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A facile method for studying competitive sorption from binary mixtures of dyes 一种研究二元混合染料竞争吸附的简便方法
Pub Date : 2023-05-13 DOI: 10.1016/j.colsuc.2023.100006
Ernani D.S. Filho, Clara D.M. Cavalcante, Vivian Y. Brizola, Marcia R. Pereira, José L.C. Fonseca

Textile industry produces a great variety of effluents, rich in dyes, which have to be treated, in order to eliminate (or to decrease to secure levels) the contents of these environmentally harmful substances. The first step is the quantitative determination of dye concentrations in the effluent. In this manuscript, we propose a simple method to determine dye concentrations in solutions with two different dyes: acid blue 260, AB, and methyl orange, MO. It was demonstrated that correlating the apparent molar absorptivity of one of the dyes with the concentration of the other dye, a numerical method can be used to determine both dye concentrations and relative errors, using a single value of absorbance for each dye. The method was applied to the sorption of AB and MO on crosslinked chitosan, C-CHIT, and the more effective sorption of AB could be characterized by the determination of different isotherm parameters, estimation of Gibbs free energy of adsorption, as well as competitive sorption by itself.

纺织业产生的废水种类繁多,富含染料,必须对其进行处理,以消除(或降低到安全水平)这些对环境有害的物质。第一步是定量测定废水中的染料浓度。在本文中,我们提出了一种简单的方法来测定两种不同染料溶液中的染料浓度:酸性蓝260,AB和甲基橙,MO。研究表明,将其中一种染料的表观摩尔吸收率与另一种染料浓度相关联,可以使用数值方法来确定染料浓度和相对误差,使用每种染料的单一吸光度值。将该方法应用于AB和MO在交联壳聚糖C-CHIT上的吸附,通过测定不同的等温线参数、估计吸附的吉布斯自由能以及自身的竞争吸附可以表征AB的更有效吸附。
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引用次数: 0
Superhydrophobic sponge with nanoneedle-like surface for efficiently separating immiscible and emulsified oil-water mixtures 具有纳米针状表面的超疏水海绵,可有效分离不混溶和乳化的油水混合物
Pub Date : 2023-05-10 DOI: 10.1016/j.colsuc.2023.100008
Yongfei Zhu , Yonggang Du , Yuxuan Li , Zhi Wang , Junming Su

To increase the collision probability between emulsified droplets and sponge surface for more efficient separation of emulsions, a durable superhydrophobic melamine sponge (MS) with nanoneedle-like surface was prepared through a simple and inexpensive route in this work. The fabrication processes included the formation of ZnO nanoneedles on MS surface via a hydrothermal method, followed by coating with polybenzoxazine based bisphenol A and dodecylamine (PB-D). As excepted, the resulting superhydrophobic sponge (PB-D/ZnO/MS) could effectively separate various surfactant-stabilized water-in-oil and oil-in-water emulsions, with a high permeation flux of up to 14,050 L m−2 h−1 and separation efficiency above 98.5 %, driven solely by gravity due to its nanoneedle-like surface. Moreover, PB-D/ZnO/MS also displayed outstanding absorption capacities for various oils and organic solvents (57.4–123.0 g/g) as well as prominent reusability, enduring 30 cycles of repeated absorption-squeezing without any evident decrease in water contact angle and absorption capacity (maintaining 90.9–96.6 % of initial value). In addition, the superhydrophobicity of PB-D/ZnO/MS remained almost unchanged after being immersed in strong acidic, alkaline and salty solutions for 48 h. Furthermore, PB-D/ZnO/MS not only showed outstanding flame retardancy but also remained rapid oil absorption rate under combustion conditions. Thus, the obtained superhydrophobic MS is a promising candidate for practical oil/water separation.

为了提高乳化液滴与海绵表面的碰撞概率,更有效地分离乳液,本工作通过一种简单而廉价的方法制备了具有纳米针状表面的耐用超疏水三聚氰胺海绵(MS)。制备工艺包括通过水热法在MS表面形成ZnO纳米针,然后用聚苯并恶嗪基双酚a和十二胺(PB-D)涂覆。除此之外,所得到的超疏水海绵(PB-D/ZnO/MS)可以有效地分离各种表面活性剂稳定的油包水和水包油乳液,由于其纳米针状表面,其高渗透通量高达14050 L m−2 h−1,分离效率超过98.5%。此外,PB-D/ZnO/MS对各种油和有机溶剂也表现出优异的吸收能力(57.4–123.0 g/g)以及显著的可重复使用性,经受了30个循环的重复吸收挤压,水接触角和吸收能力没有明显下降(保持初始值的90.9–96.6%)。此外,PB-D/ZnO/MS在强酸性、碱性和含盐溶液中浸泡48小时后,其超疏水性几乎保持不变。此外,PB-D/ZnO/MS在燃烧条件下不仅表现出优异的阻燃性,而且保持了快速的吸油率。因此,所获得的超疏水MS是实用油/水分离的有前途的候选者。
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引用次数: 0
Fixed bed adsorption of phosphate by lanthanum carbonate modified microfibrous composite 碳酸镧改性微纤维复合材料固定床吸附磷酸盐的研究
Pub Date : 2023-05-09 DOI: 10.1016/j.colsuc.2023.100007
Yi Yang

