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Synergistic effect of ZnO-GO and APTMS on the structure and performance of PVDF hollow fiber membranes ZnO-GO和APTMS对PVDF中空纤维膜结构和性能的协同效应
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139609
Junhui Ou, Jinpeng Mo, Zhenyu Wu, Meilin Zhang, Hui Wen, Zhifeng Huang, Litong Chen, Ruihang Xie, Yang Wang, Longfei Fan, Chunping Ma
Poly(vinylidene fluoride) (PVDF) hollow fiber membranes, despite their advantages in wastewater treatment, suffer from inherent hydrophobicity. This research has presented a approach to address by fabricating a composite membrane via non-solvent-induced phase separation. The membrane incorporated a hydrothermally synthesized zinc oxide-graphene oxide (ZnO-GO) composite, with 3-aminopropyltrimethoxysilane (APTMS) as a coupling agent to enhance the dispersion of ZnO-GO within the polymer matrix and introduce additional hydrophilic amino groups. The results demonstrated that the well-dispersed ZnO-GO composite, along with the chemical functionality provided by APTMS, led to a membrane with modulated surface roughness, and notably improved hydrophilicity. This synergistic modification resulted in superior separation performance: a pure water flux of 153.7 L m−2 h−1, a 99.88 % rejection rate for Direct Orange 26 dye, and an exceptional antifouling capability with over 92 % emulsified oil rejection. Furthermore, the composite membrane exhibited reduced mass transfer activation energy, underscoring its potential for energy-efficient filtration in dyeing wastewater treatment.
聚偏氟乙烯(PVDF)中空纤维膜虽然在污水处理中具有一定的优势,但其固有的疏水性是其缺点之一。本研究提出了一种通过非溶剂诱导相分离制备复合膜的方法。该膜采用水热合成的氧化锌-氧化石墨烯(ZnO-GO)复合材料,以3-氨基丙基三甲氧基硅烷(APTMS)作为偶联剂,以增强ZnO-GO在聚合物基体中的分散,并引入额外的亲水性氨基。结果表明,分散良好的ZnO-GO复合材料,加上APTMS提供的化学功能,使膜的表面粗糙度得到了调节,亲水性得到了显著提高。这种协同改性导致了卓越的分离性能:纯水通量为153.7 L m−2 h−1,直接橙26染料的去除率为99.88 %,并且具有超过92 %的乳化油去除率的特殊防污能力。此外,复合膜表现出较低的传质活化能,强调了其在印染废水处理中的节能过滤潜力。
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引用次数: 0
A versatile ionic liquid functionalized macromolecular nano-coating via surface-initiated PET-RAFT: Imparting flame retardancy, anti-dripping, and smoke suppression to polyester fabrics 一种多用途的离子液体功能化大分子纳米涂层,通过表面引发PET-RAFT:赋予聚酯织物阻燃、防滴和抑烟性
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139665
Mengru Li , Ailin Sun , Wenqing Wang , Pengfei Qi , Zhiguo Zhu , Changhuan Zhang , Menghan Guo , Yifan Yan , Rui Wang
With the wide textiles usage and the increasing concern on the public security, high-quality fire-resistant fabrics are quite demanding but still challenging. Herein, environmentally friendly ionic liquids (ILs) was empolyed as the main flame retardant and was grafted onto polyester fabrics by the photo-induced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) technology under yellow LED irradiation. Firstly, chain transfer agent (CTA) 4-Cyano-4- [(dodecylsulfanylthiocarbonyl) sulfanyl] pentanoic (CDTPA) was deposited onto polydopamine-modified polyester fabrics, followed by glycidyl methacrylate (GMA) in-suit polymerization via surface-initiated PET-RAFT. Finally, ILs were grafted via secondary functionalization. The controlled PET-RAFT growth of PGMA was realized with a linear growth in the Mn with [M]: [CTA] kept increasing within the range of [M]:[CTA]< 500:1 and a relatively narrow Mn distribution (PDI<1.25). An apparent core-shell structure of polyester fiber was observed with 200–500 nm nanocoating. When the PGMA and IL grafting ratios were 3.29 wt% and 3.13 wt% respectively, both smoke release rate and total heat release were reduced by 30.3 % and 73.5 %, respectively, exhibiting excellent fire-resistant and smoke suppression performance. Furthermore, the fabrics achieved UL-94 V-0 grade with no melt dripping, and the limiting oxygen index (LOI) got 28 %. The ID/IG value of the residual char decreased by 24.4 %, indicating promoted degree of graphitization under the ILs catalyzation. The flame-retardant performance of this material derived from the synergistic effect of gas-phase radical quenching and condensed-phase char layer protection, while the residual char also contributed to its excellent anti-dripping behavior. This study provided a robust, energy conservation and eco-friendly strategy for the fabrication of high quality flame retardant fabrics with non-melt dripping.
