Separation and Purification Technology最新文献_第3页

Bifunctional FeZr cyanide frameworks modified with Pluronic F127 and amine groups for CO2 adsorption: Performance and mechanism Pluronic F127和胺基修饰双官能团FeZr氰化物框架的CO2吸附性能及机理

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136874

Ying Wang, Linlin Geng, Xiaoya Wang, Jianwen Wei, Xuecong Ma, Lei Liao

Amine-modified adsorbents exhibit remarkable potential for efficient CO₂ capture. In this study, a series of amine-based bifunctional solid adsorbents for CO₂ capture was synthesized via an impregnation method. FeZr cyanide frameworks were first functionalized with Pluronic F127, followed by the immobilization of diethanolamine (DEA) and tetraethylenepentamine (TEPA) at different loadings (20–40 wt%). Among the resulting materials, FZ(F)-D35% (DEA) and FZ(F)-T35% (TEPA), exhibited the maximum CO₂ adsorption capacity at 45 °C, reaching 1.846 and 2.377 mmol·g⁻¹. Compared with the unmodified material (FZ), which exhibits an adsorption capacity of 0.989 mmol/g, they increased by 47% and 59%, respectively. After 6 adsorption-desorption cycles, FZ(F)-D35% and FZ(F)-T35% still retained 93.4% and 95.2% of their original capacities, respectively, exhibiting excellent cycling stability. Kinetic analysis indicated that the adsorption process followed the Avrami model (R² = 0.999), suggesting a dual mechanism involving both physisorption and chemisorption. Infrared spectroscopy further confirmed the formation of carbamate and hydrogen bonding during the CO₂ adsorption, highlighting the critical synergistic role played by amine groups and hydroxyl groups in the CO₂ adsorption mechanism. It can therefore be inferred that the CO₂ adsorption mechanism is consistent with the zwitterion mechanism. These findings highlight the potential of amine-functionalized FeZr cyanide frameworks as robust, regenerable adsorbents for moderate-temperature CO₂ capture.

胺改性吸附剂在有效捕获二氧化碳方面表现出显著的潜力。本研究采用浸渍法制备了一系列胺基双功能固体吸附剂。首先用Pluronic F127对FeZr氰化框架进行功能化，然后以不同的负载（20-40 wt%）固定二乙醇胺（DEA）和四乙基戊二胺（TEPA）。所得材料中，FZ(F)-D35% （DEA）和FZ(F)-T35% （TEPA）在45℃时的CO2吸附量最大，分别为1.846和2.377 mmol·g−1。与未改性材料FZ的吸附量（0.989 mmol/g）相比，分别提高了47%和59%。经过6次吸附-解吸循环后，FZ(F)-D35%和FZ(F)-T35%的容量仍保持在原来的93.4%和95.2%，具有良好的循环稳定性。动力学分析表明，吸附过程符合Avrami模型（R2 = 0.999），存在物理吸附和化学吸附双重机理。红外光谱进一步证实了CO2吸附过程中氨基甲酸酯和氢键的形成，凸显了胺基和羟基在CO2吸附机制中起着至关重要的协同作用。因此可以推断CO2的吸附机理与两性离子的吸附机理是一致的。这些发现突出了胺功能化FeZr氰化物框架作为稳健、可再生的中温CO2捕获吸附剂的潜力。

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引用次数: 0

Defect-engineered Co3O4-LaCoO3 heterojunctions effectively activate lattice oxygen species, enabling high-efficiency photothermal-assisted catalytic performance 缺陷工程Co3O4-LaCoO3异质结有效激活晶格氧，实现高效光热辅助催化性能

