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Probing the fouling induced by biomolecules of a polymer microfiltration membrane using 3D cryo-FIB/SEM 利用三维冷冻fib /SEM研究生物分子对聚合物微滤膜的污染
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137045
Hélène Roberge , Philippe Moreau , Estelle Couallier , Patricia Abellan
Membrane fouling is the main technical limitation to membrane filtration processes aimed at effectively separating valuable biomolecules from microalgae solutions. Although several fouling mechanisms have been proposed, they have rarely been directly observed. In this work, we demonstrate the direct nanometer-scale visualization of fouling both inside and on the surface of membranes. To mimic the microfiltration of real bioresource extracts, model solutions of lipids, proteins, and their mixtures were filtered, and the consecutively fouled membranes were analysed and reconstructed in 3D at high resolution using cryogenic focused ion beam coupled with scanning electron microscopy (cryo-FIB/SEM). Nanometer-scale analysis using deep learning segmentation tools (random forest combined with U-net model) uncovers membrane fouling mechanisms previously hypothesized, providing insights into how filtration depends on complex mixture composition. A quantitative analysis of the pores that are fouled or blocked, and open pores that can actively contribute to filtration is established. The methodology presented in this work provides directly probed, relevant information on membrane fouling structures that are scarcely accessible by other means, with broad applications to filtration processes in both industry and biotechnology research.
膜污染是膜过滤过程的主要技术限制,膜过滤过程旨在有效地从微藻溶液中分离有价值的生物分子。虽然提出了几种结垢机制,但它们很少被直接观察到。在这项工作中,我们展示了在纳米尺度上对膜内部和表面污垢的直接可视化。为了模拟真实生物资源提取物的微过滤,我们对脂质、蛋白质及其混合物的模型溶液进行了过滤,并利用低温聚焦离子束和扫描电镜(cro - fib /SEM)在高分辨率下对连续污染的膜进行了三维分析和重建。使用深度学习分割工具(随机森林与U-net模型相结合)的纳米尺度分析揭示了之前假设的膜污染机制,为过滤如何依赖于复杂的混合物组成提供了见解。对被污染或堵塞的孔隙和能够积极促进过滤的开放孔隙进行定量分析。在这项工作中提出的方法提供了直接探测的膜污染结构的相关信息,这些信息很难通过其他方式获得,在工业和生物技术研究的过滤过程中具有广泛的应用。
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引用次数: 0
A two-step precipitation strategy for zinc recovery and magnesium control in sulfate solutions: process optimization and mechanistic insights 硫酸盐溶液中锌回收和镁控制的两步沉淀策略:工艺优化和机理见解
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137047
Zhimei Xia, Jing He, Caiyi Wang, Weihuan Xia, Shengjie Yi, Longgang Ye, Shufen Liu, Li Zhang, Yujie Hu
The accumulation of magnesium in zinc hydrometallurgy systems poses significant challenges to process efficiency and product quality. Existing removal methods often suffer from low selectivity, high energy consumption, or environmental concerns. This study proposes a novel two-step precipitation strategy using sodium bicarbonate for selective zinc recovery and magnesium control from purified zinc sulfate solution (PZSS). Under optimized conditions (1 mol/L NaHCO3, 100% stoichiometric NaHCO3 relative to Zn2+, 35 °C, 5 h, and 14 mL/min feed rate), Zn was recovered as ZnCO3 with a high recovery rate of 99.86% and a low magnesium co-precipitation of only 1.64%. Subsequent magnesium removal using ammonia water achieved over 92% efficiency. The selective precipitation mechanism is attributed to the large solubility difference between ZnCO3 and MgCO3 under neutral pH conditions, coupled with the kinetic preference for ZnCO3 nucleation, as elucidated by species distribution analysis, XRD, and SEM-EDS. This method provides an efficient, environmentally friendly alternative for magnesium management in zinc hydrometallurgy.