A kind of novel adsorbent, lanthanum carbonate modified microfibrous composite (LC-MC), is synthesized through a facile combined wet lay-up paper making and hydrothermal synthesis method. The fixed bed phosphate adsorption results show that LC-MC performs best when initial phosphate concentration is 5 mg/L, flow rate is 2.7 mL/min and bed height is 2 cm, with the maximum breakthrough time of 82.5 h and maximum adsorption capacity of 38.5 mg/g. High bed height and low flow rate are beneficial to the phosphate adsorption. Acid solution conditions benefit the adsorption process but will cause leakage of the lanthanum species (over 8 mg/L). 50 mg/L co-existing anions have no significant effect on the adsorption process, while concentrations more than 100 mg/L obviously inhibit the adsorption. The adsorbent also shows a good regenerability with less than 15 % decrease in adsorption capacity after 5 cycling runs. The adsorption kinetic process can be described better by the Yoon-Nelson model than Adams-Bohart model and Thomas model. Finally, the mechanism study indicates that the formation of phosphate lanthanum is the main reason for phosphate adsorption on LC-MC. Results show that LC-MC is a promising phosphate adsorbent to be used in fixed bed.

采用湿法和水热合成相结合的方法,合成了一种新型吸附剂——碳酸镧改性超细纤维复合材料(LC-MC)。固定床对磷酸盐的吸附结果表明,当磷酸盐初始浓度为5mg/L,流速为2.7mL/min,床高为2cm时,LC-MC表现最佳,最大穿透时间为82.5h,最大吸附量为38.5mg/g。高床高和低流速有利于磷酸盐的吸附。酸性溶液条件有利于吸附过程,但会导致镧物种的泄漏(超过8mg/L)。50mg/L的共存阴离子对吸附过程没有显著影响,而超过100mg/L的浓度对吸附有明显抑制作用。该吸附剂还显示出良好的再生性,在5次循环运行后吸附容量下降不到15%。Yoon-Nelson模型比Adams-Bohart模型和Thomas模型能更好地描述吸附动力学过程。最后,机理研究表明,磷酸盐镧的形成是LC-MC吸附磷酸盐的主要原因。结果表明,LC-MC是一种很有前途的固定床磷酸盐吸附剂。
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引用次数: 1
Effect of particle size on the capture of uranium oxide colloidal particles from aqueous suspensions via high-gradient magnetic filtration 粒径对高梯度磁滤从水悬浮液中捕获氧化铀胶体颗粒的影响
Pub Date : 2023-03-31 DOI: 10.1016/j.colsuc.2023.100005
Alexander I. Wiechert , Sotira Yiacoumi , Joanna McFarlane , Charles F. Weber , Costas Tsouris

The effectiveness of High Gradient Magnetic Filtration (HGMF) in capturing uranium oxide particles from suspensions was investigated in this study. Two sets of experiments were performed to evaluate the importance of size on the capture of uranium oxide particles. The first considered two batches sieved into size bins of< 5, 5–10, 10–15, and 15–20 µm, while the second was performed using two suspensions with diameters smaller than 1.0 µm and between 1.0 and 1.5 µm. Iron oxide experiments, with particles between 0.3 and 0.8 µm, were performed for calibration purposes. In all experiments, a surfactant (Triton-X100 or sodium dodecyl sulfate) was used to prevent particle aggregation and limit the influence of non-magnetic capture mechanisms. A magnetic field of approximately 1.1 Tesla was generated using a water cooled electromagnet. HGMF was performed using tubular filters packed with ferromagnetic stainless-steel wool. Of the initial four uranium oxide particle sizes, magnetic capture was only observed for particles with a diameter of less than 5 µm, while larger particles experienced no magnetic and minimal total capture. For particles with diameters smaller than 1.0 µm and between 1.0 and 1.5 µm, capture efficiencies increased by 39 ± 9% and 34 ± 6% respectively, solely due to the magnetic field. Although the magnetic force is proportional to particle diameter, the capture efficiency decreased as diameter increased. These results suggest that Brownian diffusion, which is influential for micron sized particles and increases with decreasing particle size, is acting in conjunction with the magnetic force to influence the efficacy of HGMF for uranium oxide. This important finding underscores the effectiveness of Brownian diffusion in increasing the rate of collision between particles and collector fibers. A stochastic trajectory model was developed to incorporate the influence of Brownian motion on particle behavior and filter removal efficiency. Modeling results are discussed and compared for uranium and iron oxide particles.

