Separation and Purification Technology最新文献_第3页

Hierarchical multilevel synergy of piezoelectricity-photocatalysis-defect engineering in ZnS for boosting peroxymonosulfate activation: A sustainable strategy for azo dye degradation 压电-光催化-缺陷工程在ZnS中促进过氧单硫酸盐活化的多层次协同作用：偶氮染料降解的可持续策略

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136561

Yingxi Zhu , Die Gao , Jia Zeng , Zhou Li , Deng Li , Dan Li , Xiaodan Hu , Jiahao Lin , Kezhi Liu , Jianming Wu , Dandan Wang

The persistent presence of refractory organic pollutants in aquatic ecosystems remains a global challenge, owing to their structural stability, bioaccumulation potential, and the toxicity of their transformation products. To address this issue, a hierarchical multilevel synergistic system (denoted as the ZP system) is constructed based on simple single-component ZnS coupled with peroxymonosulfate (PMS) for the efficient degradation of direct black G (DBG). This system integrates three synergistic mechanisms: piezoelectricity-photocatalysis-defect engineering synergy, catalyst-PMS activation synergy, and adsorption-degradation synergy. The cooperative process involves: (i) synergistic separation of photogenerated charges through the piezo-photocatalytic effect and sulfur vacancies (V_S) in ZnS; (ii) amplification via a ZnS-V_S-PMS interaction, where continuous electron consumption establishes a self-sustaining “excitation-depletion-re-excitation” cycle; and (iii) an adsorption-degradation cycle that enriches pollutants near active sites and regenerates adsorption sites during degradation. ZP system maintains high removal efficiency (>85 %) over a broad pH range (2–8). Moreover, ZP system achieves complete DBG removal within 20 min in various real water matrices (pond, tap, and river water) under the Xenon lamp irradiation, and exhibits a great application potential under natural sunlight and simulated flowing water. Compared with the original DBG, the toxicity of degradation products was significantly reduced, with the cell viability of 96.8 %. Radical trapping experiments and electron paramagnetic resonance spectroscopy identify h⁺, •SO₄⁻, •OH, and •O₂⁻ as the dominant reactive species. Moreover, the ZP system exhibits excellent biocompatibility with negligible hemolysis, underscoring its environmental friendliness. This work highlights the promise of a simple single-material-based multilevel synergy as a scalable, cost-effective, and adaptable strategy for sustainable water purification.

由于其结构稳定性、生物积累潜力和转化产物的毒性，难降解有机污染物在水生生态系统中的持续存在仍然是一个全球性的挑战。为了解决这一问题，以简单的单组分ZnS与过氧单硫酸根（PMS）偶联为基础，构建了一种高效降解直接黑G （DBG）的分层多层协同体系（简称ZP体系）。该系统集成了三种协同机制：压电-光催化-缺陷工程协同，催化剂- pms活化协同，吸附-降解协同。合作过程包括：(i)通过压电光催化效应和ZnS中的硫空位（VS）协同分离光生电荷；（ii）通过ZnS-VS-PMS相互作用进行放大，其中连续的电子消耗建立了一个自我维持的“激发-耗尽-再激发”循环；（iii）吸附-降解循环，在降解过程中富集活性位点附近的污染物并再生吸附位点。ZP体系在较宽的pH范围（2-8）内保持较高的去除率（> 85%）。此外，在氙灯照射下，ZP系统在各种实际水基质（池塘水、自来水和河水）中均能在20分钟内完全去除DBG，在自然光照和模拟流水条件下具有很大的应用潜力。与原DBG相比，降解产物的毒性显著降低，细胞存活率为96.8%。自由基捕获实验和电子顺磁共振谱分析表明，h+、•SO4−、•OH和•O2−是主要的反应物质。此外，ZP系统具有良好的生物相容性，溶血可以忽略不计，强调其环境友好性。这项工作强调了简单的基于单一材料的多层次协同作用作为可持续水净化的可扩展，具有成本效益和适应性的策略的前景。

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引用次数: 0

Numerical and experimental investigation of the compaction of suspended elastic-plastic microparticles in a centrifugal force field 离心力作用下弹塑性悬浮微粒压实的数值与实验研究

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136552

André Lier, Fabian Krull, Sergiy Antonyuk

Centrifuges are widely used in processes of particle technology to separate different phases based on density. During centrifugation, the sedimented particles can undergo plastic deformation, forming a compressible cake. However, the mechanisms governing cake compressibility, particularly the nonlinear distribution of porosity and stress induced by plastic deformation, remain insufficiently understood.In this study, the compaction behaviour of elastic-plastic microparticles during centrifugation was investigated through experiments and simulations using Computational Fluid Dynamics coupled with Discrete Element Method (CFD-DEM). Spherical paraffin particles with low-temperature-dependent mechanical properties have been produced to vary plastic deformation by changing their yield pressure via temperature in the centrifuge. Ethanol-based suspensions of these particles were centrifuged at varying rotational speeds and temperatures using an analytical photocentrifuge to investigate the interplay between particle mechanics and applied centrifugal forces. The resulting sediments were analysed via micro-computed tomography (μCT) to assess the porosity distribution within the compacted cake. To model particle bed formation, CFD-DEM simulations were performed using a multiphase solver incorporating liquid, gas and particle phases, along with centrifugal, Euler and Coriolis forces. An elastic-plastic contact model was employed in the DEM, with parameters such as Young's modulus and yield pressure obtained via single particle compression tests with a nanoindenter. Both experimental and simulation results demonstrated that increasing rotational speed and thus centrifugal force enhances sediment compaction, primarily driven by particle plastic deformation and significantly influenced by the radial pressure distribution, resulting in a nonlinear porosity profile within the particle bed.

