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Rheology and interaction mechanisms of polyelectrolyte-wormlike micellar surfactant complexes: A two-dimensional correlation spectroscopy and time-concentration superposition study 聚电解质-蠕虫状胶束表面活性剂配合物的流变性和相互作用机理:二维相关光谱和时间-浓度叠加研究
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139621
Duccio Tatini , Alberto Fidi , Mert Acar , Pierandrea Lo Nostro
This study investigates the rheological behavior and molecular interaction mechanism of polyelectrolyte–wormlike micellar complexes formed by potassium oleate (KOL) with either ε-poly-L-lysine (PL) or poly(acrylic acid) (PAA) in water. Steady shear and oscillatory rheology experiments, combined with confocal laser scanning microscopy (CLSM), were performed to evaluate the effect of polyelectrolyte charge and concentration on the micellar organization. In KOL–PL systems, a critical PL concentration (≈1.5 %) triggered a sharp viscosity increase and complex flow behavior, associated with the formation of supramolecular or coacervate-like aggregates. CLSM confirmed the appearance of structured domains at high PL content. By contrast, KOL–PAA mixtures exhibited a progressive increase in viscosity and viscoelastic moduli upon PAA addition although no aggregate could be detected by visual inspection, suggesting the onset of rearrangements at the nanoscale. Two-dimensional correlation spectroscopy (2D-COS) of attenuated total reflection Fourier-transform infrared (ATR-FTIR) data revealed distinct interaction pathways: in KOL–PL the carboxylate headgroups are the most sensitive moieties to polyelectrolyte addition, followed by alkyl tails and hydration water, consistently with a direct electrostatic binding. In KOL–PAA, the first response occurred in the hydration layer and hydrogen-bonding environment before reaching the micellar headgroups and cores, suggesting an interaction mechanism mediated by counterions and hydrogen bonds. Finally, a time–cosolute concentration superposition (TCCS) approach was successfully applied to the rheological data of both systems to obtain unified master curves and scaling laws, demonstrating its predictive value for polyelectrolyte–micelle complexes.
研究了油酸钾(KOL)与ε-聚l -赖氨酸(PL)或聚丙烯酸(PAA)在水中形成的聚电解质-虫状胶束配合物的流变行为和分子相互作用机理。通过稳态剪切和振荡流变实验,结合共聚焦激光扫描显微镜(CLSM)研究了聚电解质电荷和浓度对胶束组织的影响。在KOL-PL体系中,临界PL浓度(≈1.5 %)引发粘度急剧增加和复杂的流动行为,与超分子或聚集体的形成有关。CLSM证实了高PL含量时结构域的出现。相比之下,在加入PAA后,KOL-PAA混合物的粘度和粘弹性模量逐渐增加,尽管目测没有检测到聚集体,这表明在纳米尺度上发生了重排。衰减全反射傅里叶变换红外(ATR-FTIR)数据的二维相关光谱(2D-COS)揭示了不同的相互作用途径:在KOL-PL中,羧酸酯头基是对聚电解质添加最敏感的部分,其次是烷基尾基和水合水,与直接静电结合一致。在KOL-PAA中,反应首先发生在水合层和氢键环境中,然后才到达胶束头团和胶束核,表明其相互作用机制是由反离子和氢键介导的。最后,将时间-溶质浓度叠加(TCCS)方法成功应用于两种体系的流变数据,得到统一的主曲线和标度规律,证明了其对聚电解质-胶束配合物的预测价值。
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引用次数: 0
Molecular-scale origin of extreme disjoining pressure in water confined in carbon and silica nanopores 碳纳米孔和二氧化硅纳米孔中水中极端分离压力的分子尺度起源
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139693
Ekaterina G. Odintsova , Darya L. Gurina , Yury A. Budkov
The behavior of water under nanoscale confinement is crucial for numerous technologies; yet predicting its properties remains challenging due to the complex interplay of pore geometry and surface chemistry. While the influence of general hydrophilicity is recognized, the specific role of the flexibility of surface functional groups - a key molecular-scale feature - has remained underexplored. To address this, we conducted systematic molecular dynamics simulations to investigate the structure and disjoining pressure of water confined in slit nanopores (0.6–10 nm) with distinctly different surface chemistries: hydrophobic carbon, non-hydroxylated silica, and hydroxylated silica with both mobile and immobilized hydroxyl groups. Our results reveal that strong confinement (h < 2 nm) induces pronounced water layering, generating extreme tangential pressures. A central finding is the critical role of hydroxyl group mobility: hydrophilic silica pores induce profoundly negative disjoining pressure (-90 kbar at 0.6 nm), signifying strong effective attraction between walls, while hydroxylation significantly mitigates local stresses. Mobile hydroxyl groups promote a more stable hydration structure than rigid ones, acting as a molecular buffer. In contrast, hydrophobic carbon pores exhibit weaker attraction and a more liquid-like water state. The novelty of our work lies in isolating and quantifying the effect of surface group flexibility, demonstrating that it is a decisive factor for local stresses and thermodynamic equilibrium, beyond mere chemical identity. We show that a critical pore width of ∼3 nm marks the transition from surface-dominated to bulk-like behavior. This study underscores that precise control of nanoconfined water requires integrated consideration of both pore geometry and dynamic molecular-scale chemical characteristics. The main challenge for direct experimental comparison remains the accurate measurement of local pressures at the nanoscale. Our findings provide fundamental insights into the rational design of advanced nanoporous materials for use in membrane technology and composite science. They also propose a path for future research on charged surfaces and other confined fluids.