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136883

Jinwei Liang , Mengyao Wan , Cui Li, Shan Wang, Kezhen Qi

Transition metal oxides possess high photothermal conversion efficiency and excellent thermal catalytic activity, which can be further enhanced by exploiting the photoelectric effect in semiconductors. In this study, a Co₃O₄-LaCoO₃ composite with an Step-scheme (S-scheme) heterojunction was fabricated for photo-thermal catalytic carbon monoxide oxidation under ultraviolet-visible (UV–Vis) light irradiation. The heterointerface of Co₃O₄-LaCoO₃ promotes the formation of oxygen vacancies, thereby enhancing the reactive oxygen species generation and surface lattice oxygen migration. Photoelectrochemical analysis reveals that the built-in electric field and band bending at the Co₃O₄-LaCoO₃ interface optimize photogenerated carrier transfer while maintaining high redox potentials. Under UV–Vis illumination, the rapid interfacial electron transfer facilitates the generation of more reactive free radicals. Remarkably, the Co₃O₄-LaCoO₃ composite achieves 100% CO oxidation efficiency through photo-thermal synergy at 150 °C, significantly outperforming individual components (45.06% and 64.20%). This work provides valuable guidance for designing and fabricating high-efficiency narrow-bandgap semiconductor heterojunction photothermal catalysts.

过渡金属氧化物具有较高的光热转换效率和优异的热催化活性，利用半导体中的光电效应可以进一步增强这一特性。在紫外-可见（UV-Vis）光的照射下，制备了具有阶梯结构（S-scheme）异质结的Co3O4-LaCoO3复合材料，用于光热催化一氧化碳氧化。Co3O4-LaCoO3的异质界面促进了氧空位的形成，从而促进了活性氧的生成和表面点阵氧的迁移。光电化学分析表明，Co3O4-LaCoO3界面的内置电场和能带弯曲优化了光生载流子转移，同时保持了高氧化还原电位。在UV-Vis照射下，快速的界面电子转移有利于自由基的生成。值得注意的是，Co3O4-LaCoO3复合材料在150°C时通过光热协同作用达到100%的CO氧化效率，显著优于单个组分（45.06%和64.20%）。本研究为设计和制备高效窄带隙半导体异质结光热催化剂提供了有价值的指导。

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引用次数: 0

Ligand-defect engineered amorphous MOFs via glycerol-assisted synthesis for efficient photo-Fenton degradation of fluoroquinolone antibiotics at neutral pH 甘油辅助合成配体缺陷工程无定形MOFs，用于中性pH下氟喹诺酮类抗生素的光- fenton降解

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136881

Bowen Zhu , Zuopeng Li , Qianyi Li , Chang-qing Miao , Sanbing Zhang

Amorphization offers a transformative route to dramatically enhance the catalytic performance of metal-organic frameworks (MOFs) by disrupting their perfect periodicity, thereby generating plethora of defects and highly disordered coordination environments. Herein, we present GM-100, a strikingly defective amorphous MOF synthesized for the first time via a facile, ambient in situ esterification-modulated approach, in which glycerol partially reacts with the carboxyl groups of trimesic acid to form ester bonds that occupy coordination sites otherwise destined for Fe. This deliberate partial esterification severely impairs full ligand-to-metal coordination, suppresses long-range crystallization, and yields a disordered, defect-rich framework-despite identical precursor stoichiometry to crystalline MIL-100(Fe). Under neutral pH, GM-100 exhibits outstanding photo-Fenton activity: achieving the removal rate of 96.5% of high-concentration moxifloxacin (0.5 mM) within just 90 min, and removing ≥81.4% of other fluoroquinolone antibiotics under equally challenging conditions. Mechanistic studies reveal that this exceptional performance arises from exposed partially unsaturated Fe centers, accelerated Fe³⁺/Fe²⁺ redox cycling, dramatically enhanced ROS generation, and remarkably facile substrate/oxidant diffusion enabled by pore openness induced by ligand vacancies. A quantitative structure-activity relationship (QSAR) model further confirms the catalytic versatility of GM-100 across diverse fluoroquinolone antibiotics, signaling strong potential for real-world water purification under mild, environmentally relevant conditions.

