Journal of Colloid and Interface Science最新文献_第9页

Piezoelectric-mediated two-dimensional copper-based metal–organic framework for synergistic sonodynamic and cuproptosis-driven tumor therapy 压电介导的二维铜基金属有机框架，用于协同声动力和杯突症驱动的肿瘤治疗。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-20 DOI: 10.1016/j.jcis.2024.10.108

Sonodynamic therapy (SDT) is a minimally invasive therapeutic approach that utilizes sonosensitizers to catalyze substrates and generate reactive oxygen species (ROS) under ultrasound stimulation, ultimately inducing tumor cell death. Enhancing the piezoelectric properties of nanomaterials and modulating the semiconductor energy band are effective strategies to improve the catalytic efficiency of sonosensitizers. In this study, we developed a two-dimensional (2D) copper-based piezoelectric metal–organic framework (MOF) sonosensitizer, denoted as CM, through the coordination of copper and dimethylimidazole. The unique 2D MOF structure imparts CM with piezoelectric characteristics, enabling it to enhance SDT efficacy by modulating the semiconductor bandgap and carrier mobility. Upon ultrasound irradiation, CM catalyzes oxygen to undergo a cascade reaction, producing highly toxic singlet oxygen. Additionally, cupric ions in CM can be reduced by glutathione, facilitating the spontaneous catalysis of hydrogen peroxide in tumors to generate hydroxyl radicals and deplete glutathione, thereby inducing oxidative damage. Moreover, cupric ions in CM can trigger tumor cell cuproptosis, which, in combination with the generated ROS, accelerates cell death. Thus, this study establishes a MOF-based system for controllably inducing multi-pathway cancer cell death and provides a foundation for enhancing ultrasound-catalyzed tumor therapy through the optimization of piezoelectric properties.

声动力疗法（SDT）是一种微创治疗方法，它利用声敏化剂在超声刺激下催化底物并产生活性氧（ROS），最终诱导肿瘤细胞死亡。增强纳米材料的压电特性和调节半导体能带是提高声纳敏化剂催化效率的有效策略。在这项研究中，我们通过铜和二甲基咪唑的配位，开发出了一种二维（2D）铜基压电金属有机框架（MOF）声纳敏化剂，简称 CM。独特的二维 MOF 结构赋予了 CM 压电特性，使其能够通过调节半导体带隙和载流子迁移率来提高 SDT 的功效。在超声波照射下，CM 会催化氧气发生级联反应，产生剧毒的单线态氧。此外，CM 中的铜离子可被谷胱甘肽还原，促进肿瘤中的过氧化氢自发催化生成羟自由基并消耗谷胱甘肽，从而诱发氧化损伤。此外，CM 中的铜离子可诱发肿瘤细胞的杯突症，与产生的 ROS 结合，加速细胞死亡。因此，这项研究建立了一个基于 MOF 的系统，可控地诱导多途径的癌细胞死亡，并为通过优化压电特性加强超声催化肿瘤治疗奠定了基础。

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引用次数: 0

Visualizing dynamic alterations of vitreous viscosity during elevated intraocular pressure in glaucoma with a Near-infrared/Magnetic resonance imaging dual-modal nanoprobe 用近红外/磁共振成像双模式纳米探针观察青光眼眼压升高时玻璃体粘度的动态变化。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-20 DOI: 10.1016/j.jcis.2024.10.110

Glaucoma is a chronic progressive disease leading to irreversible visual impairment and blindness. High intraocular pressure (IOP) resulting from abnormally high outflow resistance is a major risk factor for glaucoma development, however, it is unclear how IOP elevation influences the structure and function of the retina and the optic nerve via vitreous humor located between the lens and retina in the eye. To understand vitreous biomechanical and stimulus response toward IOP elevation, we developed a novel near-infrared (NIR)/MRI dual-modal nanoprobe, DTA/P-NCA/17F@Co, which is composed of N, N-dimethyl-4(thien-2-yl)-aniline group (DTA) as NIR fluorophore and the fluorine-based polyamino acid cobalt nanoparticles (P-NCA/17F@Co) as T₂ contrast agent. These nanoprobes exhibit good biocompatibility, low surface energy characteristics, and viscosity-responsive NIR emission and T₂ relaxation values. The intrinsic viscosity-sensitive mechanism of nanoprobes was ascribed to constrained molecular motion in high-viscosity vitreous chamber, which causes enhanced fluorescence emission and shortened T₂ relaxation times. By using its ability for dual-modal visualization of viscosity, we achieved non-invasive in vivo monitoring the changes in vitreous viscosity during elevated IOP in a glaucoma rat model. In vivo experiments validated that vitreous viscosity is very strongly correlated with IOP elevation induced by glaucoma, much earlier than structural and functional change in the retina. Our findings revealed that IOP elevation induced the increase of vitreous viscosity, indicating that monitoring vitreous viscosity is key to the glaucoma model. This study not only provides versatile nanoprobes for dual-modal visualization of biomechanical properties of the vitreous humor in its native environment, but also shows great potential in the early diagnosis of glaucoma.