水在纳米尺度约束下的行为对许多技术至关重要;然而,由于孔隙几何形状和表面化学的复杂相互作用,预测其性质仍然具有挑战性。虽然一般亲水性的影响是公认的,但表面官能团的柔韧性的具体作用-一个关键的分子尺度特征-仍未得到充分探索。为了解决这个问题,我们进行了系统的分子动力学模拟,研究了具有明显不同表面化学性质的水的结构和分离压力,这些水被限制在狭缝纳米孔(0.6-10 nm)中:疏水碳、非羟基化二氧化硅和具有移动羟基和固定羟基的羟基化二氧化硅。我们的研究结果表明,强约束(h < 2 nm)诱导明显的水分层,产生极端的切向压力。一个重要的发现是羟基迁移的关键作用:亲水二氧化硅孔隙诱导深刻的负分离压力(-90 kbar, 0.6 nm),表明壁之间强大的有效吸引力,而羟基化显著减轻了局部应力。可移动的羟基比刚性的羟基促进更稳定的水合结构,起到分子缓冲的作用。疏水碳孔具有较弱的吸附力和更像液态水的形态。我们工作的新颖之处在于分离和量化了表面基团柔韧性的影响,表明它是局部应力和热力学平衡的决定性因素,而不仅仅是化学同一性。我们发现临界孔径为~ 3 nm标志着从表面主导到块状行为的转变。该研究强调,纳米密闭水的精确控制需要综合考虑孔隙几何形状和动态分子尺度化学特征。直接实验比较的主要挑战仍然是在纳米尺度上精确测量局部压力。我们的发现为合理设计用于膜技术和复合材料科学的先进纳米多孔材料提供了基本见解。他们还提出了未来研究带电表面和其他受限流体的途径。
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引用次数: 0
NMR visualization experiments and dynamic stability evaluation of nanoparticle-enhanced foam in double-layer sandstone cores 双层砂岩岩心纳米颗粒增强泡沫核磁共振可视化实验及动态稳定性评价
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139686
Yuan li , Haitao Zhang , Jun Yang
Foam-assisted enhanced oil recovery (EOR) improves sweep efficiency in heterogeneous reservoirs, but its effectiveness depends critically on foam stability, which is typically evaluated using static laboratory tests. These static approaches fail to capture the continuous defoaming and re-foaming dynamics that occur in porous media under crude oil reservoir conditions. To overcome this limitation, we combined nuclear magnetic resonance (NMR) visualization with double-layer sandstone core flooding. The effects of nanoparticle(NP) type and permeability contrast on the foam flow and foam dynamic stability (FDS) were compared. In addition, we developed an extended semi-empirical foam-flooding model that includes a NP enhancement term to simulate flow behavior and FDS. The model successfully simulated stability evolution of NPs enhanced foam in heterogeneous cores, with its parameters rigorously fitted to the experimental data. The methodology presented in this work is beneficial to evaluate and understand the transport mechanisms of foam in porous media presence of oil phase.