非晶化通过破坏金属有机骨架（mof）的完美周期性，从而产生过多的缺陷和高度无序的配位环境，从而极大地提高了金属有机骨架（mof）的催化性能。本文中，我们提出了GM-100，这是一种有明显缺陷的无定形MOF，首次通过简单的环境原位酯化调制方法合成，其中甘油与三羧酸的羧基部分反应形成酯键，占据了原本用于铁的配位位点。这种故意的部分酯化严重损害了配体与金属的完全配位，抑制了远程结晶，并产生了无序的、富含缺陷的框架——尽管与晶体MIL-100（Fe）的前体化学计量相同。在中性pH条件下，GM-100表现出出色的光fenton活性：在90分钟内对高浓度莫西沙星（0.5 mM）的去除率达到96.5%，在同样具有挑战性的条件下对其他氟喹诺酮类抗生素的去除率≥81.4%。机制研究表明，这种特殊的性能源于暴露的部分不饱和铁中心，加速的Fe3+/Fe2+氧化还原循环，显著增强的ROS生成，以及配体空位诱导的孔隙开放使底物/氧化剂非常容易扩散。定量构效关系（QSAR）模型进一步证实了GM-100对多种氟喹诺酮类抗生素的催化通用性，表明在温和的环境相关条件下，现实世界的水净化具有强大的潜力。

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引用次数: 0

Crystalline-amorphous hybrid NiO on nickel foam for robust ozone decomposition under high humidity 泡沫镍上的结晶-非晶杂化NiO在高湿条件下的强臭氧分解

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136878

Jing Wang, Tianle Cai, Jialin Li, Jingling Yang, Mingshan Zhu

Catalytic ozone (O₃) decomposition is an efficient strategy to addressing the growing problem of O₃ pollution in urban and industrial environments. However, the accumulation of intermediate oxygen species and the competitive adsorption of water molecules on the active sites of catalysts lead to a decrease in the activity of O₃ catalytic decomposition. Developing O₃ decomposition catalysts that exhibit both high activity for O₃-to-O₂ conversion and excellent moisture resistance remains a critical challenge. Here, we designed a crystalline-amorphous hybrid NiO catalyst by in situ growth of NiO on a three-dimensional conductive nickel foam scaffold (denoted as NNF-2), integrating the advantages of both crystalline and amorphous phases for catalysis. Systematic characterization reveals that NNF-2 combines the strong reactant affinity of the amorphous phase with efficient electron transport properties imparted by the crystalline phase, thereby promoting O₃ adsorption and water molecule dissociation, and enabling co-decomposition of O₃ and H₂O. As a result, NNF-2 exhibits outstanding O₃ decomposition activity and stability across a broad range of relative humidity (15–90% RH) and at low temperature (−15 °C) under a gas hourly space velocity of 25,400 h⁻¹. Even under high humidity (70% RH), NNF-2 maintains 96.0% O₃ removal over 50 h. This study demonstrates a simple and efficient crystalline-amorphous hybrid design that significantly improves the practical potential of O₃ decomposition catalysts under highly humid conditions.

催化臭氧分解是解决城市和工业环境中日益严重的臭氧污染问题的有效策略。然而，中间氧的积累和水分子在催化剂活性位点的竞争性吸附导致O3催化分解活性降低。开发既具有高活性的O3- o2转化又具有优异的抗湿性的O3分解催化剂仍然是一个关键的挑战。本文通过在三维导电泡沫镍支架（表示为NNF-2）上原位生长NiO，结合晶体相和非晶态相催化的优点，设计了一种晶体-非晶态混合NiO催化剂。系统表征表明，NNF-2结合了非晶相的强亲和力和晶体相的高效电子传递特性，从而促进了O3的吸附和水分子的解离，实现了O3和H2O的共分解。因此，NNF-2在相对湿度（15 - 90% RH）和低温（- 15°C）范围内，在每小时25,400 h - 1的气体空间速度下，都表现出出色的O3分解活性和稳定性。即使在高湿条件下（70% RH）， NNF-2在50小时内也能保持96.0%的O3去除率。本研究展示了一种简单高效的结晶-非晶杂化设计，显著提高了O3分解催化剂在高湿条件下的实际应用潜力。