随着纺织品的广泛使用和人们对公共安全的日益关注,高质量的防火面料要求很高,但仍然具有挑战性。本文以环境友好型离子液体(ILs)为主要阻燃剂,在黄色LED照射下采用光致电子转移可逆加成-破碎链转移(PET-RAFT)技术将其接枝到聚酯织物上。首先,将链转移剂(CTA) 4-氰基-4-[(十二烷基磺酰硫羰基)磺酰]戊酸(CDTPA)沉积在聚多巴胺改性聚酯织物上,然后通过表面引发PET-RAFT将甲基丙烯酸缩水甘油酯(GMA)在织物上聚合。最后,通过二级官能化接枝il。在[M]:[CTA]<; 500:1范围内,[M]:[CTA]不断增大,Mn分布较窄(PDI<1.25),实现了PGMA的可控PET-RAFT生长,Mn呈线性增长。采用200-500 nm的纳米涂层,观察到聚酯纤维具有明显的核壳结构。当PGMA和IL接枝率分别为3.29 wt%和3.13 wt%时,烟释放率和总放热率分别降低30.3 %和73.5 %,具有良好的防火抑烟性能。织物达到UL-94 V-0级,无熔滴,极限氧指数(LOI)达到28 %。残炭的ID/IG值降低了24.4 %,表明在il催化下石墨化程度提高。该材料的阻燃性能来源于气相自由基猝灭和凝聚相炭层保护的协同作用,而残余炭也促成了其优异的防滴性能。本研究为制备高品质无熔滴阻燃织物提供了一种可靠、节能、环保的方法。
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引用次数: 0
Synergistic adsorption of flocculant on quartz surface: Insights from experiment and molecular dynamics simulation 絮凝剂在石英表面的协同吸附:来自实验和分子动力学模拟的见解
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139677
Xiaowei Huang , Bao Ren , Fanfei Min , Jun Chen , Jiaqiang Zhu , Shangyu Hu
Efficient treatment of fine-grained tailings represents a pressing challenge in mineral industry. This study investigates polyacrylamide-based flocculants in a two-step flocculation process for enhanced solid-liquid separation of quartz suspensions. Combining experiment and simulation elucidated the synergistic mechanism of flocculant addition sequence at the quartz / water interface. Experiments demonstrated two-step flocculation significantly improved settling performance over single-flocculant process. Cationic polyacrylamide (CPAM) as the first-step flocculant yielded superior turbidity reduction, while incorporating non-ionic polyacrylamide (NPAM) or anionic polyacrylamide (APAM) markedly improved floc settling velocity. Molecular dynamics (MD) simulations revealed a stable "cation-anion molecular bridge" in the (C+A)&Surface system. This structure arises from the sequential, strongly coupled adsorption of CPAM and APAM, stabilized by synergistic electrostatic and hydrogen-bonding interactions. Its high continuity and strong intermolecular coupling establish it as the key structural basis for achieving highly efficient flocculation. In contrast, the (C+C)&Surface and (C+N)&Surface systems showed weak interlayer connections caused poor bridging. Using NPAM or APAM as the first-step flocculant resulted in high turbidity (400 – 4000 NTU) due to weak hydrogen bonding or electrostatic repulsion. This research clarifies the micro-scale synergy mechanism of two-step flocculation. It bridges the gap in atomic-level investigation where traditional experimental methods fall short, providing a theoretical basis and technical support for improved tailings treatment process.