泡沫辅助提高采收率(EOR)提高了非均质油藏的波及效率,但其有效性主要取决于泡沫的稳定性,而泡沫稳定性通常是通过静态实验室测试来评估的。这些静态方法无法捕捉到原油储层条件下多孔介质中发生的连续消泡和再发泡动态过程。为了克服这一限制,我们将核磁共振(NMR)可视化与双层砂岩岩心驱油相结合。比较了纳米颗粒(NP)类型和渗透率对比对泡沫流动和泡沫动态稳定性的影响。此外,我们开发了一个扩展的半经验泡沫驱模型,其中包括一个NP增强项来模拟流动行为和FDS。该模型成功地模拟了非均质岩心中NPs增强泡沫的稳定性演化,其参数与实验数据拟合良好。本文所提出的方法有助于评价和理解存在油相的多孔介质中泡沫的输运机制。
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引用次数: 0
Enhancing U(VI) adsorption and recoverablity of MXene and its aerogel nanocomposite via surface alkalization treatment 通过表面碱化处理增强MXene及其气凝胶纳米复合材料对U(VI)的吸附和可回收性
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139616
Hongwei Wang , Liang Fang , Hongyu Wu , Fang Wu , Gaobin Liu , Shufang Zhang , Qirui Wang , Hongen Nian , Liyong Gan
To enhance the adsorption capacity and recoverablity of MXenes, the Ti3C2Tx were hydroxyl (OH) functionalized by a faicle alkalization treatment and the nanocomposite aerogel composed of Ti3C2(OH)0.08 and sodium alginate (SA) were subsequently fabricated. The alkalized Ti3C2Tx exhibited a maximum adsorption capacity (MAC) of 798 mg g−1 for U(VI), marking a 116 % increase over the untreated Ti3C2Tx. The adsorption experiment results were consistent with the Pseudo-second-order kinetics and the Langmuir isotherm model, confirming it is a chemisorption and monolayer adsorption. Aside from electrostatic adsorption (EA), the reduction adsorption (RA) was also found to happen during the adsorption process via a X-ray photoelectron spectroscopy (XPS) analysis, in which the U(VI) is reduced to U(IV) and the Ti(II) is oxidized to Ti(IV). The calculated adsorption energies and electron localization function (ELF) of U(VI) on the functional groups (F, O, OH) of Ti3C2Tx indicate that the OH functional group is most favorable to adsorb U(VI), which theoretically reveals the adsorption mechanism of EA&RA. Additionally, the Ti3C2(OH)0.08@SA aerogels demonstrate an efficient U(VI) adsorption even at an ultra-low concentration of 3.3 μg/L U(VI) under simulated seawater environment. The advantages of excellent adsorption, easy recovery and good reusability of the MXene- based aerogels make them very beneficial for the future practical applications as U(VI) adsorbent.
为了提高MXenes的吸附能力和可回收性,对Ti3C2Tx进行了羟基(OH)功能化处理,制备了由Ti3C2(OH)0.08和海藻酸钠(SA)组成的纳米复合气凝胶。碱化Ti3C2Tx对U(VI)的最大吸附量(MAC)为798 mg g−1,比未处理的Ti3C2Tx提高了116 %。吸附实验结果符合拟二级动力学和Langmuir等温线模型,证实其为化学吸附和单层吸附。通过x射线光电子能谱(XPS)分析发现,在吸附过程中除了静电吸附(EA)外,还发生了还原吸附(RA),其中U(VI)被还原为U(IV), Ti(II)被氧化为Ti(IV)。计算U(VI)在Ti3C2Tx官能团(F, O, OH)上的吸附能和电子定位函数(ELF)表明,OH官能团最有利于吸附U(VI),从理论上揭示了EA&;RA的吸附机理。此外,在模拟海水环境下,Ti3C2(OH)0.08@SA气凝胶即使在超低浓度3.3 μg/L U(VI)下也能有效吸附U(VI)。MXene基气凝胶具有吸附性能好、易于回收、可重复使用等优点,有利于今后作为U(VI)吸附剂的实际应用。
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引用次数: 0
Porous carbon foams prepared by CaCl2 molten salt assisted carbonization for supercapacitors CaCl2熔盐辅助炭化法制备超级电容器用多孔泡沫炭
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139683
Min Ru , Boan Wu , Wei Zhao , Bing Yan , Tao Wang , Haoyi Sun , Bin He , Zengkai Ji , Zhenlu Liu , Wujie Ge , Shuijian He , Qian Zhang
Porous carbon materials are widely used as electrode materials for supercapacitors due to their tunable structure and stability. Here, using sodium carboxymethyl cellulose (CMC-Na) as the carbon precursor, porous carbon foams with intrinsic oxygen were successfully constructed through a one-step calcium chloride (CaCl2) molten salt system assisted carbonization and activation strategy. During this process, the oxygen in CMC-Na is partially retained in situ while CaCl2 not only acts as an activator to promote mesoporous structure development but also guides the formation of stable hierarchical pore structure through ion exchange effect. The optimal sample (C-5–900) exhibits an oxygen content of 4.6 at% and a specific surface area of 722 m2 g−1, demonstrating effective in situ oxygen retention and porous architecture. In a three-electrode system, this material achieved a specific capacitance of 172 F g−1 at a current density of 0.1 A g−1 in 6 M KOH electrolyte. Symmetrical supercapacitors (C-5–900//C-5–900) maintained 99.0 % and 89.5 % capacitance retention after 20,000 and 60,000 cycles at a high current of 30 A g−1, demonstrating outstanding electrochemical stability. Notably, the device capacitance performance further improved with KI addition in electrolyte. This work provides a valuable synthetic pathway and performance reference for the controllable preparation of porous carbon materials and their application in high-efficiency energy storage devices.