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引用次数: 0

Rational selection of diaminoalkanes for grafting onto Zr-based MOFs with different pore sizes for enhanced CO2 capture 合理选择二氨基烷烃接枝到不同孔径zr基mof上以增强CO2捕集

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136875

Gyudong Lee, So Yeon Lee, Minyoung Yoon, Sung Hwa Jhung

Efficient CO₂ capture using amine-functionalized metal-organic frameworks (MOFs) requires a rational design strategy that considers the interplay between amine configuration and pore geometry. In this study, a series of Zr-based MOFs (UiO-67, MOF-808, and NU-1000) were post-synthetically functionalized by grafting diaminoalkanes of varying chain lengths onto their metal sites. The structure-function relationship between the host MOFs and the grafted amines, which governs CO₂ adsorption performance, was systematically investigated. The CO₂ uptake, isosteric heat of adsorption, and ideal adsorbed solution theory (IAST) CO₂/N₂ selectivity all initially increased and then decreased with increasing the chain length of the grafted diamines, showing maximum performance when the diamine length was optimally matched to the MOF pore size. At the optimal combinations (U67-DAB, M808-DAPen, and N1000-DAO), the materials exhibited 1.3–2.7 times the CO₂ uptake at 15 kPa and 3.3–17.8 times the CO₂/N₂ selectivity at 100 kPa compared with the pristine MOFs. Spectroscopic analyses (FTIR and XPS) confirmed that ammonium carbamate formation occurs only when the terminal amines are spatially proximate, enabling cooperative chemisorption. These results highlight that spatial compatibility between MOF pore size and diamine length is a critical factor in maximizing CO₂ capture efficiency via ammonium carbamate formation. This study provides a generalizable guideline for tailoring amine-functionalized MOFs for efficient CO₂ adsorption.

利用胺功能化金属有机框架（mof）高效捕获二氧化碳需要合理的设计策略，考虑胺结构和孔隙几何形状之间的相互作用。在本研究中，通过接枝不同链长的二氨基烷烃在其金属位点上，对一系列zr基mof （UiO-67、MOF-808和NU-1000）进行了后合成功能化。系统地研究了宿主MOFs与接枝胺之间的结构-功能关系，以及接枝胺对CO2吸附性能的影响。CO2吸收率、等等吸附热和理想吸附溶液理论（IAST） CO2/N2选择性均随接枝二胺链长的增加先增加后降低，当二胺长度与MOF孔径匹配时表现出最大的性能。在最佳组合（U67-DAB、M808-DAPen和N1000-DAO）下，材料在15 kPa下的CO2吸收率是原始mof的1.3 ~ 2.7倍，在100 kPa下的CO2/N2选择性是原始mof的3.3 ~ 17.8倍。光谱分析（FTIR和XPS）证实，氨基甲酸铵的形成只有在末端胺在空间上接近时才会发生，从而实现协同化学吸附。这些结果表明，MOF孔径和二胺长度之间的空间相容性是通过氨基甲酸铵形成最大化CO2捕获效率的关键因素。该研究为定制胺功能化mof以高效吸附CO2提供了可推广的指导方针。

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引用次数: 0

Machine learning-assisted performance prediction of pervaporation membrane for the separation of alcohol-water mixtures 机器学习辅助渗透蒸发膜分离酒精-水混合物的性能预测

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-12 DOI: 10.1016/j.seppur.2026.136880