青光眼是一种慢性进展性疾病，会导致不可逆转的视力损伤和失明。异常高的流出阻力导致的高眼压是青光眼发病的主要风险因素，然而，目前还不清楚眼压升高如何通过位于眼球晶状体和视网膜之间的玻璃体影响视网膜和视神经的结构和功能。为了了解玻璃体对眼压升高的生物力学和刺激反应，我们开发了一种新型近红外（NIR）/MRI双模态纳米探针--DTA/P-NCA/17F@Co，它由作为近红外荧光团的N, N-二甲基-4（噻吩-2-基）苯胺基团（DTA）和作为T2对比剂的氟基多胺基酸钴纳米颗粒（P-NCA/17F@Co）组成。这些纳米探针具有良好的生物相容性、低表面能特性、粘度响应型近红外发射值和 T2 弛豫值。纳米探针固有的粘度敏感机制被归因于分子在高粘度玻璃体内的受限运动，这导致了荧光发射的增强和 T2 驰豫时间的缩短。通过利用其粘度双模态可视化能力，我们在青光眼大鼠模型中实现了对眼压升高时玻璃体粘度变化的无创体内监测。体内实验验证了玻璃体粘度与青光眼引起的眼压升高密切相关，比视网膜的结构和功能变化要早得多。我们的研究结果表明，眼压升高会诱发玻璃体粘度增加，这表明监测玻璃体粘度是青光眼模型的关键。这项研究不仅为玻璃体在原生环境中的生物力学特性的双模式可视化提供了多功能纳米探针，而且在青光眼的早期诊断方面也显示出巨大的潜力。

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引用次数: 0

A high temperature-resistant, strong, and self-healing double-network hydrogel for profile control in oil recovery 用于采油过程中剖面控制的耐高温、高强度和自愈合双网水凝胶

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.077

Hydrogels are widely used in profile control to plug high-permeability zones in oil recovery. In this study, a novel double-network (DN) hydrogel is developed for profile control. The two networks of the prepared hydrogel are polyacrylamide (PAAm) crosslinked by N,N’-Methylenebisacrylamide (MBAA) and konjac glucomannan (KGM) crosslinked by borax (B), respectively. The two networks are interconnected by their interpenetrating structures and hydrogen bonds. Based on the results of a series of evaluation experiments, the AAm/KGM DN hydrogels developed in this study exhibit a strong mechanical strength with their fracture stresses exceeding 0.137 MPa. Meanwhile, the AAm/KGM DN hydrogels can remain thermally stable after being heated at 130 °C for 24 h, indicating the good high-temperature resistance of the new sample. Moreover, the prepared AAm/KGM DN hydrogels present excellent self-healing performance due to the abundant hydrogen bonds in their structures, which helps form stable and long-term plugging in porous media. In addition, the pure PAAm hydrogel and the AAm/KGM DN hydrogel are sheared into two dispersed particle gel (DPG) suspensions to investigate their plugging performances. The results demonstrate that the AAm/KGM DN DPG can effectively plug a high-permeability sandpack with a plugging efficiency of 93.2 %, while the pure AAm DPG can only provide a much lower plugging efficiency of 60.5 %. The AAm/KGM DN hydrogel developed in this study, with its high mechanical strength, high-temperature resistance, and self-healing capability, offers a promising new candidate for profile control in oil recovery.