多孔碳材料因其结构可调、稳定性好而被广泛用作超级电容器的电极材料。本研究以羧甲基纤维素钠(CMC-Na)为碳前驱体,通过一步氯化钙(CaCl2)熔盐体系辅助碳化活化策略,成功构建了含内氧多孔泡沫碳。在此过程中,CMC-Na中的氧被部分保留在原位,而CaCl2不仅作为活化剂促进介孔结构的发育,还通过离子交换作用引导稳定的分层孔结构的形成。最佳样品(C-5-900)的氧含量为4.6 at%,比表面积为722 m2 g−1,表现出有效的原位保氧和多孔结构。在三电极系统中,该材料在电流密度为0.1 a g−1时,在6 M KOH电解质中获得了172 F g−1的比电容。对称型超级电容器(C-5-900 // C-5-900)在30 a g−1的大电流下,经过2万次和6万次循环,电容保持率分别为99.0 %和89.5 %,表现出优异的电化学稳定性。值得注意的是,在电解液中加入KI后,器件的电容性能进一步提高。本工作为多孔碳材料的可控制备及其在高效储能器件中的应用提供了有价值的合成途径和性能参考。
{"title":"Porous carbon foams prepared by CaCl2 molten salt assisted carbonization for supercapacitors","authors":"Min Ru ,&nbsp;Boan Wu ,&nbsp;Wei Zhao ,&nbsp;Bing Yan ,&nbsp;Tao Wang ,&nbsp;Haoyi Sun ,&nbsp;Bin He ,&nbsp;Zengkai Ji ,&nbsp;Zhenlu Liu ,&nbsp;Wujie Ge ,&nbsp;Shuijian He ,&nbsp;Qian Zhang","doi":"10.1016/j.colsurfa.2026.139683","DOIUrl":"10.1016/j.colsurfa.2026.139683","url":null,"abstract":"<div><div>Porous carbon materials are widely used as electrode materials for supercapacitors due to their tunable structure and stability. Here, using sodium carboxymethyl cellulose (CMC-Na) as the carbon precursor, porous carbon foams with intrinsic oxygen were successfully constructed through a one-step calcium chloride (CaCl<sub>2</sub>) molten salt system assisted carbonization and activation strategy. During this process, the oxygen in CMC-Na is partially retained <em>in situ</em> while CaCl<sub>2</sub> not only acts as an activator to promote mesoporous structure development but also guides the formation of stable hierarchical pore structure through ion exchange effect. The optimal sample (C-5–900) exhibits an oxygen content of 4.6 at% and a specific surface area of 722 m<sup>2</sup> g<sup>−1</sup>, demonstrating effective <em>in situ</em> oxygen retention and porous architecture. In a three-electrode system, this material achieved a specific capacitance of 172 F g<sup>−1</sup> at a current density of 0.1 A g<sup>−1</sup> in 6 M KOH electrolyte. Symmetrical supercapacitors (C-5–900//C-5–900) maintained 99.0 % and 89.5 % capacitance retention after 20,000 and 60,000 cycles at a high current of 30 A g<sup>−1</sup>, demonstrating outstanding electrochemical stability. Notably, the device capacitance performance further improved with KI addition in electrolyte. This work provides a valuable synthetic pathway and performance reference for the controllable preparation of porous carbon materials and their application in high-efficiency energy storage devices.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"736 ","pages":"Article 139683"},"PeriodicalIF":5.4,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146036390","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
Ti3C2Tx/NF@Lys hybrid nanomaterials for photothermal-catalytic synergistic antibacterial application Ti3C2Tx/NF@Lys杂化纳米材料光热催化协同抗菌应用
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139647
Nan Zhang , Yi Li , Zhengcai Guo , Lianyuan Ge , Simin Yuan , Qiang Wu , Heyu He , Wanjun Hao , Xiaohong Wang
The escalating crisis of bacterial resistance presents a formidable challenge, necessitating the urgent development of innovative antibacterial strategies to counteract this growing threat. Nevertheless, the suboptimal production efficiency of reactive oxygen species (ROS) and the inadequate catalytic activity of single-component nanozymes continue to significantly constrain the advancement of effective therapeutic strategies. This work constructed a multifunctional nano-antibacterial platform composed of Ti3C2Tx MXene, nickel-iron bimetallic composite (NF), and lysozyme (Lys). Under near-infrared laser (NIR) irradiation, the Ti3C2Tx undergoes significant high-temperature generation via the photothermal effect, causing thermal damage to bacteria. Concurrently, NF exhibits enhanced peroxidase-like activity, accelerating H2O2 decomposition through a peroxidase-like reaction, and generating cytotoxic hydroxyl radicals (·OH) to achieve chemodynamic therapy (CDT). Additionally, NIR excited Ti3C2Tx also generate Singlet oxygen (1O2), inducing photodynamic antibacterial (PDT) effects. Notably, the intense thermal effect greatly enhances the activity of Lys, facilitating ROS attacks on bacteria. Compared with single mode systems, the tri-modal synergistic system achieves a nearly 99.9 % inactivation rate against both methicillin-resistant Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) within 5 min, demonstrating superior antibacterial performance through its triple-strategy approach. By rationally integrating enzyme-like catalysis, light-responsive materials and bioactive components, this study provides a promising antibiotic-free new paradigm for combating multidrug-resistant pathogens.
不断升级的细菌耐药性危机提出了一个巨大的挑战,迫切需要开发创新的抗菌策略来应对这一日益增长的威胁。然而,活性氧(ROS)的次优生产效率和单组分纳米酶的催化活性不足继续极大地限制了有效治疗策略的进展。本工作构建了由Ti3C2Tx MXene、镍铁双金属复合材料(NF)和溶菌酶(Lys)组成的多功能纳米抗菌平台。在近红外激光(NIR)照射下,Ti3C2Tx通过光热效应产生明显的高温,对细菌产生热损伤。同时,NF表现出增强的过氧化物酶样活性,通过过氧化物酶样反应加速H2O2分解,并产生细胞毒性羟基自由基(·OH),从而实现化学动力学治疗(CDT)。此外,近红外激发Ti3C2Tx还产生单重态氧(1O2),诱导光动力抗菌(PDT)效应。值得注意的是,强烈的热效应大大增强了Lys的活性,促进了ROS对细菌的攻击。与单模系统相比,三模协同系统在5 min内对耐甲氧西林的大肠杆菌(E. coli)和金黄色葡萄球菌(S. aureus)均达到近99.9 %的失活率,通过其三重策略的方式显示出卓越的抗菌性能。通过合理整合酶样催化、光响应材料和生物活性成分,本研究为对抗多药耐药病原体提供了一种有前景的无抗生素新范式。
{"title":"Ti3C2Tx/NF@Lys hybrid nanomaterials for photothermal-catalytic synergistic antibacterial application","authors":"Nan Zhang ,&nbsp;Yi Li ,&nbsp;Zhengcai Guo ,&nbsp;Lianyuan Ge ,&nbsp;Simin Yuan ,&nbsp;Qiang Wu ,&nbsp;Heyu He ,&nbsp;Wanjun Hao ,&nbsp;Xiaohong Wang","doi":"10.1016/j.colsurfa.2026.139647","DOIUrl":"10.1016/j.colsurfa.2026.139647","url":null,"abstract":"<div><div>The escalating crisis of bacterial resistance presents a formidable challenge, necessitating the urgent development of innovative antibacterial strategies to counteract this growing threat. Nevertheless, the suboptimal production efficiency of reactive oxygen species (ROS) and the inadequate catalytic activity of single-component nanozymes continue to significantly constrain the advancement of effective therapeutic strategies. This work constructed a multifunctional nano-antibacterial platform composed of Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> MXene, nickel-iron bimetallic composite (NF), and lysozyme (Lys). Under near-infrared laser (NIR) irradiation, the Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> undergoes significant high-temperature generation via the photothermal effect, causing thermal damage to bacteria. Concurrently, NF exhibits enhanced peroxidase-like activity, accelerating H<sub>2</sub>O<sub>2</sub> decomposition through a peroxidase-like reaction, and generating cytotoxic hydroxyl radicals (·OH) to achieve chemodynamic therapy (CDT). Additionally, NIR excited Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> also generate Singlet oxygen (<sup>1</sup>O<sub>2</sub>), inducing photodynamic antibacterial (PDT) effects. Notably, the intense thermal effect greatly enhances the activity of Lys, facilitating ROS attacks on bacteria. Compared with single mode systems, the tri-modal synergistic system achieves a nearly 99.9 % inactivation rate against both methicillin-resistant <em>Escherichia coli</em> (<em>E. coli</em>) and <em>Staphylococcus aureus</em> (<em>S. aureus</em>) within 5 min, demonstrating superior antibacterial performance through its triple-strategy approach. By rationally integrating enzyme-like catalysis, light-responsive materials and bioactive components, this study provides a promising antibiotic-free new paradigm for combating multidrug-resistant pathogens.