Ting Jiang , Qing-Yuan Han , Rong-Ze Zhu , Yong-Le Dou , Xiu Yue , Fu-Xin Ma , Sikandeer Saifuding , Wen Ma , Peng-Cheng Ma

Growing industrial demand for efficient alcohol-water separation drives the need for advanced membrane technologies such as pervaporation, which outperform conventional methods in energy efficiency and scalability but currently rely on trial-and-error development. In this study, a comprehensive dataset was established by encompassing membrane structural parameters, operational conditions, and solvent properties, including the Hildebrand parameter of polymer monomers, which reflects the sorption selectivity of solvents in membranes. Robustness was ensured by eliminating outliers and handling missing data, followed by the evaluation of nine machine learning models. The CatBoost model exhibited optimal performance for total flux prediction, whereas the XGBoost model was most effective for separation factor prediction. Through global importance analysis, the Hildebrand parameter was identified as the most influential feature for the separation factor and the third most significant contributor to the flux, underscoring the governing role of the solution-diffusion mechanism in pervaporation separation. The synergistic effects of membrane characteristics and operational parameters were further elucidated via the two-dimensional partial dependence plots. Finally, the models were generalized to predict separation performance for isopropanol-water and n-butanol-water mixtures, achieving high precision in flux prediction. The findings of the current study provide theoretical support for the design of high-performance pervaporation membranes for the separation of alcohol-water mixtures.

对高效醇水分离的工业需求不断增长，推动了对渗透蒸发等先进膜技术的需求。渗透蒸发技术在能源效率和可扩展性方面优于传统方法，但目前依赖于反复试验的开发。在这项研究中，建立了一个综合的数据集，包括膜结构参数、操作条件和溶剂性质，包括聚合物单体的希尔德布兰德参数，反映了溶剂在膜中的吸附选择性。通过消除异常值和处理缺失数据来确保鲁棒性，然后对9个机器学习模型进行评估。CatBoost模型对总通量的预测效果最佳，而XGBoost模型对分离因子的预测效果最好。通过全局重要性分析，确定了Hildebrand参数是对分离因素影响最大的特征，是通量的第三大贡献者，强调了溶液扩散机制在渗透蒸发分离中的控制作用。通过二维偏相关图进一步阐明了膜特性与操作参数的协同效应。最后，将模型推广到异丙醇-水和正丁醇-水混合物的分离性能预测中，获得了较高的通量预测精度。本研究结果为设计高性能的醇水混合分离渗透蒸发膜提供了理论支持。

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引用次数: 0

Accuracy and limitations of constant salt rejection assumption in brackish water RO membranes modeling: CFD and experimental validation 微咸水反渗透膜模型中恒盐抑制假设的准确性和局限性：CFD和实验验证

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-11 DOI: 10.1016/j.seppur.2026.136856

Mehrad Tajik, Alireza Hamidi, Alireza Jalali

Reverse osmosis (RO) is the leading desalination method due to its high removal efficiency and low energy demand. Numerical simulations are widely used to study RO processes; however, the complexity of membrane transport modeling has led many studies to treat salt rejection, <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></math></script></span>, as an intrinsic membrane property and to neglect membrane salt permeability. This study experimentally and numerically assessed that assumption for brackish water RO (BWRO) membranes using a bench-scale cross-flow test cell. Water and salt permeabilities, <em>A</em> and <em>B</em>, were determined and measurement uncertainty were quantified. <em>A</em> remained stable across operating conditions, while the apparent variability in <em>B</em> was statistically consistent with experimental uncertainty. Two numerical models were evaluated against the experimental data. Model 1 incorporates the full solution–diffusion mechanism for membrane transport, while Model 2 assumes <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></math></script></span> is an intrinsic membrane property. Both models predict water flux and concentration polarization accurately. However, for permeate concentration, <span><span><math><msub is="true"><mi is="true">C</mi><mi is="true" mathvariant="normal">p</mi></msub></math></span><script type="math/mml"><math><msub is="true"><mi is="true">C</mi><mi mathvariant="normal" is="true">p</mi></msub></math></script></span>, Model 2 under constant <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></math></script></span> assumption showed large deviations, with a maximum error of 216.25% and an average error of 61.06%, while Model 1 with constant <em>B</em> assumption reduced these errors to 18.68% and 10.1%, respectively. Using the validated numerical model, a parametric study on three commercial membranes under various BWRO operating conditions shows that <em>Rej</em> is strongly influenced by membrane characteristics, feed salinity, and pressure. For each membrane, <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></math></script></span> increases with feed concentration and pressure. At practical operating conditions, the range of <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></math></script></span> variability is limited; however, even small deviations in <span><span><math><mi is="true" mathvariant="italic">Rej</mi></math></span><script type="math/mml"><math><mi mathvariant="italic" is="true">Rej</mi></ma