锌湿法冶金系统中镁的积累对工艺效率和产品质量提出了重大挑战。现有的去除方法往往存在选择性低、能耗高或环境问题。本研究提出了一种利用碳酸氢钠对纯化硫酸锌溶液(PZSS)进行选择性锌回收和镁控制的新型两步沉淀策略。优化条件为:NaHCO3浓度为1 mol/L, NaHCO3相对于Zn2+浓度为100%,加料温度为35℃,加料时间为5 h,加料速率为14 mL/min。在此条件下,锌以ZnCO3的形式回收,回收率高达99.86%,镁共析出率仅为1.64%。随后使用氨水去除镁的效率达到92%以上。通过物种分布分析、XRD和SEM-EDS分析,发现选择性沉淀机制是由于中性pH条件下ZnCO3和MgCO3的溶解度差异较大,加之动力学倾向于ZnCO3成核。该方法为湿法锌冶炼中镁的管理提供了一种高效、环保的替代方法。
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引用次数: 0
Machine learning–driven identification of key factors governing hormone adsorption by agrifood waste–derived adsorbents 机器学习驱动的农业食品垃圾吸附剂对激素吸附的关键因素识别
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137033
Masud Parvez , Ahasanul Karim , Zarifeh Raji , Isa Ebtehaj , Hossein Bonakdari , Seddik Khalloufi
Hormone contamination in aquatic systems threatens human health and ecosystems, demanding efficient and sustainable separation strategies. This study aims to develop a machine learning (ML) framework to predict hormone adsorption using agrifood waste-derived adsorbents and to identify the key variables governing adsorption efficiency. A dataset of 604 observations with nine input variables was compiled from peer-reviewed studies. Three ensemble ML algorithms—Random Forest (RF), Least Squares Boosting, and M5 model trees—were evaluated across 511 models generated from all combinations of one to nine input variables. RF demonstrated the highest predictive accuracy, achieving a maximum test coefficient of determination (R2) of 0.976 and a minimum mean absolute error of 4.26 using eight input variables. Model robustness was assessed using a Combined Index (CI) integrating six statistical metrics, which decreased from a median value of 0.78 for single-input models to 0.0006 for the optimal eight-input configuration; the full nine-input model yielded CI = 0.0019. Bayesian optimization using the Expected Improvement per Second acquisition function further improved model performance, producing the highest test Nash–Sutcliffe efficiency (0.951) and the lowest normalized root mean square error (0.162) and ratio of root mean square error to standard deviation (0.221). Feature importance analysis identified initial concentration, contact time, pH, and adsorbent-to-solution ratio as the most influential predictors of adsorption efficiency. Hormone-specific analyses for 17β-estradiol (318 data points) and 17α-ethinylestradiol (106 data points) confirmed the robustness of these findings. The results show that optimized ML models support the design of sustainable adsorption-based hormone removal systems.
水生系统中的激素污染威胁着人类健康和生态系统,需要有效和可持续的分离策略。本研究旨在开发一个机器学习(ML)框架,以预测使用农业食品垃圾衍生吸附剂的激素吸附,并确定控制吸附效率的关键变量。从同行评议的研究中编译了604个观察结果和9个输入变量的数据集。三种集成ML算法——随机森林(RF)、最小二乘增强和M5模型树——在511个模型中进行了评估,这些模型是由1到9个输入变量的所有组合生成的。RF具有最高的预测精度,8个输入变量的最大检验决定系数(R2)为0.976,最小平均绝对误差为4.26。模型稳健性评估采用综合六个统计指标的综合指数(CI),从单输入模型的中位数0.78下降到最佳八输入配置的0.0006;完整的9个输入模型的CI = 0.0019。贝叶斯优化利用每秒预期改进(Expected Improvement per Second)获取函数进一步提高了模型的性能,产生最高的检验Nash-Sutcliffe效率(0.951),最低的归一化均方根误差(0.162)和均方根误差与标准差之比(0.221)。特征重要性分析表明,初始浓度、接触时间、pH值和吸附剂与溶液的比例是影响吸附效率的最重要因素。对17β-雌二醇(318个数据点)和17α-炔雌醇(106个数据点)的激素特异性分析证实了这些发现的稳健性。结果表明,优化的ML模型支持基于可持续吸附的激素去除系统的设计。
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引用次数: 0
La vacancy-induced enhancement of CoO and oxygen vacancy for efficient chlorobenzene oxidation La空位诱导CoO和氧空位增强对氯苯的有效氧化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137035
Mingjiao Tian , Yaruo Zhao , Qin Yang , Changwei Chen , Han Xu , Dong Guo , Zeyu Jiang , Haohua Kang , Shan Ren , Chi He
The environmentally friendly purification of chlorinated volatile organic compounds (CVOCs) is a challenge in current air pollution control. Construction of active oxygen species on the catalyst surface is a promising strategy to promote the cleavage of CCl bond and the destruction of CVOC molecules. Herein, an oxygen-vacancy-rich perovskite-type 3LaCoO3 catalyst was constructed for the efficient catalytic oxidation of chlorobenzene (CB). The partial removal of La in 3LaCoO3 structure effectively modulates charge redistribution of Co sites, facilitating the Co3+/Co2+ redox cycle. Additionally, the La vacancy significantly enhanced the mobility of surface O22−, O2, and O species of 3LaCoO3 along with the generation of oxygen vacancies, exhibiting the optimal oxygen activation capacity, which enhances the pathway: CB → phenolate species → C=C/CH3/COOH → HCl/CO2/H2O and suppresses the formation of hazardous vinyl chloride, trichloroethane, dichloromethane, and chloroform. This study provides critical insights into the construction of oxygen vacancies and the development of active surface oxygen species for industrial CVOC stable and efficient elimination.