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"737 ","pages":"Article 139647"},"PeriodicalIF":5.4,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146076403","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
Tetraaniline-functionalized UiO-66 enabling synergistic pH-triggered inhibitor release and enhanced redox-mediated passivation for corrosion protective coatings 四苯胺功能化的UiO-66能够协同ph触发的抑制剂释放和增强氧化还原介导的防腐涂层钝化
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139607
Chen Wang , Yinzheng Xia , Yue Li , Qianhong Shen , Hui Yang
This work presents the design of UiO-66-PDA@TANI, a novel MOF-oligomer nanocomposite that synergistically integrates pH-triggered inhibitor release with redox-mediated passivation to enhance epoxy coating protection. Release studies revealed a 13-fold increase in alkaline-activated Zr4 + /ligand release, while cyclic voltammetry and electron paramagnetic resonance analyses confirmed that heterogenous integration of UiO-66 improves the electron transfer efficiency of TANI. Potentiodynamic polarization tests demonstrated that UiO-66-PDA@TANI achieved a corrosion inhibition efficiency of 75.62 % in saline solution within 24 h. Long-term EIS measurements showed superior barrier properties, with the composite epoxy coating exhibiting |Z|0.01 Hz = 1.85 × 1010 Ω·cm2 after 60 d of immersion, compared to 5.51 × 107 Ω·cm2 for pure epoxy. Artificial defect experiments further revealed self-healing behavior, with an improvement efficiency of 229.67 % after 48 h, indicating localized protection beyond that of pristine coatings. These findings demonstrate that the synergistic interplay between UiO-66 and TANI enables dual protection: rapid inhibitor delivery at corrosion sites via pH-induced framework disintegration and regeneration of passivation films via enhanced TANI redox cycling for long-term durability. This work introduces a previously unreported strategy that leverages UiO-66 for electron conduction-enhanced corrosion protection, offering fundamental design principles for pH/redox dual-responsive protective systems.
这项工作提出了UiO-66-PDA@TANI的设计,这是一种新型的mof低聚物纳米复合材料,它协同集成了ph触发的抑制剂释放和氧化还原介导的钝化,以增强环氧涂层的保护。释放研究表明,碱活化Zr4 + /配体释放量增加了13倍,而循环伏安法和电子顺磁共振分析证实,UiO-66的异质整合提高了TANI的电子传递效率。动电位极化试验表明,UiO-66-PDA@TANI在24 h内的缓蚀效率为75.62 %。长期的EIS测试显示出优异的阻隔性能,在浸泡60 d后,复合环氧涂层的|Z|0.01 Hz = 1.85 × 1010 Ω·cm2,而纯环氧涂层的|Z|0.01 Hz = 5.51 × 107 Ω·cm2。人工缺陷实验进一步揭示了涂层的自修复行为,48 h后涂层的自修复效率为229.67 %,表明涂层的局部保护能力超过了原始涂层。这些发现表明,UiO-66和TANI之间的协同作用可以实现双重保护:通过ph诱导的框架分解在腐蚀部位快速释放抑制剂,通过增强TANI氧化还原循环再生钝化膜,从而获得长期耐用性。这项工作介绍了一种以前未报道的策略,该策略利用UiO-66进行电子传导增强腐蚀保护,为pH/氧化还原双响应保护系统提供了基本设计原则。
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引用次数: 0
Gravity-driven silver nanocatalytic membranes for continuous water treatment 用于连续水处理的重力驱动银纳米催化膜
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-22 DOI: 10.1016/j.colsurfa.2026.139690
Yan Wang , Jingyu Lu , Shuang Guo , Shuai Wang , Jingjing Pan , Yinghua Wu , Haifang Hu , Chuanjie Fang , Liping Zhu