反渗透（RO）因其去除效率高、能耗低而成为海水淡化的主要方法。数值模拟被广泛用于研究RO过程；然而，由于膜传输模型的复杂性，导致许多研究将盐排斥（RejRej）视为膜的固有特性，而忽略了膜盐的渗透性。本研究通过实验和数值方法对微咸水反渗透（BWRO）膜进行了验证。测定水和盐渗透率A和B，并量化测量不确定度。A在操作条件下保持稳定，而B的表观变异性在统计上与实验不确定性一致。根据实验数据对两种数值模型进行了评价。模型1包含了膜运输的完整溶液扩散机制，而模型2假设RejRej是一种固有的膜性质。两种模式都能准确预测水通量和浓度极化。然而，对于渗透浓度CpCp，模型2在恒定RejRej假设下的偏差较大，最大误差为216.25%，平均误差为61.06%，而模型1在恒定B假设下的误差分别减小到18.68%和10.1%。利用验证的数值模型，对三种不同BWRO操作条件下的工业膜进行了参数化研究，结果表明，Rej受膜特性、进料盐度和压力的影响很大。对于每个膜，RejRej随进料浓度和压力的增加而增加。在实际操作条件下，RejRej可变性的范围是有限的；然而，在高饲料浓度下，即使RejRej的微小偏差也会显著影响渗透浓度CpCp。

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引用次数: 0

Trimetallic PCN-250 MOFs for synergistic radical-mediated photocatalytic degradation of microplastics 协同自由基介导光催化降解微塑料的三金属PCN-250 mof

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-11 DOI: 10.1016/j.seppur.2026.136842

Muhammad Haris Khan , Zareen Zuhra , Wajid Hussain , Zhang Zhaowei , Shafqat Ali

Microplastics (MPs) are among the most persistent and hazardous forms of plastic pollution, and their degradation under ambient environmental conditions requires the development of unique materials. In this study, we designed a series of diverse metal-based PCN-250 MOFs, including FeCuMn, Fe₂Cu, Fe₂Mn, and Fe₃, engineered to exploit multimetallic synergy for the enhanced photocatalytic degradation of polystyrene (PS) and polypropylene (PP) MPs. The photocatalytic performance results revealed that PCN-250(FeCuMn) exhibited excellent activity, achieving 91.2% and 97.0% degradation, respectively, within 8 h. Furthermore, the excellent reusability retained 78.6% efficiency after five cycles without structural loss of PCN-250 FeCuMn. This superior performance was attributed to the synergistic role of multimetallic centers in enhancing redox activity, high surface area (925.7 m²g⁻¹), narrowing the band gap (2.47 eV), and generating multiple reactive oxygen species (•OH, O₂•⁻, ¹O₂). Mechanistic insights were provided through EPR, radical quenching, FT-IR and LC-MS analyses, which provide the evidence of extensive structural degradation and fragmentation of MPs into oxygenated low molecular weight intermediates. The study introduces a promising photocatalyst platform with potential applications for sustainable microplastic (MP) remediation.