水凝胶被广泛用于剖面控制，以堵塞采油过程中的高渗透区。本研究开发了一种用于剖面控制的新型双网络（DN）水凝胶。所制备水凝胶的两个网络分别是由 N,N'-亚甲基双丙烯酰胺（MBAA）交联的聚丙烯酰胺（PAAm）和由硼砂（B）交联的魔芋葡甘露聚糖（KGM）。这两种网络通过相互渗透结构和氢键相互连接。根据一系列评估实验的结果，本研究开发的 AAm/KGM DN 水凝胶具有很强的机械强度，其断裂应力超过 0.137 兆帕。同时，AAm/KGM DN 水凝胶在 130 °C 下加热 24 小时后仍能保持热稳定性，表明新样品具有良好的耐高温性能。此外，所制备的 AAm/KGM DN 水凝胶因其结构中含有大量氢键而具有优异的自愈合性能，有助于在多孔介质中形成长期稳定的堵塞。此外，还将纯 PAAm 水凝胶和 AAm/KGM DN 水凝胶剪切成两种分散颗粒凝胶（DPG）悬浮液，研究它们的堵塞性能。结果表明，AAm/KGM DN DPG 能有效堵塞高渗透性砂层，堵塞效率高达 93.2%，而纯 AAm DPG 的堵塞效率则低得多，只有 60.5%。本研究开发的 AAm/KGM DN 水凝胶具有较高的机械强度、耐高温性和自愈合能力，为采油过程中的剖面控制提供了一种前景广阔的新候选材料。

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引用次数: 0

Wetting and emulsification properties of cellulose nanocrystals modified with tannic acid and alkyl cellulose derivatives 用单宁酸和烷基纤维素衍生物改性的纤维素纳米晶体的润湿性和乳化性

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.080

Hypothesis

Cellulose nanocrystals (CNCs) are sustainable rod-like nanoparticles that can be used to stabilize oil-in-water emulsions and can create hydrophilic coatings. Modifying the surface of CNCs can improve emulsion properties and allow for adjustable wettability.

Experiments

This study explores the improvement of Pickering emulsion properties for various oils and the adjustability of coated surfaces through the physical modification of CNCs, without chemical functionalization. Bio-based additives, including antioxidant tannic acid (TA), methyl cellulose (MC), and ethyl cellulose (EC) were used as surface modifiers. The identification of optimal formulations involved varying the weight fraction of the alkyl cellulose derivatives.

Findings

The findings suggest that, akin to pure CNCs, Pickering emulsions stabilized by TA and/or MC-modified CNCs demonstrate comparably high stability. The introduction of MC at a low weight fraction enhances hydrophilicity, and AFM analysis reveals smooth surfaces, mitigating the potential influence of roughness. In contrast, EC-modified CNCs result in less stable emulsions but exhibit more hydrophobic surfaces. This translates to a broad spectrum of characteristics, ranging from quasi-superhydrophilic to nearly hydrophobic (with contact angles spanning from below 11° up to 68°), all controllable through a straightforward physical coating process. This facile preparation of coated CNCs provides a versatile approach to customizing the wetting and emulsification properties of nanomaterials.

假设纤维素纳米晶体（CNCs）是一种可持续的棒状纳米粒子，可用于稳定水包油型乳液，并可形成亲水性涂层。本研究探讨了在不进行化学功能化的情况下，通过物理改性 CNCs 来改善各种油类的皮克林乳液特性以及涂层表面的可调节性。生物基添加剂，包括抗氧化剂单宁酸（TA）、甲基纤维素（MC）和乙基纤维素（EC）被用作表面改性剂。研究结果表明，与纯氯化萘类似，由 TA 和/或 MC 改性氯化萘稳定的皮克林乳液也具有相当高的稳定性。以较低重量分数引入 MC 可增强亲水性，原子力显微镜分析显示表面光滑，减轻了粗糙度的潜在影响。相比之下，EC 改性 CNC 产生的乳液稳定性较差，但表面更疏水。这就体现了从准超亲水性到近疏水性（接触角从 11°以下到 68°）的广泛特性，所有这些都可以通过简单的物理涂层工艺进行控制。这种简便的涂层 CNC 制备方法为定制纳米材料的润湿和乳化特性提供了一种通用方法。

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引用次数: 0

Boosting electrochemical ammonia synthesis via dynamic nitrogen carriers coupled with electron-rich Lewis acidic sites on TiO2−x nanofiber 通过 TiO2-x 纳米纤维上的动态氮载体和富含电子的路易斯酸位点促进电化学氨合成。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.093