研究了高梯度磁过滤(HGMF)从悬浮液中捕获氧化铀颗粒的有效性。进行了两组实验来评估尺寸对捕获氧化铀颗粒的重要性。第一个考虑将两个批次筛入<;5、5–10、10–15和15–20µm,而第二次是使用两种直径小于1.0µm且在1.0和1.5µm之间的悬浮液进行的。氧化铁实验的颗粒在0.3和0.8µm之间,用于校准目的。在所有实验中,使用表面活性剂(Triton-X100或十二烷基硫酸钠)来防止颗粒聚集并限制非磁性捕获机制的影响。使用水冷电磁体产生大约1.1特斯拉的磁场。使用填充有铁磁性不锈钢棉的管状过滤器进行HGMF。在最初的四种氧化铀颗粒尺寸中,仅对直径小于5µm的颗粒进行了磁性捕获,而较大的颗粒没有进行磁性捕获,总捕获量最小。对于直径小于1.0µm且介于1.0和1.5µm之间的颗粒,仅由于磁场的作用,捕获效率分别提高了39±9%和34±6%。尽管磁力与颗粒直径成比例,但捕获效率随着直径的增加而降低。这些结果表明,布朗扩散对微米级颗粒有影响,并随着颗粒尺寸的减小而增加,它与磁力一起作用,影响HGMF对氧化铀的效力。这一重要发现强调了布朗扩散在增加颗粒和收集器纤维之间碰撞速率方面的有效性。建立了一个随机轨迹模型,以纳入布朗运动对颗粒行为和过滤器去除效率的影响。讨论并比较了铀和氧化铁颗粒的建模结果。
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引用次数: 1
Role of hydrogen bonding on solvent separation using amphiphilic sorbitan ester 氢键在两亲性山梨醇酯溶剂分离中的作用
Pub Date : 2023-03-15 DOI: 10.1016/j.colsuc.2023.100004
Bibiana Bartokova , Alejandro G. Marangoni , Thamara Laredo , Erica Pensini

Tetrahydrofuran (THF) and water are miscible and interact trough hydrogen (H) bonds. Span 80 (sorbitan ester) is soluble in THF, but not water. Nonetheless, Span 80 H bonds with water, as shown by attenuated total reflectance – Fourier transform infrared spectroscopy. In pure water, species are single (SD) or double (DD) donors, and single (SA) or double (DA) acceptors. In pure water, SD-SA and DD-DA are dominant and have similar abundance. Span 80 and THF alter the distribution of water species. When THF and Span 80 compete for the same water species, THF separation from water is most effective. Span 80 induces a marked shift of SD-SA to higher wavenumbers, which are close to DD-DA. This species intermediate between DD-DA and SD-SA is dominant, indicating that Span 80 mainly interacts with it. This same species is also dominant in THF-water mixtures containing 50–70% THF. Instead, DD-DA is dominant up to 40% THF, while DD-SA dominate at the highest THF percentages. Bottle tests show that Span 80 separates THF and water into bulk phases with 50–70% THF within 1 hr. In contrast, outside this THF range, emulsions are stable for more than 1 hr, as observed by either light scattering or optical microscopy. In mixtures with 50–70% THF, bulk phase separation occurs within 1 hr, because Span 80 competes with THF for the same water species. Separation is poorer outside of this THF range, where Span 80 and THF interact with different water species.