氯化挥发性有机物的环境友好净化是当前大气污染治理的一个挑战。在催化剂表面构建活性氧是促进CCl键断裂和破坏CVOC分子的一种很有前途的策略。本文构建了富氧空位钙钛矿型3LaCoO3催化剂,用于氯苯(CB)的高效催化氧化。3LaCoO3结构中La的部分去除有效地调节了Co位点的电荷再分配,促进了Co3+/Co2+的氧化还原循环。此外,La空位显著增强了3LaCoO3表面O22−、O2−和O−的迁移率,同时氧空位的生成,表现出最佳的氧活化能力,强化了CB→酚类物质→C=C/CH3/COOH→HCl/CO2/H2O的途径,抑制了有害物质氯乙烯、三氯乙烷、二氯甲烷和氯仿的生成。该研究为氧空位的构建和活性表面氧的开发提供了重要的见解,以稳定和有效地消除工业CVOC。
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引用次数: 0
Regulating electronic state of δ-MnO2 through an organic-inorganic hybrid engineering for boosted low-temperature NOx elimination 通过有机-无机杂化工程调节δ-MnO2的电子态,促进低温NOx的去除
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137036
Hanbo Shi , Nannan Zhang , Wei Guo , Tancheng Dong , Bihui Zhou , Lanlan Yu , Baojun Liu , Jincheng Mu
Birnessite-type δ-MnO2 is a promising candidate for low-temperature NH3-SCR reaction owning to its excellent redox properties. However, its performance is severely hampered by the excessive oxidation state of Mn species, which induces strong NH3 chemisorption and subsequent over-oxidation to NOx. Herein, phenylalanine-functionalized δ-MnO2 nanosheets (MnOx-Phe) were developed, leveraging Phe's coordinating –NH2 group to modulate surface properties of Mn species. The optimal MnOx-Phe-0.1 catalyst achieves ∼90% NOx conversion at 75 °C with a broad temperature window from 75 to 210 °C (GHSV = 50,000 h−1), representing a reaction rate 4.8 to 8.2 times greater than that of pure δ-MnO2. Additionally, the catalyst exhibits remarkable resistance against SO2 and H2O. Comprehensive characterizations and density functional theory calculations reveal that Phe modification shifts down the d-band center of δ-MnO2 from −1.22 eV to −2.78 eV, and attenuates the oxidation state of Mn species. This unique configuration suppresses the over-oxidation of NH3 and weakens the interaction between catalyst and poisons, while promoting the activation of NH3 to *NH2 with a lower energy barrier, thus driving a desired Eley-Rideal pathway and endowing strong tolerance against SO2 and H2O at low temperatures. This work provides a novel organic-inorganic hybrid strategy for designing robust low-temperature NH3-SCR catalysts with superior activity and poison resistance.
birnite型δ-MnO2具有良好的氧化还原性能,是低温NH3-SCR反应的理想候选物。然而,锰的过度氧化状态严重阻碍了其性能,导致NH3的强烈化学吸附和随后的NOx的过度氧化。本文开发了苯丙氨酸功能化的δ-MnO2纳米片(MnOx-Phe),利用Phe的配位-NH2基团来调节Mn的表面性质。最佳的mnox - ph -0.1催化剂在75°C和75 ~ 210°C的宽温度窗口(GHSV = 50,000 h−1)下实现了~ 90%的NOx转化率,其反应速率是纯δ-MnO2的4.8 ~ 8.2倍。此外,该催化剂对SO2和H2O具有显著的抗性。综合表征和密度泛函理论计算表明,Phe修饰使δ-MnO2的d带中心从- 1.22 eV下移至- 2.78 eV,并减弱了Mn的氧化态。这种独特的结构抑制了NH3的过度氧化,减弱了催化剂与毒物的相互作用,同时促进NH3以较低的能垒活化为*NH2,从而驱动了理想的ley- rideal途径,并赋予了低温下对SO2和H2O的强耐受性。本研究为设计具有优良活性和耐毒性的低温NH3-SCR催化剂提供了一种新的有机-无机杂化策略。
{"title":"Regulating electronic state of δ-MnO2 through an organic-inorganic hybrid engineering for boosted low-temperature NOx elimination","authors":"Hanbo Shi ,&nbsp;Nannan Zhang ,&nbsp;Wei Guo ,&nbsp;Tancheng Dong ,&nbsp;Bihui Zhou ,&nbsp;Lanlan Yu ,&nbsp;Baojun Liu ,&nbsp;Jincheng Mu","doi":"10.1016/j.seppur.2026.137036","DOIUrl":"10.1016/j.seppur.2026.137036","url":null,"abstract":"<div><div>Birnessite-type δ-MnO<sub>2</sub> is a promising candidate for low-temperature NH<sub>3</sub>-SCR reaction owning to its excellent redox properties. However, its performance is severely hampered by the excessive oxidation state of Mn species, which induces strong NH<sub>3</sub> chemisorption and subsequent over-oxidation to NO<sub>x</sub>. Herein, phenylalanine-functionalized δ-MnO<sub>2</sub> nanosheets (MnO<sub>x</sub>-Phe) were developed, leveraging Phe's coordinating –NH<sub>2</sub> group to modulate