细粒尾矿的高效处理是矿业行业面临的一个紧迫挑战。本研究考察了聚丙烯酰胺基絮凝剂在两步絮凝过程中对石英悬浮液固液分离的增强作用。实验与模拟相结合,阐明了絮凝剂添加顺序在石英/水界面的协同作用机理。实验表明,两步絮凝比单步絮凝明显改善了沉降性能。阳离子聚丙烯酰胺(CPAM)作为第一步絮凝剂具有较好的降浊效果,而加入非离子聚丙烯酰胺(NPAM)或阴离子聚丙烯酰胺(APAM)可显著提高絮凝体沉降速度。分子动力学(MD)模拟表明,在(C+ a)表面体系中存在一个稳定的“阳离子-阴离子分子桥”。这种结构源于CPAM和APAM的顺序,强耦合吸附,通过协同静电和氢键相互作用稳定。它的高连续性和强分子间偶联使其成为实现高效絮凝的关键结构基础。相比之下,(C+C)&;Surface和(C+N)&;Surface体系的层间连接较弱,导致桥接不良。使用NPAM或APAM作为一级絮凝剂,由于氢键或静电斥力较弱,导致浊度较高(400 - 4000 NTU)。本研究阐明了两步絮凝的微观协同机理。它弥补了传统实验方法在原子水平研究上的不足,为改进尾矿处理工艺提供了理论依据和技术支持。
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引用次数: 0
Construction of responsive photonic crystal patterns via tunable evaporation-induced assembly of soft core-shell nanospheres 通过可调蒸发诱导组装软核-壳纳米球构建响应光子晶体模式
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139675
Huiyang Wang , Xiaohu Wu , Ting Lü , Dongming Qi , Ying Pan , Dihua Wu , Suling Zhang , Dong Zhang , Hongting Zhao
Evaporation-induced assembly of responsive core-shell soft nanospheres is one of the most convenient routes to construct responsive photonic crystal (RPC) film patterns. Nevertheless, a fundamental understanding of how emulsion composition and film formation conditions dictate the microstructure of resulting RPC films is still lacking. This lack of mechanistic insight constitutes a major bottleneck to promote the quality and functionality of RPC films. In this study, a series of monodisperse core-shell nanospheres with different size and glass transition temperature (Tg) have been facilely synthesized via soap-free emulsion polymerization, and then used to fabricate RPC film patterns by just drying the nanosphere emulsion in the patterned concaves under various conditions. Impacts of the ethylene glycol (EG) content, film formation humidity and temperature on the microstructure of resultant RPC films were mainly studied, and their influence mechanism was then clarified by combination of the structural color display of RPC film patterns after contact with water. The originally prepared RPC films were transparent, but could display brilliant structural color after wetting with water due to the increase of refractive index (RI) contrast of colloidal array. With EG content or humidity increasing, the structural color showed blue shift due to the denser colloidal stacking in pattern center induced by the suppression of the coffee-ring effect. With film formation temperature rising, the structural color displayed red shift at first due to the aroused coffee-ring effect, but then turned blue shift due to the formation of colloid skin (i.e. ordered accumulation and arrangement of nanospheres at air-liquid interface), which became denser with rising temperature. Besides, the fabricated RPC film patterns could display responsive structural color change under the stimuli of the pH, ionic strength and temperature of water as well as the organic solvent. Eventually, a multi-responsive colloidal crystal film pattern was successfully constructed. In summary, this study systematically elucidates the regulatory mechanisms of the microstructure of RPC films, providing a solid theoretical foundation and feasible process strategies for the controllable fabrication of high-performance anti-counterfeiting patterns.
响应性核壳软纳米球的蒸发诱导组装是构建响应性光子晶体(RPC)薄膜模式最便捷的途径之一。然而,对乳液组成和成膜条件如何决定RPC膜的微观结构的基本理解仍然缺乏。这种缺乏机制的洞察力构成了提高RPC薄膜质量和功能的主要瓶颈。在本研究中,通过无皂乳液聚合制备了一系列具有不同尺寸和玻璃化转变温度(Tg)的单分散核壳纳米球,然后在不同条件下将纳米球乳液在图案凹面中干燥,制备RPC膜图案。主要研究了乙二醇(EG)含量、成膜湿度和温度对所得RPC膜微观结构的影响,并结合RPC膜图案与水接触后的结构显色,阐明了它们的影响机理。原制备的RPC膜是透明的,但由于胶体阵列的折射率(RI)对比度增加,经水润湿后可以显示出明亮的结构颜色。随着EG含量或湿度的增加,由于咖啡环效应的抑制,图案中心的胶体堆积更加密集,结构颜色呈现蓝移。随着成膜温度的升高,由于咖啡环效应的激发,结构颜色先呈现红移,然后由于胶体皮的形成(即纳米球在气液界面的有序堆积和排列)而呈现蓝移,随着温度的升高,胶体皮变得更致密。此外,制备的RPC膜图案在水的pH、离子强度、温度以及有机溶剂的刺激下表现出响应性的结构颜色变化。最终,成功构建了一个多响应的胶体晶体薄膜结构。综上所述,本研究系统地阐明了RPC膜微观结构的调控机制,为高性能防伪图案的可控制备提供了坚实的理论基础和可行的工艺策略。
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引用次数: 0
Influence of sulfate and amide groups in different polysaccharides (fucoidan, chitosan, and levan) on the intermolecular interaction affinity with albumin 不同多糖(岩藻聚糖、壳聚糖和levan)中硫酸盐和酰胺基团对与白蛋白分子间相互作用亲和力的影响