四氢呋喃(THF)和水是可混溶的,并通过氢(H)键相互作用。Span 80(山梨醇酯)可溶于THF,但不溶于水。尽管如此,Span 80H与水结合,如衰减的全反射-傅立叶变换红外光谱所示。在纯水中,物种是单(SD)或双(DD)供体,以及单(SA)或双重(DA)受体。在纯水中,SD-SA和DD-DA占主导地位,丰度相似。跨度80和THF改变了水物种的分布。当THF和Span 80竞争相同的水物种时,THF与水的分离是最有效的。跨度80引起SD-SA向更高波数的显著偏移,更高波数接近DD-DA。这种介于DD-DA和SD-SA之间的物种占主导地位,表明Span 80主要与其相互作用。在含有50-70%THF的THF-水混合物中,这种物种也占主导地位。相反,DD-DA在高达40%的THF时占主导地位,而DD-SA在THF百分比最高时占主导。瓶子测试表明,Span 80在1小时内将THF和水分离成体积相,THF为50-70%。相反,在该THF范围之外,乳液稳定超过1小时,如通过光散射或光学显微镜观察到的。在THF为50–70%的混合物中,体相分离在1小时内发生,因为Span 80与THF竞争相同的水物种。在该THF范围之外,分离较差,其中Span 80和THF与不同的水物种相互作用。
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引用次数: 4
Fabrication of superhydrophilic mask non-woven fabric with cellulose/GO composite coating for oil/water separation 纤维素/氧化石墨烯复合涂层制备油水分离超亲水性掩膜无纺布
Pub Date : 2023-03-11 DOI: 10.1016/j.colsuc.2023.100003
Jinlong Wu , Yukun Fu , Haoqi Li , Mengyan Tan , Yonglan Zhang

Superwettable coatings have aroused considerable attention in oil/water separation materials research benefit from their many advantages, such as various preparation methods, high separation efficiency, and low cost. However, many of these coatings are not suitable for practical separation due to the complex composite methods and poor biodegradability. The development of novel superwettable oil/water separation materials with simple fabrication and eco-friendly coating has become a noteworthy target in oil/water separation fields. Since the outbreak of COVID-19, a large number of waste masks abandoned in the natural environments have caused serious environmental hazards. The mask non-woven fabric (MNF) from waste disposable medical masks is a good separation material for its rich microporous. Herein, regenerated degreasing cotton cellulose and graphene oxide (GO) were used to successfully construct an environmentally friendly composite coating on the MNF through a simple dip coating method, and the obtained Cellulose/GO@MNF has excellent superhydrophilicity and underwater superoleophobicity. The fabricated coating possesses favorable chemical stability and nice mechanical strength after being destroyed by corrosive solutions (acid, alkali, salt solution) and physical processing (scratches). Various oil/water mixtures can be separated with high separation efficiency (>98%), and the separation efficiency is absent a substantive drop even after 10 separate cycles. Water can be removed quickly and continuously from the oil/water mixture by the as-fabricated MNF linking with a peristaltic pump. Besides, toluene oil-in-water emulsion can also be separated effectively. What is more significant is that, the Cellulose/GO@MNF fabric fabricated via a simple method and using biodegradable coating materials has potential application prospects in solving both recycling problems of waste masks and oil/water pollution.

超湿性涂料以其制备方法多样、分离效率高、成本低等优点,在油水分离材料的研究中引起了广泛的关注。然而,由于复合方法复杂,生物降解性差,许多涂层不适合实际分离。开发制造简单、涂层环保的新型超润湿性油水分离材料已成为油水分离领域的一个值得关注的目标。新冠肺炎疫情发生以来,大量废弃在自然环境中的废弃口罩造成了严重的环境危害。从废弃一次性医用口罩中提取的口罩无纺布具有丰富的微孔性,是一种很好的分离材料。本文利用再生脱脂棉纤维素和氧化石墨烯(GO),通过简单的浸涂方法,成功地在MNF上构建了一种环保的复合涂层,得到了纤维素/GO@MNF具有优异的超亲水性和水下超疏油性。所制备的涂层经腐蚀性溶液(酸、碱、盐溶液)和物理处理(划痕)破坏后,具有良好的化学稳定性和良好的机械强度。可以以高分离效率(>;98%)分离各种油/水混合物,并且即使在10个分离循环之后,分离效率也没有显著下降。通过与蠕动泵连接的所制造的MNF,可以快速且连续地从油/水混合物中去除水。此外,甲苯水包油乳液也能有效分离。更重要的是,纤维素/GO@MNF采用可生物降解涂层材料,通过简单的方法制备的织物在解决废弃口罩回收和油/水污染问题方面具有潜在的应用前景。
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引用次数: 0
Modelling the reaction of uranium with carboxylic groups on surfaces through mono- and multi- dentate surface complexes on the basis of pH and redox potential 在pH值和氧化还原电位的基础上,通过单齿和多齿表面配合物模拟铀与表面羧基的反应
Pub Date : 2023-02-26 DOI: 10.1016/j.colsuc.2023.100002
Steven McGowan, Claude Degueldre, Farid Aiouache