微塑料（MPs）是最持久和最危险的塑料污染形式之一，在环境条件下降解它们需要开发独特的材料。在这项研究中，我们设计了一系列不同金属基的PCN-250 mof，包括FeCuMn、Fe₂Cu、Fe₂Mn和Fe₃，旨在利用多金属协同作用来增强光催化降解聚苯乙烯（PS）和聚丙烯（PP） MPs。结果表明，PCN-250（FeCuMn）具有优异的光催化活性，在8 h内降解率分别为91.2%和97.0%。此外，PCN-250 FeCuMn在5次循环后仍保持78.6%的效率，且没有结构损失。这种优异的性能归因于多金属中心的协同作用，增强了氧化还原活性，高表面积（925.7 m2−1），缩小了带隙（2.47 nm），并产生了多种活性氧（•OH, O₂•−,O₂）。通过EPR、自由基猝灭、FT-IR和LC-MS分析提供了机制见解，这些分析提供了MPs广泛的结构降解和裂解成含氧低分子量中间体的证据。该研究介绍了一种具有潜在应用前景的光催化剂平台，用于可持续微塑料（MP）修复。

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引用次数: 0

Tailoring NiFe2O4 nanoparticles via electron-rich co centers and abundant redox pairs: boosting peroxymonosulfate activation for micropollutant degradation 通过富电子co中心和丰富的氧化还原对定制NiFe2O4纳米颗粒：促进过氧单硫酸盐活化微污染物降解

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-11 DOI: 10.1016/j.seppur.2026.136859

Bao Pan, Jiahao Zhang, Ruobai Li, Yanle Zhou, Jiani Qin, Rong Xu, Chuanyi Wang

The pervasive presence of pharmaceutical and personal care products (PPCPs) in water bodies underscores the urgency for the advancement of efficient and sustainable methods for their removal. Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have demonstrated significant potential in water purification, with their effectiveness largely hinging on the development of high-performance catalysts. In this study, cobalt-doped nickel ferrite (Co-NFO) nanocatalysts were synthesized using a sol-gel combined with calcination method to enhance PMS activation for the degradation of micropollutants. Characterization results confirmed the successful incorporation of Co into the spinel lattice of NFO, which improved phase purity and electronic properties without significantly affecting textural features. The optimized 2.5%Co-NFO catalyst demonstrated exceptional performance in the degradation of carbamazepine (CBZ), achieving a 92.7% degradation efficiency within 15 min, significantly outperforming the undoped NFO catalyst. The system demonstrated broad applicability across various micropollutants and maintained excellent stability and reusability over multiple reaction cycles. In-depth mechanistic studies, incorporating radical quenching experiments, electron paramagnetic resonance (EPR) analysis, electrochemical measurements, and density functional theory (DFT) calculations, have elucidated that the degradation process is driven by a multitude of reactive species. The enhanced catalytic activity was attributed to the improved electron transfer efficiency and stronger PMS adsorption at Co-active sites. Potential CBZ degradation pathways were proposed, and toxicity assessment indicated a general reduction in the acute toxicity of the generated intermediates. This study introduces an innovative Co-doped magnetic catalyst, which, through the doping process, significantly enhances its catalytic activity for PMS activation, thereby offering a promising solution for efficient water purification.