In light of the high energy consumption and substantial carbon emissions associated with traditional NH₃ production based on the Haber–Bosch process, the aqueous electrochemical nitrogen reduction reaction (NRR) offers a clean and sustainable alternative production route. Nevertheless, activating the NN bonds at room temperature is challenging due to the high bond energy, severely hindering the development and commercialization of the electrochemical NRR. Herein, we report a synergistic strategy for achieving efficient N₂ activation at ambient conditions that combines electrolyte engineering with catalytic site-modulated TiO_2−x nanofiber electrocatalysts. The synthesized TiO_2−x nanofiber electrocatalysts contained abundant intrinsic oxygen vacancies and were further modified with hydroxyl groups to create electron-rich Lewis acidic Ti sites. Additionally, BF₃ was engineered into the electrolyte microenvironment, and it could form adducts with N₂, serving as a dynamic carrier for N₂ transport. The electron-rich Lewis acidic sites and the dynamic carriers exerted a ‘pull–pull’ effect on N₂, thereby weakening the NN bonds. Through electrochemical performance evaluation, the designed electrocatalytic scheme achieved an NH₃ yield of ∼57.15 μg h⁻¹ mg⁻¹ and a Faradaic efficiency of ∼15.14 %. We anticipate that this methodology will provide new insights into the development of electrochemical ammonia synthesis, particularly in relation to multifaceted design.

鉴于基于哈伯-博什工艺的传统 NH3 生产过程能耗高、碳排放量大，水基电化学氮还原反应（NRR）提供了一条清洁、可持续的替代生产路线。然而，由于键能较高，在室温下激活氮还原键具有挑战性，严重阻碍了电化学氮还原反应的开发和商业化。在此，我们报告了一种在常温条件下实现高效 N2 活化的协同策略，该策略将电解质工程与催化位点调制 TiO2-x 纳米纤维电催化剂相结合。合成的 TiO2-x 纳米纤维电催化剂含有丰富的固有氧空位，并用羟基进一步修饰以形成富电子路易斯酸钛位点。此外，还在电解质微环境中加入了 BF3，它可以与 N2 形成加合物，成为 N2 运输的动态载体。富电子的路易斯酸性位点和动态载体对 N2 产生了 "拉-拉 "效应，从而削弱了 NN 键。通过电化学性能评估，所设计的电催化方案实现了 ∼57.15 μg h-1 mg-1 的 NH3 产量和 ∼15.14 % 的法拉第效率。我们预计该方法将为电化学氨合成的发展提供新的见解，特别是在多方面设计方面。

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引用次数: 0

Reversible silicon anodes enabled by fluorinated inorganic-organic hybrid coating 氟化无机-有机混合涂层实现可逆硅阳极

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.104

Silicon anodes deliver batteries with energy densities much higher than those based on today’s dominant graphite anodes. However, they commonly exhibit huge volume variations and unfavorable interface stability, causing a gradually diminishing capacity on extended cycling. Most Si-based batteries consisting Si/C composites in industry can only use a very limited amount of Si (<30 % by weight). Exploiting molecular layer deposition (MLD) technique, a fluorine-rich flexible inorganic–organic hybrid alucone (AlFHQ) shell is controllably deposited onto Si electrodes. Employing ex situ XPS and AFM, the AlFHQ film presents reversible electrochemical evolutions in terms of composition and morphology. The interactions the between Li⁺ and −O−2,3,5,6-fluorobenzene functional groups help to construct a mechanically-chemically robust LiF-rich hybrid solid electrolyte interphase (SEI) on Si anode, delivering enhanced interfacial stability and integrity of electrode. An optimized coating thickness (≈5 nm) for interfacial stabilization and Li⁺ transport kinetics is demonstrated, namely, Si@AlFHQ-20. The reported fluorine-rich hybrid modification technique endows (a), stable cycling of Si anode (≈3.8 mAh cm⁻²) with an ultrahigh initial Coulombic efficiency (ICE) of 92.3 %; (b), enhanced rate capability of 1468 mAh/g at 2.0 A g⁻¹ and good cycling performance; and (c), overall cell (Si@AlFHQ-20//LiCoO₂@Al₂O₃) operational stability for more than 100 cycles under stringent cathode conditions (2.68 mAh cm⁻², high cutoff voltage at 4.55 V).

