , Lei Chen , Sheng Tang , Hian Kee Lee , Hai-Wei Shi , Sheng-Jin Gong
Sodium alginate (ALG) is widely used as a taste-masking excipient in pediatric oral formulations, yet its release behavior is strongly governed by molecular structure. azithromycin (AZM, targeted bitterness probes)-loaded ALG microspheres using five different ALG specifications (with various molecular weights or mannuronic-to-guluronic acid (M/G) ratios) were prepared, with loading efficiencies between 17.71–19.48%. Thereafter, an on-line release-evaluation method was developed by integrating a flow-pump dissolution model with direct analysis in real time mass spectrometry (DART-MS), enabling dynamic monitoring of AZM release under simulated oral conditions. Consequently, both molecular weights and M/G ratios were verified that can significantly affect the release behavior of the microspheres. Microspheres prepared by ALG with lower M/G ratios showed consistently limited release across the 1200-s testing period, reaching approximately 3% cumulative release. In contrast, those derived from ALG with higher M/G ratios displayed faster initial release during 0–300 s and achieved approximately 12% cumulative release at 1200 s. Molecular weight further modulated late-stage release, with lower-molecular-weight ALG samples exhibiting more significant increases in total AZM release. This approach offers a quantitative and mechanism-supported framework for optimizing polysaccharide-based taste-masking systems and achieving controlled drug release in pediatric formulations.
海藻酸钠(ALG)作为一种掩味赋形剂广泛应用于儿科口服配方中,但其释放行为受其分子结构的强烈影响。制备了5种不同ALG规格(不同分子量或甘露醛酸与古鲁醛酸(M/G)比)的阿奇霉素(AZM,靶向苦味探针)负载ALG微球,其负载效率在17.71 ~ 19.48%之间。随后,将流动泵溶出模型与实时质谱直接分析(DART-MS)相结合,建立了一种在线释放评价方法,实现了模拟口腔条件下AZM释放的动态监测。结果表明,分子量和M/G比对微球的释放行为有显著影响。较低M/G比的ALG制备的微球在1200-s的测试周期内释放持续有限,累积释放量约为3%。相比之下,高M/G比的ALG在0-300秒内表现出更快的初始释放,在1200秒时达到约12%的累积释放。分子量进一步调节了后期释放,低分子量ALG样品的AZM总释放量增加更显著。这种方法提供了一个定量和机制支持的框架,优化以多糖为基础的味觉掩蔽系统,并在儿科配方中实现药物释放控制。
{"title":"Quantitative evaluation of release behavior of synthetic taste-masking drugs using polysaccharide-based carrier with direct analysis in real-time mass spectrometry","authors":"Zhao-Liang Hu ,&nbsp;Ke Wang ,&nbsp;Xiao-Hua Zhou ,&nbsp;Xun Zhao ,&nbsp;Mei Zhang ,&nbsp;Yao-Zuo Yuan ,&nbsp;Wen-Yuan Liu ,&nbsp;Bao-Cheng Wang ,&nbsp;Lei Chen ,&nbsp;Sheng Tang ,&nbsp;Hian Kee Lee ,&nbsp;Hai-Wei Shi ,&nbsp;Sheng-Jin Gong","doi":"10.1016/j.carpta.2026.101085","DOIUrl":"10.1016/j.carpta.2026.101085","url":null,"abstract":"<div><div>Sodium alginate (ALG) is widely used as a taste-masking excipient in pediatric oral formulations, yet its release behavior is strongly governed by molecular structure. azithromycin (AZM, targeted bitterness probes)-loaded ALG microspheres using five different ALG specifications (with various molecular weights or mannuronic-to-guluronic acid (M/G) ratios) were prepared, with loading efficiencies between 17.71–19.48%. Thereafter, an on-line release-evaluation method was developed by integrating a flow-pump dissolution model with direct analysis in real time mass spectrometry (DART-MS), enabling dynamic monitoring of AZM release under simulated oral conditions. Consequently, both molecular weights and M/G ratios were verified that can significantly affect the release behavior of the microspheres. Microspheres prepared by ALG with lower M/G ratios showed consistently limited release across the 1200-s testing period, reaching approximately 3% cumulative release. In contrast, those derived from ALG with higher M/G ratios displayed faster initial release during 0–300 s and achieved approximately 12% cumulative release at 1200 s. Molecular weight further modulated late-stage release, with lower-molecular-weight ALG samples exhibiting more significant increases in total AZM release. This approach offers a quantitative and mechanism-supported framework for optimizing polysaccharide-based taste-masking systems and achieving controlled drug release in pediatric formulations.