surface properties of Mn species. The optimal MnO<sub>x</sub>-Phe-0.1 catalyst achieves ∼90% NO<sub>x</sub> conversion at 75 °C with a broad temperature window from 75 to 210 °C (GHSV = 50,000 h<sup>−1</sup>), representing a reaction rate 4.8 to 8.2 times greater than that of pure δ-MnO<sub>2</sub>. Additionally, the catalyst exhibits remarkable resistance against SO<sub>2</sub> and H<sub>2</sub>O. Comprehensive characterizations and density functional theory calculations reveal that Phe modification shifts down the <em>d</em>-band center of δ-MnO<sub>2</sub> from −1.22 eV to −2.78 eV, and attenuates the oxidation state of Mn species. This unique configuration suppresses the over-oxidation of NH<sub>3</sub> and weakens the interaction between catalyst and poisons, while promoting the activation of NH<sub>3</sub> to *NH<sub>2</sub> with a lower energy barrier, thus driving a desired Eley-Rideal pathway and endowing strong tolerance against SO<sub>2</sub> and H<sub>2</sub>O at low temperatures. This work provides a novel organic-inorganic hybrid strategy for designing robust low-temperature NH<sub>3</sub>-SCR catalysts with superior activity and poison resistance.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137036"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The ternary TiO2/γ-Fe2O3/γ-AlOOH magnetic composite adsorbent material with excellent catalytic oxidation-adsorption capacity for trivalent arsenic (As(III)): Material characterization, adsorption investigation, mechanism exploration 具有优异催化氧化吸附三价砷(As(III))能力的TiO2/γ-Fe2O3/γ-AlOOH三元磁性复合吸附材料:材料表征、吸附研究及机理探讨
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137005
He Guowen , Wu Dan , Ma Dechong , Li Yuanping , Wang Liqin , Yang Fanming , Li Yibing , Li Zhonglin
Arsenic(III) [As(III)] contamination in wastewater poses severe threats to ecosystems and human health, demanding efficient treatment technologies. Herein, a ternary magnetic TiO2/γ-Fe2O3/H-γ-AlOOH composite with synergistic photocatalytic oxidation and adsorption capabilities is novelly constructed via a sol–gel-hydrothermal method, using γ-Fe2O3/H-γ-AlOOH as the precursor. Comprehensive characterizations (XRD, FT-IR, BET, SEM/TEM, XPS, UV–Vis DRS, VSM) confirms that anatase TiO2 nanoparticles (≈15 nm) are uniformly coated on the precursor surface, forming a flower-like mesoporous structure (specific surface area of 116.48 m2 g−1, pore volume of 0.21 cm3 g−1, average pore size of 6.33 nm). The composite exhibits a saturation magnetization (MS) of 18.28 emu g−1 for rapid magnetic separation and a narrowed band gap (2.41 eV) for enhanced photocatalytic activity. Static adsorption experiments illustrate the saturated As(III) adsorption capacity is 93.25 ± 2.961 mg g−1, and Kinetic and isotherm analyses indicates the process conforms to the PSO model and Langmuir model, confirming monolayer chemical adsorption. Thermodynamic results (ΔG < 0, ΔH = 6.321 kJ mol−1, ΔS = 114.628 J mol−1 K−1) reveals spontaneous, endothermic, and entropy-driven adsorption. The underlying mechanism demonstrates that TiO2 is photocatalysized to generate •O2 radicals under UV irradiation to oxidize most As(III) to As(V), both As(III) and As(V) then underwent ligand exchange with surface –OH groups of Al, Fe, and Ti components to form stable inner-sphere complexes. The as-constructed multifunctional composite integrates efficient oxidation, adsorption, magnetic recovery, and cyclic stability, offering a promising solution for As(III)-containing wastewater treatment and a strategy for designing heavy metal remediation materials.