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139678
Iago Dillion Lima Cavalcanti , Andreza Tallyne de Aguiar Silva , Vinícius Alexandre Fiaia Costa , Bruno Júnior Neves , Leandro Paes de Brito , José Maria Barbosa-Filho , Evandro Ferreira da Silva , Marcelo Sobral da Silva , Francisca Crislândia Oliveira Silva , Eloisa Berbel Manaia , Gilles Ponchel , Nereide Stela Santos Magalhães , Mariane Cajubá de Britto Lira Nogueira , Francisco Humberto Xavier-Júnior
Polysaccharides are increasingly being utilized in the development of pharmaceutical products due to their therapeutic properties, as well as their biocompatibility and biodegradability. Human serum albumin (HSA), an abundant protein in the body responsible for the biodistribution of molecules, has also been used to develop pharmaceutical products. Evaluating the interaction of these molecules is one of the extremely important preliminary steps in the development of a new product, considering the formation of complexes for the adsorption of albumin on the surface of nanocapsules, for example, for the targeted release of drugs at specific locations. Therefore, this study aimed to evaluate the interactions between fucoidan, chitosan, and levan with HSA, considering physicochemical and computational parameters. Isothermal titration calorimetry (ITC), Fourier-transform infrared spectroscopy (FT-IR), Hydrogen nuclear magnetic resonance (1H NMR), Scanning electron microscopy (SEM), and molecular docking to identify the mechanisms of interaction between the polysaccharides and HSA. By ITC analysis, all bindings occurred spontaneously (ΔG < 0), when fucoidan and chitosan were used, the interaction occurred through endothermic interactions (ΔH > 0 kJ.mol−1), while levan presented exothermic ones (ΔH= −128 kJ.mol−1). 1H NMR and FT-IR analysis indicate distinct binding mechanisms, wherein fucoidan seems to be associated primarily with sulfate groups, chitosan with hydroxyl groups, and levan with interactions occurring notably in the furanose region. The SEM results suggest the formation of complexes, with changes in the surface of the materials after the formation of the polysaccharide-HSA complex. Subsequently, an ensemble docking protocol revealed that chitosan exhibited the most stable interactions with HSA, characterized by high binding affinity and stable hydrogen bonds. Fucoidan, chitosan, and levan interact with HSA, however, chitosan stands out for its greater binding affinity. This work introduces techniques that allow for the evaluation of the interaction of polysaccharides with HSA, with consistent results that corroborate those presented in the literature. Furthermore, it offers innovative results that ensure the use of these complexes in the development of new products.
多糖由于其治疗特性以及生物相容性和生物可降解性,越来越多地应用于医药产品的开发。人血清白蛋白(HSA)是一种丰富的蛋白质,负责分子的生物分布,也被用于开发药物产品。评估这些分子的相互作用是开发新产品的极其重要的初步步骤之一,考虑到在纳米胶囊表面吸附白蛋白的配合物的形成,例如,在特定位置靶向释放药物。因此,本研究旨在考虑物理化学和计算参数,评估岩藻糖聚糖、壳聚糖和李凡与HSA的相互作用。采用等温滴定量热法(ITC)、傅里叶变换红外光谱法(FT-IR)、氢核磁共振(1H NMR)、扫描电镜(SEM)、分子对接等方法对多糖与HSA的相互作用机制进行了研究。通过ITC分析,所有结合都是自发发生的(ΔG < 0),当使用岩藻糖聚糖和壳聚糖时,相互作用通过吸热相互作用发生(ΔH > 0 kJ)。(ΔH=−128 kJ.mol−1)。1H NMR和FT-IR分析显示了不同的结合机制,其中褐藻糖聚糖似乎主要与硫酸盐基团相关,壳聚糖与羟基相关,而利文则主要发生在呋喃糖区域的相互作用。SEM结果表明,多糖- hsa复合物形成后,材料表面发生了变化。结果表明,壳聚糖与HSA的相互作用最稳定,具有较高的结合亲和力和稳定的氢键。岩藻聚糖、壳聚糖和利凡与HSA相互作用,然而,壳聚糖以其更大的结合亲和力而脱颖而出。这项工作介绍了技术,允许评价多糖与HSA的相互作用,一致的结果,证实了那些在文献中提出的。此外,它提供了创新的结果,确保这些配合物在新产品开发中的使用。
{"title":"Influence of sulfate and amide groups in different polysaccharides (fucoidan, chitosan, and levan) on the intermolecular interaction affinity with albumin","authors":"Iago Dillion Lima Cavalcanti ,&nbsp;Andreza Tallyne de Aguiar Silva ,&nbsp;Vinícius Alexandre Fiaia Costa ,&nbsp;Bruno Júnior Neves ,&nbsp;Leandro Paes de Brito ,&nbsp;José Maria Barbosa-Filho ,&nbsp;Evandro Ferreira da Silva ,&nbsp;Marcelo Sobral da Silva ,&nbsp;Francisca Crislândia Oliveira Silva ,&nbsp;Eloisa Berbel Manaia ,&nbsp;Gilles Ponchel ,&nbsp;Nereide Stela Santos Magalhães ,&nbsp;Mariane Cajubá de Britto Lira Nogueira ,&nbsp;Francisco Humberto