</div></div>","PeriodicalId":100213,"journal":{"name":"Carbohydrate Polymer Technologies and Applications","volume":"13 ","pages":"Article 101085"},"PeriodicalIF":6.5,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145977595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Development of UV-resistant carboxymethyl cellulose/ZnONPs based nanocomposite films derived from Zea mays husk and reinforced with Ananas comosus peel extract for active food packaging 玉米皮增强抗紫外羧甲基纤维素/ZnONPs纳米复合膜的研制
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-05 DOI: 10.1016/j.carpta.2026.101083
Md Abu Rayhan, Md. Murad Hossain, Tamanna Rahman, Md. Suhel Mia, Wahidu Zzaman
The increasing environmental burden of petroleum-based packaging underscores the need for biodegradable materials with enhanced functional performance. This study reports the development of composite films from carboxymethyl cellulose (CMC) derived from Zea mays husk, reinforced with zinc oxide nanoparticles (ZnONPs) and Ananas comosus peel extract (APE). Films were fabricated using a fixed ZnONPs concentration (5 wt % relative to CMC) and varying APE contents (5–15 % wt % relative to CMC), and their physicochemical, structural, and functional properties were systematically evaluated. The findings indicated that the CMC-ZnO-APE 10 % film exhibited optimal performance, with tensile strength increasing to 26.05 MPa, and water vapor permeability decreased by 32 %, along with lower moisture sensitivity, enhanced thermal stability with degradation onset above 200 °C, and near-complete UV shielding. Antioxidant activity (DPPH radical scavenging) increased to 45.99 %, while effective antimicrobial inhibition against Staphylococcus aureus and Escherichia coli was observed. Additionally, high biodegradability of the polymeric matrix was achieved, with over 96 % weight loss after three weeks of soil burial. Structural analyses confirmed uniform nanoparticle dispersion within the CMC matrix. These findings advance the novelty of valorizing Zea mays husk and Ananas comosus peel into high-performance, biodegradable films with strong potential for sustainable food packaging applications.
石油基包装日益增加的环境负担强调了对具有增强功能性能的生物可降解材料的需求。本文报道了以玉米壳为原料制备羧甲基纤维素(CMC)、氧化锌纳米粒子(ZnONPs)和蚕豆皮提取物(APE)增强复合膜的研究进展。采用固定的ZnONPs浓度(相对于CMC的重量为5 wt %)和不同的APE含量(相对于CMC的重量为5 wt %)制备薄膜,并对其物理化学、结构和功能特性进行系统评价。研究结果表明,CMC-ZnO-APE 10%的薄膜性能最佳,抗拉强度提高到26.05 MPa,水蒸气渗透性降低32%,同时具有较低的水分敏感性,增强的热稳定性,在200°C以上开始降解,并且几乎完全屏蔽紫外线。抗氧化活性(DPPH自由基清除率)提高至45.99%,对金黄色葡萄球菌和大肠杆菌有较好的抑菌作用。此外,聚合物基质具有很高的生物降解性,在土壤掩埋三周后,重量减轻了96%以上。结构分析证实纳米颗粒在CMC基体内均匀分散。这些发现促进了玉米壳和蚕豆皮的创新,使其成为高性能、可生物降解的薄膜,具有可持续食品包装应用的强大潜力。
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引用次数: 0
Antibiofilm activity of lactose and κ-carrabiose chitosan derivates 乳糖和κ- carcarose壳聚糖衍生物的抗膜活性
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2026-01-01 DOI: 10.1016/j.carpta.2025.101082
Romina Cingolani , Fernanda Buzzola , Diego A. Navarro