废水中的砷(III) [As(III)]污染对生态系统和人类健康构成严重威胁,需要高效的处理技术。本文以γ-Fe2O3/H-γ-AlOOH为前驱体,采用溶胶-凝胶-水热法制备了具有协同光催化氧化和吸附能力的TiO2/γ-Fe2O3/H-γ-AlOOH三元磁性复合材料。综合表征(XRD、FT-IR、BET、SEM/TEM、XPS、UV-Vis DRS、VSM)证实锐钛矿型TiO2纳米颗粒(≈15 nm)均匀包裹在前驱体表面,形成花状介孔结构(比表面积为116.48 m2 g−1,孔体积为0.21 cm3 g−1,平均孔径为6.33 nm)。该复合材料具有18.28 emu g−1的饱和磁化强度(MS)和2.41 eV的窄带隙(MS),有利于快速磁分离和增强光催化活性。静态吸附实验表明,饱和As(III)的吸附量为93.25±2.961 mg g−1,动力学和等温线分析表明,该过程符合PSO模型和Langmuir模型,确认为单层化学吸附。热力学结果(ΔG < 0, ΔH = 6.321 kJ mol−1,ΔS = 114.628 jmol−1 K−1)揭示了自发、吸热和熵驱动的吸附。潜在的机制表明,在紫外照射下,TiO2被光催化生成•O2−自由基,将大部分As(III)氧化为As(V), As(III)和As(V)与Al、Fe和Ti组分的表面-OH基团进行配体交换,形成稳定的球内配合物。该多功能复合材料集高效氧化、吸附、磁回收和循环稳定性于一体,为含砷废水处理和重金属修复材料的设计提供了一种有前景的解决方案。
{"title":"The ternary TiO2/γ-Fe2O3/γ-AlOOH magnetic composite adsorbent material with excellent catalytic oxidation-adsorption capacity for trivalent arsenic (As(III)): Material characterization, adsorption investigation, mechanism exploration","authors":"He Guowen ,&nbsp;Wu Dan ,&nbsp;Ma Dechong ,&nbsp;Li Yuanping ,&nbsp;Wang Liqin ,&nbsp;Yang Fanming ,&nbsp;Li Yibing ,&nbsp;Li Zhonglin","doi":"10.1016/j.seppur.2026.137005","DOIUrl":"10.1016/j.seppur.2026.137005","url":null,"abstract":"<div><div>Arsenic(III) [As(III)] contamination in wastewater poses severe threats to ecosystems and human health, demanding efficient treatment technologies. Herein, a ternary magnetic TiO<sub>2</sub>/<em>γ</em>-Fe<sub>2</sub>O<sub>3</sub>/H-<em>γ</em>-AlOOH composite with synergistic photocatalytic oxidation and adsorption capabilities is novelly constructed via a sol–gel-hydrothermal method, using <em>γ</em>-Fe<sub>2</sub>O<sub>3</sub>/H-<em>γ</em>-AlOOH as the precursor. Comprehensive characterizations (XRD, FT-IR, BET, SEM/TEM, XPS, UV–Vis DRS, VSM) confirms that anatase TiO<sub>2</sub> nanoparticles (≈15 nm) are uniformly coated on the precursor surface, forming a flower-like mesoporous structure (specific surface area of 116.48 m<sup>2</sup> g<sup>−1</sup>, pore volume of 0.21 cm<sup>3</sup> g<sup>−1</sup>, average pore size of 6.33 nm). The composite exhibits a saturation magnetization (MS) of 18.28 emu g<sup>−1</sup> for rapid magnetic separation and a narrowed band gap (2.41 eV) for enhanced photocatalytic activity. Static adsorption experiments illustrate the saturated As(III) adsorption capacity is 93.25 ± 2.961 mg g<sup>−1</sup>, and Kinetic and isotherm analyses indicates the process conforms to the PSO model and Langmuir model, confirming monolayer chemical adsorption. Thermodynamic results (<em>ΔG</em> &lt; 0, <em>ΔH</em> = 6.321 kJ mol<sup>−1</sup>, <em>ΔS</em> = 114.628 J mol<sup>−1</sup> K<sup>−1</sup>) reveals spontaneous, endothermic, and entropy-driven adsorption. The underlying mechanism demonstrates that TiO<sub>2</sub> is photocatalysized to generate •O<sub>2</sub><sup>−</sup> radicals under UV irradiation to oxidize most As(III) to As(V), both As(III) and As(V) then underwent ligand exchange with surface –OH groups of Al, Fe, and Ti components to form stable inner-sphere complexes. The as-constructed multifunctional composite integrates efficient oxidation, adsorption, magnetic recovery, and cyclic stability, offering a promising solution for As(III)-containing wastewater treatment and a strategy for designing heavy metal remediation materials.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137005"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Algae-resistant microfiltration membranes with silica brush structures for efficient chlorella harvesting 抗藻微滤膜硅刷结构高效小球藻收获
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137037
Yanlin Zhang , Haiyan Lu , Dehao Yu , Yuhao Chen , Tengfang Zhang , Wenguang Wang , Haixiang Sun , Baosheng Ge