The removal of refractory organic pollutants from water sources poses a critical challenge for environmental protection. Catalytic membranes that integrate separation and degradation functionalities have emerged as a promising strategy. However, their practical implementation has been hampered by inadequate catalyst stability and complex fabrication processes. In this study, we report a facile strategy to fabricate a robust Ag-based catalytic membrane (Ag-PDA-M0) via the in situ growth of Ag nanoparticles on a polydopamine (PDA)-modified nylon substrate. The PDA interlayer provides abundant anchoring sites for Ag nanoparticles, enabling the formation of a dense and uniform catalytic layer throughout the membrane matrix. Under gravity-driven filtration conditions, the membrane demonstrated exceptional performance with 99 % removal efficiency for methylene blue without requiring additional catalyst recovery steps. Notably, it maintained 92 % of its initial catalytic activity after eight consecutive operation cycles, demonstrating remarkable stability under continuous-flow conditions. Comprehensive characterization confirmed that the enhanced performance originated from the synergistic combination of high catalyst loading, optimized mass transfer, and strong metal-support interaction provided by the PDA modification. This work presents a practical and scalable approach for designing high-performance catalytic membranes, offering new insights into the development of energy-efficient water treatment technologies for sustainable pollutant removal.
从水源中去除难降解有机污染物是环境保护的一个重要挑战。集分离和降解功能于一体的催化膜已成为一种很有前途的策略。然而,它们的实际应用受到催化剂稳定性不足和制造工艺复杂的阻碍。在这项研究中,我们报告了一种简单的策略,通过在聚多巴胺(PDA)修饰的尼龙衬底上原位生长银纳米粒子来制备坚固的银基催化膜(Ag-PDA- m0)。PDA中间层为银纳米粒子提供了丰富的锚定位点,使其能够在整个膜基质中形成致密而均匀的催化层。在重力驱动过滤条件下,该膜表现出优异的性能,去除亚甲基蓝的效率达到99% %,无需额外的催化剂回收步骤。值得注意的是,在连续8个操作循环后,它保持了92% %的初始催化活性,在连续流动条件下表现出显著的稳定性。综合表征证实,性能的增强源于高催化剂负载、优化的传质以及PDA改性所提供的强金属-载体相互作用的协同结合。这项工作为设计高性能催化膜提供了一种实用且可扩展的方法,为可持续去除污染物的节能水处理技术的发展提供了新的见解。
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引用次数: 0
Protonation-driven interfacial behavior and foam stability in mixed cationic–nonionic surfactant systems 阳离子-非离子表面活性剂混合体系中质子驱动的界面行为和泡沫稳定性
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139666
Feng Yang, Liang Cao, Yongjun Peng
Understanding how mixed ionic–nonionic surfactant systems control foam stability is critical for designing tailored interfacial systems in industrial and scientific applications. Here, we investigate the molecular mechanisms by which the cationic surfactant dodecylamine (DDA) and the nonionic surfactant methyl isobutyl carbinol (MIBC) regulate foam formation and stability. Using a multiscale approach combining macroscopic foam analysis (Dynamic Foam Analysis, DFA; Focused Beam Reflectance Measurement, FBRM), interfacial characterization (surface tension, zeta potential), and molecular-scale techniques (1H Nuclear Magnetic Resonance,1H NMR and Small-Angle X-ray Scattering, SAXS), we link protonation-dependent behavior of DDA to interfacial adsorption, aggregation, and foam-stabilizing properties. At low DDA concentrations, protonated DDA (DDAH+) forms uniform, positively charged interfacial layers, which synergize with MIBC to enhance interfacial packing and stabilize foam through combined electrostatic and hydration effects. At higher DDA concentrations, the increased fraction of neutral DDA disrupts interfacial charge uniformity and hydration layers, while MIBC promotes adsorption of unprotonated DDA, accelerating bubble coalescence and reducing foam stability. This integrated mechanistic study reveals how ionic surfactant protonation and co-adsorption with nonionic surfactants govern foam behavior, providing a framework for the rational design of mixed surfactant systems with controlled foam properties.