The use of natural polysaccharides, particularly chitosan and its derivatives, as agents to prevent biofilm formation and attenuate virulence properties of pathogenic bacteria has received increasing attention in recent years. In this study chitosan and some selected derivatives were tested for their antibacterial activity, with a N-alkylated lactose chitosan derivative and a N-alkylated κ-carrabiose chitosan derivative showing promising results as inhibitors of in vitro biofilm formation in the bacterial strain Staphylococcus aureus ATCC25923. In combination with the antibiotic ciprofloxacin, the selected lactose derivative showed a reduction in biofilm formation compared to the use of the antibiotic alone and was effective in alleviating the enhancement of biofilm formation that arrives as an unwanted effect of the antibiotic use. The novel κ-carrabiose-chitosan derivatives were synthesized using response surface methodology (RSM) and products with different degrees of substitution were obtained in a controlled manner. The reaction conditions were selected based on the prior optimization by RSM of the influential variables (reagent concentrations, volume, time and temperature) in the synthesis of lactose-chitosan derivatives. The reductive amination reaction using 2-picoline borane as a reducing agent was selected to achieve the synthesis of the chitosan derivatives, making the reaction and work-up greener and safer.
近年来,利用天然多糖,特别是壳聚糖及其衍生物,作为防止致病菌形成生物膜和减弱致病菌毒力的药剂受到越来越多的关注。本研究对壳聚糖及其衍生物的抑菌活性进行了测试,其中n -烷基化乳糖壳聚糖衍生物和n -烷基化κ-卡拉糖壳聚糖衍生物对金黄色葡萄球菌ATCC25923的体外生物膜形成具有抑制作用。与抗生素环丙沙星联合使用时,与单独使用抗生素相比,所选择的乳糖衍生物显示出生物膜形成的减少,并且有效地减轻了生物膜形成的增强,而生物膜形成是抗生素使用的不良影响。利用响应面法(RSM)合成了新型κ- carcar糖-壳聚糖衍生物,并在可控的条件下得到了不同取代度的产物。对影响乳糖-壳聚糖衍生物合成的影响因素(试剂浓度、体积、时间和温度)进行了RSM优化,确定了反应条件。选择以2-吡啶硼烷为还原剂的还原性胺化反应来合成壳聚糖衍生物,使反应和加工更环保、更安全。
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引用次数: 0
Self-crosslinked fucoidan nanoparticles via electron beam irradiation: Synthesis, physicochemical analysis, and drug delivery application 电子束辐照下的自交联岩藻聚糖纳米颗粒:合成、理化分析和给药应用
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2025-12-31 DOI: 10.1016/j.carpta.2025.101081
Kyung Won Kim , Heeyeol Lee , Seung Tae Jung , Wan Ook Kim , Seongwhan Cho , Phuong Tu Huynh , Muhammad Zeeshan , Yuri Kim , Dong-Mok Lee , Jinku Kim , Kwang Soo Cho , Jeongsoo Yoo
Naturally derived polysaccharides have great potential in biomedical applications due to their biocompatibility, biodegradability, and non-toxicity. In this study, we successfully synthesized nanoparticles of fucoidan, a sulfated polysaccharide derived from brown algae, via electron beam irradiation. This method enabled simple and efficient synthesis in aqueous solution without the need for chemical cross-linkers or toxic reagents. By adjusting the electron beam irradiation intensity and fucoidan concentration, the nanoparticle size could be tuned from 100 to 215 nm. Structural analysis (FT-IR, 1H-NMR, XRD) confirmed that irradiation led to increased crystallinity and cross-linking. Additionally, rheological analysis suggested a mechanism by which electron beam irradiation induced simultaneous chain scission and cross-linking. Doxorubicin loading into the nanoparticles resulted in pH-sensitive drug release properties, demonstrating stability at physiological pH and accelerated release under acidic conditions. In cell and animal assays, the doxorubicin-loaded nanoparticles exhibited high cytotoxicity against EMT6 breast cancer cells and reduced tumor volume by more than four-fold in vivo. This study presents a green and scalable method for preparing fucoidan nanoparticles using electron beam irradiation; it demonstrates their potential applications in cancer therapy and drug delivery systems.