Advanced membrane separation technology exhibits great potential for achieving algae harvesting. However, it is challenging to solve the issues of membrane fouling caused by algal cells and extracellular organic matter. Herein, a polyaminophenylene (PAP) layer is constructed on the polyethersulfone (PES) microfiltration membrane surface through the diazonium-induced anchoring process (DIAP), followed by a two-step crosslinking reaction with trimesoyl chloride (TMC) and γ-aminopropyltriethoxysilane (APTES) to form the modified layer with the silicon brush structure. Various physicochemical characterizations and molecular dynamic simulations elucidate that compared with the pristine PES membrane, the silicon brush structure causes the APTES-modified membranes (AMMs) to possess lower surface energy, lower interaction energy and higher electrostatic repulsion between pollutants and the surface, which significantly improve the membrane antifouling performance. The optimal membrane (AMM-0.5) demonstrates outstanding performance with high water permeance (nearly 2500 L·m−2·h−1·bar−1) and flux recovery rate (99.4%), and maintain stable operation with just approximately 10% flux decline during six chlorella harvesting concentration cycles. This study can provide an economical, sustainable separation technology of industrial-scale microalgae production for bioenergy, food and pharmaceutical sectors.
先进的膜分离技术在实现藻类收获方面显示出巨大的潜力。然而,解决由藻细胞和胞外有机物引起的膜污染问题是一个挑战。本文通过重氮诱导锚定工艺(DIAP)在聚醚砜(PES)微滤膜表面构建聚氨基苯(PAP)层,然后与三甲酰氯(TMC)和γ-氨基丙基三乙氧基硅烷(APTES)进行两步交联反应,形成具有硅刷结构的改性层。各种物理化学表征和分子动力学模拟表明,与原始PES膜相比,硅刷结构使aptes修饰膜具有更低的表面能、更低的相互作用能和更高的污染物与表面之间的静电排斥,从而显著提高了膜的防污性能。最优膜(am -0.5)具有较高的透水性(接近2500 L·m−2·h−1·bar−1)和通量回收率(99.4%),并且在6次小球藻收集浓缩循环中通量下降仅约10%的情况下保持稳定运行。该研究可为生物能源、食品和制药行业提供一种经济、可持续的工业规模微藻分离技术。
{"title":"Algae-resistant microfiltration membranes with silica brush structures for efficient chlorella harvesting","authors":"Yanlin Zhang ,&nbsp;Haiyan Lu ,&nbsp;Dehao Yu ,&nbsp;Yuhao Chen ,&nbsp;Tengfang Zhang ,&nbsp;Wenguang Wang ,&nbsp;Haixiang Sun ,&nbsp;Baosheng Ge","doi":"10.1016/j.seppur.2026.137037","DOIUrl":"10.1016/j.seppur.2026.137037","url":null,"abstract":"<div><div>Advanced membrane separation technology exhibits great potential for achieving algae harvesting. However, it is challenging to solve the issues of membrane fouling caused by algal cells and extracellular organic matter. Herein, a polyaminophenylene (PAP) layer is constructed on the polyethersulfone (PES) microfiltration membrane surface through the diazonium-induced anchoring process (DIAP), followed by a two-step crosslinking reaction with trimesoyl chloride (TMC) and γ-aminopropyltriethoxysilane (APTES) to form the modified layer with the silicon brush structure. Various physicochemical characterizations and molecular dynamic simulations elucidate that compared with the pristine PES membrane, the silicon brush structure causes the APTES-modified membranes (AMMs) to possess lower surface energy, lower interaction energy and higher electrostatic repulsion between pollutants and the surface, which significantly improve the membrane antifouling performance. The optimal membrane (AMM-0.5) demonstrates outstanding performance with high water permeance (nearly 2500 L·m<sup>−2</sup>·h<sup>−1</sup>·bar<sup>−1</sup>) and flux recovery rate (99.4%), and maintain stable operation with just approximately 10% flux decline during six chlorella harvesting concentration cycles. This study can provide an economical, sustainable separation technology of industrial-scale microalgae production for bioenergy, food and pharmaceutical sectors.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137037"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Purifying circRNA by ultrafiltration with membranes having well-defined pores 通过具有明确孔隙的膜的超滤纯化环状rna
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137031
Karen Guillen-Cuevas, Caroline C. Hansen, Deepraj Sarmah, Marc R. Birtwistle, Scott M. Husson
Circular RNA (circRNA) is a promising therapeutic modality owing to its enhanced stability conferred by exonuclease resistance. However, large-scale production remains limited by inefficient purification methods, as the standard approach using size-exclusion chromatography suffers from peak overlap and low yield. Here, we present an ultrafiltration strategy for purifying circRNA using polycarbonate track-etched membranes with precisely controlled pore diameters. Membrane pore sizes were fine-tuned by gold plating to separate circular and linear RNA conformers. Sieving coefficients of purified RNA conformers were measured to establish operating conditions, and continuous diafiltration