Xavier-Júnior","doi":"10.1016/j.colsurfa.2026.139678","DOIUrl":"10.1016/j.colsurfa.2026.139678","url":null,"abstract":"<div><div>Polysaccharides are increasingly being utilized in the development of pharmaceutical products due to their therapeutic properties, as well as their biocompatibility and biodegradability. Human serum albumin (HSA), an abundant protein in the body responsible for the biodistribution of molecules, has also been used to develop pharmaceutical products. Evaluating the interaction of these molecules is one of the extremely important preliminary steps in the development of a new product, considering the formation of complexes for the adsorption of albumin on the surface of nanocapsules, for example, for the targeted release of drugs at specific locations. Therefore, this study aimed to evaluate the interactions between fucoidan, chitosan, and levan with HSA, considering physicochemical and computational parameters. Isothermal titration calorimetry (ITC), Fourier-transform infrared spectroscopy (FT-IR), Hydrogen nuclear magnetic resonance (<sup>1</sup>H NMR), Scanning electron microscopy (SEM), and molecular docking to identify the mechanisms of interaction between the polysaccharides and HSA. By ITC analysis, all bindings occurred spontaneously (<em>ΔG</em> &lt; 0), when fucoidan and chitosan were used, the interaction occurred through endothermic interactions (<em>ΔH</em> &gt; 0 kJ.mol<sup>−1</sup>), while levan presented exothermic ones (ΔH= −128 kJ.mol<sup>−1</sup>). <sup>1</sup>H NMR and FT-IR analysis indicate distinct binding mechanisms, wherein fucoidan seems to be associated primarily with sulfate groups, chitosan with hydroxyl groups, and levan with interactions occurring notably in the furanose region. The SEM results suggest the formation of complexes, with changes in the surface of the materials after the formation of the polysaccharide-HSA complex. Subsequently, an ensemble docking protocol revealed that chitosan exhibited the most stable interactions with HSA, characterized by high binding affinity and stable hydrogen bonds. Fucoidan, chitosan, and levan interact with HSA, however, chitosan stands out for its greater binding affinity. This work introduces techniques that allow for the evaluation of the interaction of polysaccharides with HSA, with consistent results that corroborate those presented in the literature. Furthermore, it offers innovative results that ensure the use of these complexes in the development of new products.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"736 ","pages":"Article 139678"},"PeriodicalIF":5.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146036457","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
In-situ precipitation synthesis of BiVO4/AgBiO3 heterojunction with enhanced charge dynamics and superior photodegradation performance 原位沉淀法合成具有增强电荷动力学和光降解性能的BiVO4/AgBiO3异质结
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139672
Guyu Sun , Jingshun Xu , Jianwei Tao , Rui Zhang , Yuhong Wang
How to design semiconductor-based photocatalyst with enhanced charge separation efficiency, broader light absorption, and structural robustness remains some challenges. Herein, we report the construction of a BiVO4/AgBiO3 (BA) heterojunction photocatalyst via a facile in-situ precipitation method. The heterojunction, featuring a type-II band alignment, enables efficient spatial separation of photogenerated carriers and improved interfacial charge transfer. Among the prepared heterojunctions, the optimized BA-1.5 exhibits superior visible-light-driven degradation efficiencies of 95 % for rhodamine B and 82 % for tetracycline, markedly outperforming the pristine BiVO4 and AgBiO3. Mechanism investigations reveal that the photodegradation process is dominated by holes (h⁺) and superoxide radicals (·O₂⁻). This study provides a new material platform and mechanistic insight for rationally designing heterojunction photocatalysts with enhanced charge dynamics, offering a viable strategy for future photocatalytic environmental remediation.