天然来源的多糖具有生物相容性、可生物降解性和无毒性等特点,在生物医学领域具有很大的应用潜力。在这项研究中,我们成功地通过电子束辐照合成了褐藻多糖的纳米颗粒。该方法简便、高效,无需化学交联剂或有毒试剂。通过调节电子束辐照强度和褐藻糖聚糖浓度,纳米颗粒的粒径可在100 ~ 215 nm范围内调节。结构分析(FT-IR, 1H-NMR, XRD)证实辐照导致结晶度和交联增加。此外,流变学分析表明,电子束辐照可同时引起链断裂和交联。将多柔比星装载到纳米颗粒中导致pH敏感的药物释放特性,在生理pH下表现出稳定性,在酸性条件下加速释放。在细胞和动物实验中,负载阿霉素的纳米颗粒对EMT6乳腺癌细胞表现出很高的细胞毒性,并在体内将肿瘤体积缩小了四倍以上。本研究提出了一种绿色、可扩展的电子束辐照制备岩藻聚糖纳米颗粒的方法;它展示了它们在癌症治疗和药物输送系统中的潜在应用。
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引用次数: 0
Process-intensified production of TEMPO-oxidized cellulose nanofibrils: Application to several lignocellulosic feedstocks tempo氧化纤维素纳米原纤维的工艺强化生产:在几种木质纤维素原料中的应用
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2025-12-29 DOI: 10.1016/j.carpta.2025.101079
Jose Luis Sanchez-Salvador , Aleta Duque , Diego Lopez-Monte , Raquel Cañadas , Quim Tarrés , Marc Delgado-Aguilar , Angeles Blanco , Carlos Negro
Despite the remarkable properties of cellulose nanofibrils (CNFs), large-scale production remains limited by the lack of efficient, scalable oxidation and fibrillation technologies. Achieving processes that ensure product quality at industrial performance levels is essential for cost reduction and broadening CNF applications. This study addresses the scale-up of TEMPO-mediated oxidation (TMO) to produce oxidized pulps (OPs) from five lignocellulosic materials, and CNFs after mechanical fibrillation. Five oxidation configurations were tested under comparable conditions: laboratory-scale batch oxidation in a stirred reactor, a batch kneader (K100), and a continuous twin-screw extruder (TSE) in three configurations. Results showed that K100 and the single-pass TSE achieved the highest OP production efficiency, reaching 0.57 kg/h. Although additional TSE passes progressively lowered throughput, they yielded greater reductions in degree of polymerization, facilitating microfibril disintegration. Comparative analysis, including PCA, revealed that the raw material is the dominant factor driving differences among the CNFs, while variations in the TMO configuration caused only minor effects. Nonetheless, the oxidation step remains essential to achieve nanoscale fibrillation, with carboxyls in 0.7–1.0 mmol COOH/g depending on feedstock and configuration. These findings validate the technical feasibility of scaling-up the TMO process, providing viable, sustainable routes for industrial CNF manufacturing, demonstrating significant water consumption reduction.