An analytical expression is proposed to simulate effects of pH and redox potential (E) on the sorption of uranium onto bioorganic model particles in saline or other aquatic environments. The elaborated expression is intended to avoid use of the classical approach of sorption which relies on experimental data and empirical models. The goal is to produce an expression that provides a distribution coefficient (Kd e.g. mL g−1) as function of pH, E and ligand concentration (through complex formation in solution) by applying a surface complexation model on one type of mono-dentate surface sites> (SuOH) as well as utilizing multi-dentate surface sites> (SuOH)c. The formulation of the worked out expression makes use of correlations between the surface complexation and hydrolysis constants for all species and sorption sites. The model was applied to the sorption of uranium onto bioorganic sites with and without carbonates in solution e.g. Log Kd: + 2.75 at pH 8 for 2 sites per nm2. The calculated distribution coefficients were found very sensitive to the presence of carbonates, e.g. Log Kd: − 7.0 at pH 8 for 2 × 10−3 M total carbonate. The potential reduction of uranium U(VI) and its complexes (carbonates) which are the primary stable species in surface waters, to U(IV) during sorption was simulated in association with a decrease in the redox potential and was found generally below the redox stability limits of water. The calculated distribution coefficient values were validated by the values reported in literature for the sorption of uranium onto specific adsorbents. The investigated simulations are also applicable to the sorption of other redox sensitive elements.

提出了一个分析表达式来模拟pH和氧化还原电位(E)对盐水或其他水生环境中生物有机模型颗粒吸附铀的影响。详细的表述旨在避免使用依赖于实验数据和经验模型的经典吸附方法。目标是通过在一种类型的单齿表面位点上应用表面络合模型来产生提供作为pH、e和配体浓度(通过在溶液中形成络合物)的函数的分布系数(Kd,例如mL g−1)的表达式>;(SuOH)以及利用多齿表面位点>;(SuOH)c。计算出的表达式的公式利用了所有物种和吸附位点的表面络合和水解常数之间的相关性。该模型应用于在溶液中含有和不含有碳酸盐的生物有机位点上吸附铀,例如在pH 8下,对数Kd:+2.75,每nm2吸附2个位点。计算的分布系数对碳酸盐的存在非常敏感,例如,对于2×10−3 M的总碳酸盐,在pH 8时的对数Kd:−7.0。铀U(VI)及其络合物(碳酸盐)是地表水中的主要稳定物种,在吸附过程中被模拟为U(IV)的电势还原与氧化还原电势的降低有关,并且通常低于水的氧化还原稳定性极限。计算的分布系数值通过文献中报道的铀在特定吸附剂上的吸附值进行了验证。所研究的模拟也适用于其他氧化还原敏感元素的吸附。
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引用次数: 0
Study on droplet wettability of low surface tension working medium based on special-shaped microstructure surface 基于异形微结构表面的低表面张力工质液滴润湿性研究
Pub Date : 2023-02-09 DOI: 10.1016/j.colsuc.2023.100001
Chao Dang , Xiaowei Wang , Hao Li , Liaofei Yin , Mengjie Song

The wetting properties of droplets on microstructure surfaces directly determine the hydrophobic properties of the surface, and the size effect is an important part of the study of droplet wettability on microstructure surfaces. Taking reentrant special-shaped microstructure and doubly-reentrant special-shaped microstructure as the research objects, the influences of many geometric parameters of microstructure on the wetting characteristics of droplet with low surface tension were obtained by numerical simulation and theoretical analysis, and the concept of critical intrinsic contact angle was proposed. It is found that the two kinds of special-shaped microstructures can suspend the droplet with low surface tension, and the droplet finally presents a large apparent contact angle. However, there are three kinds of wetting transition (Cassie state →Wenzel state transition) on the surface of the doubly-reentrant special-shaped microstructure, so the wetting regulation mechanism of the surface with the same geometric parameters is different from that of the reentrant special-shaped microstructure. In addition, by analyzing the energy barrier at the pinning point, it is further proved that the doubly-reentrant special-shaped microstructure has better performance of inhibiting the wetting transition of droplet.

微滴在微观结构表面的润湿性能直接决定了表面的疏水性能,尺寸效应是微滴在微结构表面润湿性研究的重要组成部分。以凹入型异形微结构和双凹入型异型微结构为研究对象,通过数值模拟和理论分析,得到了微结构的许多几何参数对低表面张力液滴润湿特性的影响,并提出了临界本征接触角的概念。研究发现,这两种异形微结构可以以较低的表面张力悬浮液滴,液滴最终呈现出较大的表观接触角。然而,有三种类型的润湿转变(卡西态→Wenzel态转变),因此具有相同几何参数的表面的润湿调节机制与凹形异形微观结构的润湿调节机理不同。此外,通过分析钉扎点的能垒,进一步证明了双凹入异形微结构具有更好的抑制液滴润湿转变的性能。
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引用次数: 1
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Colloids and Surfaces C: Environmental Aspects
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