硅阳极电池的能量密度远高于目前主流的石墨阳极电池。然而，硅阳极通常会表现出巨大的体积变化和不利的界面稳定性，导致电池容量在长时间循环后逐渐降低。大多数由硅/碳复合材料组成的硅基电池只能使用非常有限的硅（按重量计为 30%）。利用分子层沉积（MLD）技术，一种富含氟的柔性无机-有机杂化丙酮（AlFHQ）外壳被可控地沉积到硅电极上。利用原位 XPS 和原子力显微镜（AFM），AlFHQ 薄膜在成分和形态方面呈现出可逆的电化学演变。Li+ 与-O-2,3,5,6-氟苯官能团之间的相互作用有助于在硅阳极上构建一个机械化学性质坚固的富含 LiF 的混合固体电解质相（SEI），从而增强了界面稳定性和电极的完整性。针对界面稳定性和 Li+ 传输动力学，展示了一种优化的涂层厚度（≈5 nm），即 Si@AlFHQ-20。所报道的富氟杂化改性技术可（a）实现硅阳极（≈3.8 mAh cm-2）的稳定循环，并具有 92.3 % 的超高初始库仑效率（ICE）；（b）在 2.0 A g-1 时的 1468 mAh/g 速率能力和良好的循环性能；以及 (c)在严格的阴极条件下（2.68 mAh cm-2，4.55 V 的高截止电压），电池（Si@AlFHQ-20//LiCoO2@Al2O3）整体工作稳定性超过 100 个循环。

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引用次数: 0

The effect of emulsifier concentration on turbulent drop breakup – An experimental study based on single drop visualizations 乳化剂浓度对湍流液滴破裂的影响--基于单滴可视化的实验研究。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.078

Hypothesis

A modified Weber number can capture the effect of emulsifier concentration and the effect of external stress in turbulent drop breakup. Moreover, the effect of emulsifiers on turbulent drop breakup cannot be adequately understood from classic slow/laminar techniques and quasi steady state interfacial tension.

Experiments

Single drop breakup visualizations are used to study the effect of polysorbate 20 on turbulent drop deformation and breakup. Comparisons are made to drop tensiometry and emulsification experiments.

Findings

A high concentration of the emulsifier increases breakup probability and breakup rate and decreases breakup timescales. These effects scale with a Weber number, indicating a lowering of the effective interfacial tension to 71 % of its pure interface value. This is far less than the observed lowering of interfacial tension as measured by quiescent drop tensiometry. Mechanistically, this shows that adsorption during emulsification cannot be limited by diffusion. Studying the effect cross a range of emulsifier concentrations suggest an elastic resistance at intermediate concentrations, further helping to understand the origin of similar effects previously reported in emulsification experiments. Overall, the results show the need to study emulsifiers under turbulent conditions to understand their effects during emulsification, as opposed to the slow/laminar techniques previously used.

假设：修正的韦伯数可以捕捉乳化剂浓度的影响以及湍流液滴破裂时外部应力的影响。此外，经典的慢速/层流技术和准稳态界面张力无法充分了解乳化剂对湍流液滴破裂的影响：实验：使用单滴破裂可视化方法研究聚山梨醇酯 20 对湍流液滴变形和破裂的影响。实验：采用单滴破裂可视化方法研究聚山梨醇酯 20 对湍流液滴变形和破裂的影响，并与液滴张力测量法和乳化实验进行比较：研究结果：高浓度乳化剂会增加破裂概率和破裂率，并缩短破裂时间尺度。这些效应与韦伯数字成比例关系，表明有效界面张力降低到纯界面值的 71%。这远小于静止液滴张力测量法所观测到的界面张力降低。从机理上讲，这表明乳化过程中的吸附作用不会受到扩散的限制。对乳化剂浓度范围的影响进行研究表明，在中间浓度时会出现弹性阻力，这有助于进一步了解之前乳化实验中报告的类似影响的起源。总之，研究结果表明，有必要在湍流条件下研究乳化剂，以了解它们在乳化过程中的影响，而不是之前使用的慢速/层流技术。

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引用次数: 0

Sustainable synthesis and dual adsorption of methyl orange and cadmium ions using biogenic silica-based fibrous silica functionalized with crown ether ionic liquid 利用冠醚离子液体功能化的生物硅基纤维状二氧化硅实现甲基橙和镉离子的可持续合成与双重吸附