尽管纤维素纳米原纤维(CNFs)具有显著的性能,但由于缺乏高效、可扩展的氧化和纤维化技术,大规模生产仍然受到限制。实现确保产品质量达到工业性能水平的工艺对于降低成本和扩大CNF应用至关重要。本研究解决了tempo介导氧化(TMO)的规模扩大,从五种木质纤维素材料和机械纤颤后的CNFs中生产氧化纸浆(OPs)。在类似的条件下测试了五种氧化配置:实验室规模的搅拌反应器中的间歇氧化,间歇捏合机(K100)和连续双螺杆挤出机(TSE)的三种配置。结果表明,K100和单道TSE的OP生产效率最高,达到0.57 kg/h。虽然额外的TSE通道逐渐降低了吞吐量,但它们产生了更大的聚合程度降低,促进了微纤维的分解。包括主成分分析在内的比较分析表明,原料是驱动CNFs差异的主要因素,而TMO结构的变化仅引起较小的影响。尽管如此,氧化步骤对于实现纳米级纤颤仍然是必不可少的,根据原料和配置,羧基在0.7-1.0 mmol COOH/g之间。这些发现验证了扩大TMO工艺的技术可行性,为工业CNF制造提供了可行的、可持续的路线,并证明了显著的水消耗减少。
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引用次数: 0
Bottom-up assembly of cellulose nanocrystals as a green entry to structured functional carbons 纤维素纳米晶体的自下而上组装作为结构功能碳的绿色入口
IF 6.5 Q1 CHEMISTRY, APPLIED Pub Date : 2025-12-29 DOI: 10.1016/j.carpta.2025.101080
Lucas Güemes , Víctor Calvo , Vanessa B. Maya-Segura , Elísabet Pires , Wolfgang K. Maser , Ana M. Benito , Enrique García-Bordejé , José M. González-Domínguez
The bottom-up assembly of cellulose nanocrystals (CNCs) into porous scaffolds offers a sustainable route to translate their intrinsic properties into functional 3D materials. This strategy enables precise control over porous architectures, unlocking opportunities for high-performance materials tailored to specific applications. Here, we present the fabrication of structured carbons derived from nanocellulose precursors. CNCs are isolated from cellulosic feedstock in type-I and type-II crystalline allomorphs via a one-pot synthesis process followed by minimal processing steps. The resulting aqueous CNC colloids self-assemble into cross-linked hydrogels through controlled hydrothermal aggregation, followed by lyophilization to produce macroporous aerogels (bulk porosities up to 98%). Each allomorph exhibits distinct aggregation behavior, explored for the first time with type-II CNCs. As proof of concept, these aerogels undergo pyrolysis at varying temperatures and subsequent sulfonation, yielding highly porous carbons functionalized with sulfonic acid groups (functionalization degree of ca. 2400 μmol·g−1). The resulting materials combine macroporosity from hydrothermal assembly with microporosity generated during pyrolysis and sulfonation, forming a hierarchical structure ideal for catalytic applications. Their performance is demonstrated in solketal synthesis (yielding ∼90% of solketal in consecutive cycles after 4 h at room temperature) positioning CNC-based sulfonated aerogels as a greener alternative to conventional Brønsted acid catalysts and surpassing classical activated carbons in sustainability and design.
纤维素纳米晶体(cnc)自底向上组装成多孔支架,为将其固有特性转化为功能性3D材料提供了一条可持续的途径。这种策略可以精确控制多孔结构,为特定应用量身定制的高性能材料提供机会。在这里,我们提出了由纳米纤维素前体衍生的结构碳的制造。cnc是从i型和ii型晶体异形体的纤维素原料中分离出来的,通过一锅合成过程,然后进行最小的加工步骤。所得的CNC水性胶体通过受控的水热聚集自组装成交联的水凝胶,然后进行冻干生产大孔气凝胶(体积孔隙率高达98%)。每种异构体都表现出不同的聚集行为,这是第一次用ii型cnc进行研究。作为概念的证明,这些气凝胶在不同温度下进行热解和随后的磺化,得到具有磺酸基的高多孔碳(功能化度约为2400 μmol·g−1)。所得到的材料结合了水热组装的大孔隙和热解和磺化过程中产生的微孔隙,形成了理想的催化应用的分层结构。它们的性能在溶胶合成中得到了证明(在室温下连续循环4小时后产生约90%的溶胶),这使得基于cnc的磺化气凝胶成为传统Brønsted酸催化剂的更环保的替代品,并且在可持续性和设计上超越了传统活性炭。
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Carbohydrate Polymer Technologies and Applications
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