experiments were conducted within the range of flux values predicted to achieve both high purity and yield. This approach resulted in 94% purity and 59% yield of circRNA from in vitro transcription mixtures after six diavolumes. Transfection studies in HEK293T cells confirmed that diafiltered circRNA exhibited gene expression levels comparable to enzymatically purified circRNA, albeit with modestly reduced transfection efficiency. These results establish membrane-based ultrafiltration with tailored pore sizes as a scalable, non-chromatographic platform for purifying circRNA and provide a framework for further development toward therapeutic circRNA manufacturing.
环状RNA (circRNA)是一种很有前途的治疗方式,由于其增强的稳定性赋予外切酶抗性。然而,大规模生产仍然受到效率低下的纯化方法的限制,因为使用尺寸排除色谱的标准方法存在峰重叠和低收率的问题。在这里,我们提出了一种超滤策略,用于净化环状rna,使用具有精确控制孔径的聚碳酸酯轨迹蚀刻膜。通过镀金微调膜孔径,分离环状和线性RNA构象。测定纯化RNA构象的筛分系数以确定操作条件,并在预测的通量值范围内进行连续滤滤实验,以获得高纯度和高产量。该方法在六次回积后,从体外转录混合物中获得94%的纯度和59%的产量。HEK293T细胞的转染研究证实,滤过的circRNA表现出与酶纯化的circRNA相当的基因表达水平,尽管转染效率略有降低。这些结果建立了具有定制孔径的基于膜的超滤技术,作为一种可扩展的、非色谱的circRNA净化平台,并为进一步开发治疗性circRNA制造提供了框架。
{"title":"Purifying circRNA by ultrafiltration with membranes having well-defined pores","authors":"Karen Guillen-Cuevas,&nbsp;Caroline C. Hansen,&nbsp;Deepraj Sarmah,&nbsp;Marc R. Birtwistle,&nbsp;Scott M. Husson","doi":"10.1016/j.seppur.2026.137031","DOIUrl":"10.1016/j.seppur.2026.137031","url":null,"abstract":"<div><div>Circular RNA (circRNA) is a promising therapeutic modality owing to its enhanced stability conferred by exonuclease resistance. However, large-scale production remains limited by inefficient purification methods, as the standard approach using size-exclusion chromatography suffers from peak overlap and low yield. Here, we present an ultrafiltration strategy for purifying circRNA using polycarbonate track-etched membranes with precisely controlled pore diameters. Membrane pore sizes were fine-tuned by gold plating to separate circular and linear RNA conformers. Sieving coefficients of purified RNA conformers were measured to establish operating conditions, and continuous diafiltration experiments were conducted within the range of flux values predicted to achieve both high purity and yield. This approach resulted in 94% purity and 59% yield of circRNA from <em>in vitro</em> transcription mixtures after six diavolumes. Transfection studies in HEK293T cells confirmed that diafiltered circRNA exhibited gene expression levels comparable to enzymatically purified circRNA, albeit with modestly reduced transfection efficiency. These results establish membrane-based ultrafiltration with tailored pore sizes as a scalable, non-chromatographic platform for purifying circRNA and provide a framework for further development toward therapeutic circRNA manufacturing.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137031"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Accelerating Cu(II)/Cu(I) cycling via Ni/S synergy for selective and efficient electrocatalytic ammonia oxidation Ni/S协同加速Cu(II)/Cu(I)循环选择性高效电催化氨氧化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137034
Hailong Wang , Chenjian Ye , Ruijie Ge , Jianzhong Zhu , Binglu Teng
The practical application of electrocatalytic ammonia oxidation reaction (EAOR), in the clean treatment of ammonia-containing wastewater, is constrained by slow reaction kinetics and low selectivity of dinitrogen. In this study, a stable Ni-MIL(Cu)-S electrocatalyst by synergistic regulation of Cu sites through Ni/S on a MIL-like framework confining catalytic platform was constructed. It reveals that Ni serves as an electron trap while S acts as an electron donor, cooperatively optimizing the coordination electronic structure of Cu site. This accelerates its valence state cycling (Cu(II)/Cu(I)), lowering the energy barrier of EAOR. Wherein, the key step of “*NH₂ dimerization to form N–N bond” is preferably accelerated, effectively avoiding the generation of byproducts. Consequently, 98.70% NH4+-N removal rate and 98.03% N₂ selectivity were achieved with good cycling stability. This study provides a novel approach for electronic structure regulation in developing efficient and selective EAOR electrocatalysts.