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.103

In pursuit of sustainable nanomaterial production, this study presents a novel biogenic fibrous silica sphere functionalized with a crown ether ionic liquid for advanced dual-adsorption of methyl orange and Cd(II) from aqueous solution. Sorghum waste serves as the silica source in the adsorbent preparation process, ensuring an eco-friendly approach. The benzo-15-crown-5 ionic liquid is coupled to thiol-functionalized fibrous silica spheres through an efficient thiol-ene click reaction. Under constant conditions (temperature: 298 K, solution volume = 50 mL, adsorbent dosage = 5 mg, pH = 7, shaking speed = 200 rpm), the synthesized material demonstrates maximum adsorption capacities of 507.1 mg g⁻¹ and 306.3 mg g⁻¹ for methyl orange and Cd(II), respectively, according to the Langmuir model. Thermodynamic investigations reveal exothermic adsorption for methyl orange with an enthalpy change of −77.49 KJ mol⁻¹, while endothermic adsorption is observed for Cd(II) with an enthalpy of +24.10 KJ mol⁻¹. The entropy change of adsorption is −0.153 KJ mol⁻¹ K⁻¹ for methyl orange, indicating a more ordered state, and + 0.192 KJ mol⁻¹ K⁻¹ for Cd(II), suggesting increased disorder. The change in Gibbs free energy ranges from −32.66 to −29.60 KJ mol⁻¹ for methyl orange and −32.29 to −35.99 KJ mol⁻¹ for Cd(II), demonstrating that both adsorption processes are spontaneous. These results indicate that the adsorbent has potential as a dual-adsorption material for water remediation applications.

为了追求可持续的纳米材料生产，本研究提出了一种新型的生物纤维状二氧化硅球，它具有冠醚离子液体的功能，可用于水溶液中甲基橙和镉(II)的高级双重吸附。高粱废料是吸附剂制备过程中的二氧化硅来源，确保了该方法的生态友好性。通过高效的硫醇-烯点击反应，苯并-15-冠醚-5 离子液体与硫醇官能化的纤维状二氧化硅球结合在一起。在恒定条件下（温度：298 K，溶液体积：50 mL，吸附剂用量：5 mg，pH 值：7，振荡速度：200 rpm），根据 Langmuir 模型，合成材料对甲基橙和镉(II)的最大吸附容量分别为 507.1 mg g-1 和 306.3 mg g-1。热力学研究表明，甲基橙的吸附为放热吸附，焓变为 -77.49 KJ mol-1，而镉(II)的吸附为内热吸附，焓变为 +24.10 KJ mol-1。甲基橙的吸附熵变化为 -0.153 KJ mol-1 K-1，表明吸附状态更有序；而镉（II）的吸附熵变化为 + 0.192 KJ mol-1 K-1，表明吸附状态更无序。甲基橙的吉布斯自由能变化范围为 -32.66 至 -29.60 KJ mol-1，镉（II）的吉布斯自由能变化范围为 -32.29 至 -35.99 KJ mol-1，表明这两种吸附过程都是自发的。这些结果表明，该吸附剂具有作为双吸附材料应用于水修复的潜力。

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引用次数: 0

Investigating the interactions between an industrial lipase and anionic (bio)surfactants 研究工业脂肪酶与阴离子（生物）表面活性剂之间的相互作用。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.060

In laundry formulations, synergies between amphiphiles and other additives such as enzymes increase sustainability through a large decrease in energy consumption. However, traditional surfactants are derived from petroleum, requiring chemical modifications (sulfonation, ethoxylation, or esterification) and generating environmental pollution through toxicity and low degradability. Use of biosurfactants removes these issues. To provide a firmer basis for the use of biosurfactants, we report on the interactions between the industrial lipase LIPEX® and three common biosurfactants, rhamnolipids, sophorolipids, and surfactin. The model surfactant sodium dodecyl sulfate (SDS) is included in the study for comparison. A thorough characterization by Small-angle X-ray scattering (SAXS) provides valuable information on the enzyme’s oligomerization and the surfactant micelles’ ellipsoidal morphology. Additionally, the enzymatic activity and complex formation in different surfactant mixtures are studied using isothermal titration calorimetry, activity assays, and SAXS. SDS activates the enzyme while promoting a controlled association of monomers while the biosurfactants inhibit the enzyme, independent of their effects on its quaternary structure. Rhamnolipids and surfactin promote lipase dimerization while sophorolipids have no significant effect on lipase quaternary structure. Based on these data, we propose a partial replacement that allows the enzyme to retain enzymatic activity while improving the environmental footprint of the formulation.