如何设计出电荷分离效率高、光吸收范围广、结构坚固的半导体光催化剂仍然是一个挑战。在此,我们报道了用原位沉淀法构建BiVO4/AgBiO3 (BA)异质结光催化剂。该异质结具有ii型带对准,可实现光生载流子的有效空间分离,并改善界面电荷转移。在所制备的异质结中,优化后的BA-1.5对罗丹明B的可见光降解效率为95 %,对四环素的可见光降解效率为82 %,明显优于原始的BiVO4和AgBiO3。机理研究表明,光降解过程以空穴(h +)和超氧自由基(·O₂⁻)为主。本研究为合理设计具有增强电荷动力学的异质结光催化剂提供了新的材料平台和机理见解,为未来光催化环境修复提供了可行的策略。
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引用次数: 0
Interfacial charge engineering through in-situ Ag2S@S/CoAl-LDH heterojunction: Dual kinetic promotion via built-in electric field for efficient water oxidation 原位Ag2S@S/煤- ldh异质结界面电荷工程:内置电场双动力学促进高效水氧化
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.colsurfa.2026.139644
Hua-nan Zhang , Zhengang Guo , Huiping Zhang , Pengju Li , Hongyan Shen , Chaopeng Ren
The construction and regulation of heterojunctions and their associated built-in electric fields (BIEFs) represent an effective strategy for enhancing the electrochemical overall water splitting performance of transition metal-based electrocatalysts. In this study, we develop an innovative approach to induce a strong BIEF through in-situ construction of a heterojunction, enabling precise electronic structure modulation of CoAl-LDH within the heterojunction framework, thereby significantly improving electrocatalytic water splitting performance. Specifically, an Ag2S@S/CoAl-LDH heterojunction system was designed and synthesized via interfacial chemical coupling between a p-type semiconductor (Ag2S) and an n-type semiconductor (CoAl-LDH). Both theoretical and experimental results confirm the formation of a high-intensity BIEF at the heterojunction interface, which drives directional charge transfer across the interface. Furthermore, the BIEF induces electronic localization reconstruction at the metal centers (Co2 +) of CoAl-LDH, significantly elevating the d-band center and enhancing its catalytic activity. Benefiting from this optimized electronic structure, the Ag2S@S/CoAl-LDH catalyst exhibits outstanding oxygen evolution reaction (OER) performance in 1.0 M KOH, requiring an overpotential of only 197 mV to achieve a current density of 10 mA·cm−2, along with a low Tafel slope of 56.6 mV·dec−1. Density functional theory (DFT) calculations further reveal that the enhanced BIEF at the p-n heterojunction interface significantly reduces the energy barrier of the OER rate-determining step while optimizing the adsorption free energy of reaction intermediates. These findings underscore the dual role of interfacial electronic interactions in promoting reaction kinetics: the BIEF not only facilitates interfacial charge transfer but also strengthens the adsorption of reactants and intermediates, thereby improving both the reaction rate and overall catalytic performance. This study employs a p-n heterojunction engineering strategy to induce a built-in electric field, offering key insights for the design of high-performance electrode materials. The spontaneous construction of a BIEF for electrode optimization demonstrates considerable potential for application in clean energy technologies.
异质结及其相关内置电场的构建和调控是提高过渡金属基电催化剂电化学整体水分解性能的有效策略。在本研究中,我们开发了一种创新的方法,通过原位构建异质结来诱导强BIEF,从而在异质结框架内实现对煤- ldh的精确电子结构调制,从而显着提高电催化水分解性能。具体而言,通过p型半导体(Ag2S)和n型半导体(CoAl-LDH)之间的界面化学耦合,设计并合成了Ag2S@S/CoAl-LDH异质结体系。理论和实验结果均证实在异质结界面处形成了高强度的BIEF,并驱动了电荷在界面上的定向转移。此外,BIEF诱导了煤- ldh金属中心(Co2 +)的电子定位重建,显著提升了d带中心,增强了其催化活性。得益于这种优化的电子结构,Ag2S@S/煤- ldh催化剂在1.0 M KOH下表现出出色的析氧反应(OER)性能,只需要197 mV的过电位就可以实现10 mA·cm−2的电流密度,以及56.6 mV·dec−1的低塔非斜率。密度泛函理论(DFT)计算进一步表明,在p-n异质结界面处增强的BIEF显著降低了OER速率决定步骤的能垒,同时优化了反应中间体的吸附自由能。这些发现强调了界面电子相互作用在促进反应动力学中的双重作用:BIEF不仅促进了界面电荷转移,还加强了对反应物和中间体的吸附,从而提高了反应速率和整体催化性能。本研究采用p-n异质结工程策略来诱导内置电场,为高性能电极材料的设计提供关键见解。自发构建用于电极优化的BIEF在清洁能源技术中具有相当大的应用潜力。
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引用次数: 0
Rational design and mechanistic elucidation of targeted lysosomal quantum dot nanoplatforms for enhanced anticancer efficacy 靶向溶酶体量子点纳米平台增强抗癌功效的合理设计和机制阐明
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.colsurfa.2026.139640
Peng Yuan , Wen-Hao Zhang , Bin Ren , Mei-Xia Zhao