电催化氨氧化反应(EAOR)在含氨废水清洁处理中的实际应用受到反应动力学缓慢和二氮选择性低的限制。本研究在类mil框架约束催化平台上,通过Ni/S对Cu位点进行协同调节,构建了稳定的Ni- mil (Cu)-S电催化剂。结果表明,Ni作为电子陷阱,S作为电子给体,协同优化了Cu位点的配位电子结构。这加速了其价态循环(Cu(II)/Cu(I)),降低了EAOR的能垒。其中,“* nh2二聚化形成N-N键”的关键步骤最好加快,有效避免了副产物的产生。NH4+-N去除率为98.70%,N选择性为98.03%,循环稳定性好。本研究为开发高效选择性EAOR电催化剂提供了电子结构调控的新途径。
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引用次数: 0
Ionic interactions drive SC[4]A to regulate polyamide networks for achieving high-efficiency Li+/Mg2+ separation 离子相互作用驱动SC bbbba调节聚酰胺网络,以实现高效的Li+/Mg2+分离
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-24 DOI: 10.1016/j.seppur.2026.137014
Wei Shao , Xiuling Liu , Zhaojing Jing , Ziyang Guo , Xiaowen Huo , Weihao Zhang , Haitao Wang , Na Chang
The selective separation of lithium and magnesium by conventional nanofiltration (NF) membranes remains a major challenge for lithium extraction from salt-lake brine. This difficulty results from the extremely fast and disordered nature of the interfacial polymerization process, which hampers precise control over the pore size of the separation layer. In this study, to utilize the hollow internal cavity of the macrocycle, calix[4]arene was directly sulfonated to prepare hydrophilic sulfonated calix[4]arene (SC[4]A), which was incorporated as an aqueous-phase additive into the piperazine (PIP) solution. NF membranes were then fabricated via interfacial polymerization (IP) on a self-made polysulfone (PSf) substrate. The results demonstrated that SC[4]A effectively accelerated the kinetics of the IP reaction. More importantly, SC[4]A, which was ionically bonded into the polyamide (PA), served as the additional mass transfer channel and formed a separation layer with a smaller free volume, narrower pore size distribution, and enhanced negative surface charge. The prepared TFC-0.5 membrane exhibited a Li+/Mg2+ separation factor as high as 28.90, a 2.19-fold increase over the pristine membrane. Additionally, the incorporation of SC[4]A improved the hydrophilicity of the membrane surface, imparting superior antifouling properties to the modified membrane. By precisely regulating the IP process and tailoring the free volume of the separation layer, this study provides a new strategy for developing high-performance lithium‑magnesium separation NF membranes.
传统纳滤膜对锂和镁的选择性分离一直是盐湖卤水锂提取面临的主要挑战。这种困难源于界面聚合过程的极快和无序性,这阻碍了对分离层孔径的精确控制。本研究利用大环中空的内腔,将杯[4]芳烃直接磺化制备亲水性磺化杯[4]芳烃(SC[4]A),并将其作为水相添加剂掺入哌嗪(PIP)溶液中。然后在自制的聚砜(PSf)衬底上通过界面聚合(IP)制备了纳滤膜。结果表明,SC[4]A有效地加速了IP反应的动力学。更重要的是,SC[4]A与聚酰胺(PA)离子键结合,作为额外的传质通道,形成了自由体积更小、孔径分布更窄、表面负电荷增强的分离层。制备的TFC-0.5膜的Li+/Mg2+分离系数高达28.90,是原始膜的2.19倍。此外,SC[4]A的掺入改善了膜表面的亲水性,使改性膜具有优异的防污性能。通过精确调节IP过程和定制分离层的自由体积,本研究为开发高性能锂镁分离NF膜提供了新的策略。
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Separation and Purification Technology
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