了解混合离子-非离子表面活性剂系统如何控制泡沫稳定性对于设计工业和科学应用中定制的界面系统至关重要。本文研究了阳离子表面活性剂十二烷基胺(DDA)和非离子表面活性剂甲基异丁基甲醇(MIBC)调控泡沫形成和稳定性的分子机制。使用多尺度方法结合宏观泡沫分析(动态泡沫分析,DFA;聚焦束反射测量,FBRM),界面表征(表面张力,zeta电位)和分子尺度技术(1H核磁共振,1H NMR和小角度x射线散射,SAXS),我们将DDA的质子依赖行为与界面吸附,聚集和泡沫稳定特性联系起来。在低DDA浓度下,质子化的DDA (DDAH+)形成均匀的、带正电的界面层,与MIBC协同作用,通过静电和水合作用增强界面填充,稳定泡沫。在较高的DDA浓度下,中性DDA比例的增加破坏了界面电荷均匀性和水化层,而MIBC促进了未质子化DDA的吸附,加速了气泡的聚并,降低了泡沫的稳定性。这项综合机理研究揭示了离子表面活性剂的质子化和与非离子表面活性剂的共吸附如何影响泡沫行为,为合理设计具有可控泡沫性能的混合表面活性剂体系提供了框架。
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引用次数: 0
An investigation on the synergistic effect of hydroxyl and oxime groups in oxime collectors and their application in malachite flotation 肟基捕收剂中羟基与肟基的协同作用及其在孔雀石浮选中的应用研究
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.colsurfa.2026.139684
Ruyi Zhang , Sheng Liu , Fangxu Li
This study investigated the structure-performance relationships of p-tert-butylsalicylaldoxime (TBSO), p-tert-butylbenzaldehyde oxime (TBBAO), and benzohydroxamic acid (BHA) to guide oxime collector design. Density functional theory (DFT) calculations revealed that TBSO and BHA owned narrower HOMO-LUMO energy gaps than TBBAO, indicating higher chemical reactivity. Adsorption and zeta potential measurements confirmed that TBSO and BHA adsorb more strongly on malachite and induce larger zeta potential shifts than TBBAO. Log P values followed the order: TBBAO (3.87) > TBSO (3.48) > BHA (1.11). However, contact angle results revealed a different trend in hydrophobicity: TBSO > BHA > TBBAO. Although BHA owned strongest affinity to malachite, the contact angle of BHA-treated malachite was not the highest, indicating that the hydrophobicity of mineral after collector treatment was related with the collector’s affinity and hydrophobization ability. Flotation results of artificially mixed mineral revealed that TBSO exhibited better flotation performance to separate malachite and calcite than BHA and TBBAO, it recovered 97.26 % malachite and 6.24 % calcite with the difference in flotation recovery of 91.02 %. The superior flotation performance of TBSO was assigned to its strong adsorption on malachite by the hydroxyl and oxime groups with the formation of Cu-O and Cu-N bonds and its hydrophobic structure.
本研究考察了对叔丁基水杨醛肟(TBSO)、对叔丁基苯甲醛肟(TBBAO)和苯甲羟肟酸(BHA)的结构性能关系,以指导肟捕收剂的设计。密度泛函理论(DFT)计算表明,TBSO和BHA的HOMO-LUMO能隙比TBBAO更窄,表明其化学反应活性更高。吸附和zeta电位测量证实,TBSO和BHA对孔雀石的吸附比TBBAO更强,并引起更大的zeta电位位移。Log P值依次为:TBBAO (3.87) >; TBSO (3.48) >; BHA(1.11)。然而,接触角结果显示了不同的疏水性趋势:TBSO >; BHA >; TBBAO。虽然BHA对孔雀石的亲和性最强,但经BHA处理的孔雀石的接触角并不是最高的,说明捕收剂处理后矿物的疏水性与捕收剂的亲和性和疏水能力有关。人工混合矿物浮选结果表明,TBSO对孔雀石和方解石的分离效果优于BHA和TBBAO,孔雀石和方解石的回收率分别为97.26 %和6.24 %,两者浮选回收率相差91.02 %。TBSO具有优异的浮选性能,主要是由于其羟基和肟基在孔雀石上具有很强的吸附作用,形成Cu-O和Cu-N键,并具有疏水结构。
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Colloids and Surfaces A: Physicochemical and Engineering Aspects
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