Quantum dot (QD)-based nano-drug delivery systems (DDSs) represent a promising strategy to overcome the limitations of conventional cancer therapies, such as poor bioavailability, off-target effects, and systemic toxicity. In this study, we developed a lysosome-targeted nano-drug delivery system (LT-DDS) designated as CdSe/ZnS@PEI-SS-COOH-DOX-TAT, which was constructed using CdSe/ZnS core/shell QDs with high fluorescence quantum yield and excellent colloidal stability, synthesized via a well-established organometallic route. The LT-DDS exhibited enhanced tumor selectivity, preferentially accumulating in the lysosomes of cancer cells while showing minimal cytotoxicity toward normal cells. Mechanistic studies revealed that the system not only significantly inhibited tumor cell proliferation but also induced mitochondria-mediated apoptosis through activation of caspase-3 signaling pathways. Conjugation with the trans-activator of transcription (TAT) peptide promoted efficient cellular uptake and lysosomal trafficking, ultimately leading to lysosomal membrane permeabilization (LMP) and subsequent caspase activation. These findings establish the LT-DDS as a promising tumor-specific drug delivery platform, offering improved therapeutic efficacy and biosafety over conventional DDSs.
基于量子点(QD)的纳米药物递送系统(dds)代表了一种很有前途的策略,可以克服传统癌症治疗的局限性,如生物利用度差、脱靶效应和全身毒性。在本研究中,我们开发了一种靶向溶酶体的纳米药物递送系统(LT-DDS),命名为CdSe/ZnS@PEI-SS-COOH-DOX-TAT,该系统采用CdSe/ZnS核/壳量子点构建,具有高荧光量子产率和优异的胶体稳定性,通过完善的有机金属途径合成。LT-DDS表现出增强的肿瘤选择性,优先积聚在癌细胞的溶酶体中,同时对正常细胞表现出最小的细胞毒性。机制研究表明,该系统不仅能显著抑制肿瘤细胞增殖,还能通过激活caspase-3信号通路诱导线粒体介导的细胞凋亡。与转录反式激活因子(TAT)肽的结合促进了高效的细胞摄取和溶酶体运输,最终导致溶酶体膜渗透(LMP)和随后的半胱天冬酶激活。这些研究结果表明,LT-DDS是一种有前景的肿瘤特异性药物传递平台,与传统的dds相比,它具有更好的治疗效果和生物安全性。
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引用次数: 0
Organic–inorganic hybrid PVDF membranes constructed via click chemistry for efficient oil–water emulsion separation 有机-无机杂化PVDF膜通过点击化学构建高效油水乳液分离
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.colsurfa.2026.139645
Zhenyu Ni, Mengnan Yu, Yanwei Du, Tianxiang Wu, Rongzhan Liu
The high stability of emulsified oily wastewater and the susceptibility of conventional membranes to oil fouling often led to severe flux decline and reduced separation efficiency, making the development of efficient and stable oil/water emulsion separation membranes an urgent challenge. Here, we developed an organic-inorganic hybrid poly (vinylidene fluoride) (PVDF) composite membrane by constructing a hierarchical three-layer structure. Specifically, a one-pot sol-gel process generated a rough titania (TiO2) layer enriched with thiol groups, which subsequently served as anchoring sites for the covalent grafting of poly (dimethylsiloxane) (PDMS) molecular brushes via a UV-initiated thiol-ene click chemistry reaction. The robust PDMS brushes not only tailored the surface wettability but also endowed the membrane with remarkable anti-fouling and easy-cleaning capabilities, and the methyl blue contaminants on the membrane surface can be removed by water droplets. The membrane exhibits outstanding hydrophobic-oleophilic properties, with a water contact angle of 131.3° and an oil contact angle of 0°, achieving a separation efficiency of 99.3 % for water/soybean oil emulsions with a flux of 548.7 L·m−2·h−1, outperforming unmodified membranes in separation efficiency. This performance enhancement is attributed to the synergistic effect between the selective oil-capturing behavior of PDMS molecular brushes and the capillary effect of the rough TiO2 structure, which together promote preferential oil transport and efficient water-blocking performance. In addition, the covalently anchored interface provides excellent chemical stability, allowing it to maintain stable performance even in harsh environments. This research provides a novel strategy for developing highly efficient and stable organic-inorganic hybrid separation membranes, offering broad application prospects in the treatment of oily wastewater.