水体中普遍存在的药品和个人护理产品（PPCPs）强调了推进有效和可持续的去除方法的紧迫性。基于过氧单硫酸盐（PMS）的高级氧化工艺（AOPs）在水净化方面显示出巨大的潜力，其有效性很大程度上取决于高性能催化剂的开发。本研究采用溶胶-凝胶结合煅烧法制备了钴掺杂镍铁氧体（Co-NFO）纳米催化剂，以提高PMS的活性，降解微污染物。表征结果证实，Co成功掺入NFO的尖晶石晶格中，在不显著影响织构特征的情况下，提高了相纯度和电子性能。优化后的2.5%Co-NFO催化剂对卡马西平（CBZ）的降解性能优异，在15 min内达到92.7%的降解效率，明显优于未掺杂的NFO催化剂。该系统广泛适用于各种微污染物，并在多个反应周期中保持良好的稳定性和可重复使用性。深入的机理研究，包括自由基猝灭实验、电子顺磁共振（EPR）分析、电化学测量和密度泛函理论（DFT）计算，已经阐明了降解过程是由多种反应物质驱动的。催化活性的增强是由于电子转移效率的提高和共活性位点对PMS的吸附作用增强。提出了潜在的CBZ降解途径，毒性评估表明生成的中间体的急性毒性普遍降低。本研究介绍了一种新型共掺杂磁性催化剂，通过掺杂工艺，显著提高了其对PMS活化的催化活性，为高效水净化提供了一种很有前景的解决方案。

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引用次数: 0

Enhanced capacitive deionization of Cu2+ via hollow tubular structure-mediated facet synergy in CuS 通过空心管结构介导的cu小面协同作用增强Cu2+的电容性去离子

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-11 DOI: 10.1016/j.seppur.2026.136872

Yingjun Gao , Yinyan Guan , Jiyan Liang , Weichun Gao , Shengnan Chen , Xueyong Tian , Cong Geng

Copper sulfide (CuS) cathodes leveraged their homologous characteristics with Cu²⁺ to achieve targeted capture via hybrid capacitive deionization (HCDI), aiding copper remediation and resource recovery from industrial wastewater. Spherical, tubular, and lamellar CuS were constructed hydrothermally, revealing how morphology regulates key facet exposure. Spherical agglomeration shielded active facets, while lamellar stacking collapse compromised the hydrophobic (110) barrier, accelerating corrosion and reducing selectivity. Conversely, the hollow tubular structure fostered spatial synergy between hydrophobic (110) and reduction-active (102) facets. The dense sulfur packing on the (110) facet forms a hydrophobic barrier that inhibits H⁺ attack and sulfur dissolution in acid. Simultaneously, the high-density CuS dimer sites on the (102) facet drive the deep reduction of Cu²⁺ to Cu₂S. This synergy enabled a high adsorption capacity of 611.86 mg·g⁻¹ and > 90% selectivity amid coexisting heavy metals. Electrochemical analysis and post-cycling characterization confirmed that the interconnected tubular structure ensured efficient electron transport, while the optimized mass transfer pathways and stable interfacial environment collectively suppressed byproduct formation and electrode degradation. This study developed a new strategy for designing electrode materials capable of achieving high-capacity, high-selectivity copper removal and resource recovery from industrial wastewater characterized by strong acidity and multi-ion coexistence.

硫化铜（cu）阴极利用其与Cu2+的同源特性，通过混合电容去离子（HCDI）实现定向捕获，有助于工业废水中铜的修复和资源回收。球形、管状和片状cu是水热构建的，揭示了形态学如何调节关键关节面暴露。球形团聚层屏蔽了活性面，而层状堆积层坍塌破坏了疏水性（110）屏障，加速了腐蚀并降低了选择性。相反，空心管状结构促进了疏水性（110）和还原活性（102）面的空间协同作用。（110）表面的致密硫填料形成疏水屏障，抑制H+攻击和硫在酸中的溶解。同时，（102）表面高密度的cu二聚体位点驱动Cu2+深度还原为Cu2S。这种协同作用使其在共存的重金属中具有611.86 mg·g−1的高吸附容量和>； 90%的选择性。电化学分析和后循环表征证实，相互连接的管状结构确保了高效的电子传递，而优化的传质途径和稳定的界面环境共同抑制了副产物的形成和电极的降解。本研究提出了一种设计电极材料的新策略，能够实现强酸性、多离子共存的工业废水中高容量、高选择性的除铜和资源回收。

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引用次数: 0