在洗衣配方中，双亲化合物与酶等其他添加剂之间的协同作用可大幅降低能耗，从而提高可持续性。然而，传统的表面活性剂来自石油，需要进行化学改性（磺化、乙氧基化或酯化），毒性和低降解性会造成环境污染。使用生物表面活性剂则可以解决这些问题。为了给生物表面活性剂的使用提供更坚实的基础，我们报告了工业脂肪酶 LIPEX® 与三种常见生物表面活性剂（鼠李糖脂、槐脂和表面活性剂）之间的相互作用。研究中还加入了模型表面活性剂十二烷基硫酸钠（SDS）进行比较。利用小角 X 射线散射（SAXS）进行的全面表征为酶的低聚作用和表面活性剂胶束的椭圆形形态提供了有价值的信息。此外，还利用等温滴定量热法、活性测定法和 SAXS 研究了不同表面活性剂混合物中的酶活性和复合物形成。SDS 能激活酶，同时促进单体的受控结合，而生物表面活性剂则能抑制酶，这与它们对酶的四元结构的影响无关。鼠李糖脂和表面活性剂可促进脂肪酶的二聚化，而槐脂对脂肪酶的四元结构没有明显影响。根据这些数据，我们提出了一种部分替代品，既能保持酶的活性，又能改善配方对环境的影响。

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引用次数: 0

Z-type heterojunction Pt/Zn0.2Cd0.8S/Cs3PW12O40: Mitigating photocorrosion, leveraging photochromism, and efficient photocatalytic hydrogen evolution Z 型异质结 Pt/Zn0.2Cd0.8S/Cs3PW12O40：减缓光腐蚀、利用光变色和高效光催化氢进化。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-19 DOI: 10.1016/j.jcis.2024.10.090

Catalysts are key components in the photocatalytic hydrogen precipitation process. However, commonly used catalysts such as sulfides, suffer from severe photogenerated carrier recombination and photocorrosion. To address this problem, in this work, Cs₃PW₁₂O₄₀, polyoxometalates with reversible photochromic effect, and Zn_0.2Cd_0.8S with photocorrosivity are constructed to form a Z-type heterojunction to facilitate the separation of photogenerated carriers, and at the same time synergize with the unique photochromic effect of Cs₃PW₁₂O₄₀ to mitigate photocorrosion. Moreover, by introducing the co-catalyst Pt to form a Schottky barrier, which further promotes the separation of photogenerated carriers, the Pt/Zn_0.2Cd_0.8S/Cs₃PW₁₂O₄₀ Z-type heterojunction ternary composites were finally rationally designed and applied to photocatalytic hydrogen precipitation for the first time. The photocatalytic hydrogen precipitation rate of the optimal heterojunction composite was 10.4 mmol/g/h, and its apparent quantum efficiency at a single wavelength of 420 nm could reach 8.15 %. Therefore, this study provides a new strategy for alleviating the photocorrosion of sulfides and the application of polyoxometalates in photocatalytic hydrogen precipitation.

催化剂是光催化析氢过程的关键组成部分。然而，硫化物等常用催化剂存在严重的光生载流子重组和光腐蚀问题。为解决这一问题，本研究将 Cs3PW12O40、具有可逆光致变色效应的多氧金属盐和具有光腐蚀性的 Zn0.2Cd0.8S 构建成 Z 型异质结，以促进光生载流子的分离，同时与 Cs3PW12O40 独特的光致变色效应协同作用，减轻光腐蚀性。此外，通过引入助催化剂铂形成肖特基势垒，进一步促进了光生载流子的分离，最终合理设计出 Pt/Zn0.2Cd0.8S/Cs3PW12O40 Z 型异质结三元复合材料，并首次应用于光催化析氢。最优异质结复合材料的光催化析氢速率为 10.4 mmol/g/h，在 420 nm 单波长下的表观量子效率可达 8.15%。因此，这项研究为减轻硫化物的光腐蚀性和聚氧化金属酸盐在光催化析氢中的应用提供了一种新策略。

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引用次数: 0