乳化含油废水的高稳定性和常规膜对油垢的易感性往往导致通量严重下降,分离效率降低,开发高效、稳定的油水乳化分离膜是一个迫切的挑战。在这里,我们通过构建层次化的三层结构,开发了有机-无机杂化聚偏氟乙烯(PVDF)复合膜。具体来说,一锅溶胶-凝胶工艺生成了富含巯基的粗糙二氧化钛(TiO2)层,该层随后通过紫外线引发的巯基点击化学反应作为聚二甲基硅氧烷(PDMS)分子刷共价接枝的锚定位点。坚固耐用的PDMS毛刷不仅定制了膜的表面润湿性,还赋予了膜卓越的防污和易清洗能力,膜表面的甲基蓝污染物可以通过水滴去除。该膜具有优异的疏油亲水性,水接触角为131.3°,油接触角为0°,对水/豆油乳剂的分离效率为99.3 %,通量为548.7 L·m−2·h−1,分离效率优于未改性膜。这种性能的增强是由于PDMS分子刷的选择性捕油行为与粗糙TiO2结构的毛细效应之间的协同作用,共同促进了油的优先输运和高效的阻水性能。此外,共价锚定界面提供了出色的化学稳定性,即使在恶劣环境下也能保持稳定的性能。本研究为开发高效、稳定的有机-无机杂化分离膜提供了新思路,在含油废水处理中具有广阔的应用前景。
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引用次数: 0
EPSTI1 inhibitor-encapsulated RADA16@GelMA multifunctional hydrogel for the repair of osteoporotic bone defects EPSTI1抑制剂包封RADA16@GelMA多功能水凝胶修复骨质疏松性骨缺损
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.colsurfa.2026.139648
Yong Tao , Yuxing Chen , Qingtao Wang , Qianxing Deng , Bin He
The repair of osteoporotic bone defects is still challenging because the injury sites are accompanied by elevated bone resorption and reduced bone regeneration. Our previous study found that the inhibition of epithelial stromal interaction 1 (EPSTI1) was effective to hinder bone resorption, while RADA16 peptide nanofibers were beneficial to improve bone formation. Thus, one multifunctional composite hydrogel (i.e. RADA16/siEPSTI1@GelMA hydrogel) containing EPSTI1 inhibitor (i.e. EPSTI1 siRNA) and RADA16 peptide nanofibers was designed and constructed in present research. In vitro experiments showed that the addition of EPSTI1 siRNA (siEPSTI1) into the composite hydrogel effectively restrained osteoclastogenic differentiation and osteoclastogenesis, while this RADA16/siEPSTI1@GelMA hydrogel also promoted osteogenic differentiation and calcium nodule formation. In vivo animal experiments exhibited that the composite hydrogel can substantially inhibit bone resorption and enhance the repair of osteoporotic bone defects. Collectively, these findings imply that RADA16/siEPSTI1@GelMA multifunctional hydrogel holds great promise to promote the repair of osteoporotic bone defects in terms of reducing bone resorption and enhancing bone formation.
骨质疏松性骨缺损的修复仍然具有挑战性,因为损伤部位伴随着骨吸收升高和骨再生减少。我们前期研究发现,抑制上皮基质相互作用1 (epithelial stromal interaction 1, EPSTI1)可有效阻碍骨吸收,而RADA16肽纳米纤维有利于促进骨形成。因此,本研究设计并构建了一种含有EPSTI1抑制剂(即EPSTI1 siRNA)和RADA16肽纳米纤维的多功能复合水凝胶(即RADA16/siEPSTI1@GelMA水凝胶)。体外实验表明,在复合水凝胶中加入EPSTI1 siRNA (siEPSTI1)能有效抑制破骨细胞分化和破骨细胞发生,同时该RADA16/siEPSTI1@GelMA水凝胶还能促进成骨分化和钙结节形成。体内动物实验表明,复合水凝胶能显著抑制骨吸收,促进骨质疏松性骨缺损的修复。总之,这些发现表明RADA16/siEPSTI1@GelMA多功能水凝胶在减少骨吸收和促进骨形成方面具有促进骨质疏松性骨缺损修复的巨大希望。
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Colloids and Surfaces A: Physicochemical and Engineering Aspects
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