离心机广泛应用于颗粒技术过程中，根据密度分离不同的相。在离心过程中，沉淀的颗粒会发生塑性变形，形成可压缩的饼。然而，控制饼可压缩性的机制，特别是由塑性变形引起的孔隙率和应力的非线性分布，仍然没有得到充分的了解。本文采用计算流体力学与离散元法（CFD-DEM）相结合的方法，通过实验和模拟研究了弹塑性微粒在离心过程中的压实行为。具有低温依赖力学性能的球形石蜡颗粒在离心机中通过温度改变其屈服压力来改变塑性变形。这些颗粒的乙醇基悬浮液在不同的转速和温度下使用分析光离心机进行离心，以研究颗粒力学和施加离心力之间的相互作用。通过微计算机断层扫描（μCT）对所得沉积物进行分析，以评估压实饼内的孔隙度分布。为了模拟颗粒床的形成，使用多相求解器进行了CFD-DEM模拟，包括液体、气体和颗粒相，以及离心、欧拉和科里奥利力。该模型采用弹塑性接触模型，通过纳米压头单颗粒压缩试验获得杨氏模量和屈服压力等参数。实验和模拟结果均表明，转速的增加和离心力的增加增强了沉积物的压实，这主要是由颗粒塑性变形驱动的，并受到径向压力分布的显著影响，导致颗粒床内的非线性孔隙率分布。

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引用次数: 0

A potential DES-driven membrane applied in electrodialysis coupled extraction for the ultra-high separation of 7Li isotopes 一种潜在的des驱动膜用于电渗析耦合萃取中7Li同位素的超高分离

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136545

Zhongxuan Sun, Zhiwan Li, Meiying Xie, Yongduo Sun, Liyan Xue, Xinyuan Lan, Fan Yang

In this work, a deep eutectic solvent (DES)-driven electrodialysis membrane material was constructed, with which an electrodialysis platform was first formed by coupling electrodialysis. Separation and enrichment of ⁷Li⁺ isotopes were carried out with the electrodialysis coupled extraction platform. Because of its lower binding energy barrier for forming complexes with ⁷Li⁺, a β-diketone-driven DES composed of tri-n-octyl phosphine oxide (TOPO) and 2-thenoyltrifluoroacetone (HTTA) was introduced to the separation and enrichment of ⁷Li⁺ isotopes. Furthermore, DES extractant was used to prepare supported liquid membranes (SLMs) because of its ability to drive extraction, its liquid state at room temperature and its good hydrogen bond network. Compared with the reported extraction systems, the separation coefficient of ⁷Li⁺/⁶Li⁺ (β_7Li/6Li) reaches 1.173 at an applied potential of 1.0 V, which is now the highest known β-value in these reported extraction systems. The Gibbs free energy change (∆G) of the electrodialysis coupled extraction process reaches −395.996 J·mol⁻¹, which explains the preferred extraction of ⁷Li⁺ isotopes. The competition and enhancement mechanisms between electromigration and extraction in electrodialysis coupled extraction were investigated by studying the Li⁺ concentration, separation coefficient of ⁷Li⁺/⁶Li⁺ and Gibbs free energy change of electrodialysis coupled extraction. The separation of ⁷Li⁺ isotopes via electrodialysis coupled extraction system has potential application in chemical engineering field.

本研究构建了一种深共晶溶剂（DES）驱动的电渗析膜材料，并首次通过耦合电渗析形成了电渗析平台。采用电渗析耦合萃取平台对7Li+同位素进行分离富集。由于与7Li+形成配合物的结合能垒较低，采用β-二酮驱动的由三正辛烷基氧化膦（TOPO）和2-烯酰三氟丙酮（HTTA）组成的DES用于7Li+同位素的分离和富集。此外，由于DES萃取剂具有驱动萃取的能力、室温下的液态状态以及良好的氢键网络，因此将其用于制备支撑液膜（SLMs）。与已有的萃取体系相比，在1.0 V的作用电位下，7Li+/6Li+ (β7Li/6Li)的分离系数达到1.173，是目前已知的萃取体系中最高的β值。电渗析耦合萃取过程的吉布斯自由能变化∆G达到−395.996 J·mol−1，说明7Li+同位素优先萃取。通过对电渗析耦合萃取中Li+浓度、7Li+/6Li+分离系数和吉布斯自由能变化的研究，探讨了电迁移与萃取在电渗析耦合萃取中的竞争与增强机制。电渗析耦合萃取系统分离7Li+同位素在化工领域具有潜在的应用前景。

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引用次数: 0

Silver nanoparticles loaded pyrazole-based hypercrosslinked microporous polymer for the effective separation of Xe/Kr 纳米银负载吡唑基超交联微孔聚合物用于Xe/Kr的有效分离

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136554

Geng Chen, Mengying Wei, Mengjie Jing, Rui Zhang, Zhe Wang, Yifan Li, Yingsi Huo, Keliang Shi, Tonghuan Liu, Kang Kang

The separation of xenon (Xe) and krypton (Kr) from gaseous mixtures is a crucial yet challenging industrial process, primarily due to the inherent inertness and similar physicochemical properties. Herein, we report the synthesis of a novel pyrazole-based microporous organic polymer for efficient Xe/Kr separation. This porous organic polymer possesses abundant nitrogen sites and a concentrated microporous network with pore sizes predominantly centered within the 4–6 Å range. The material exhibited promising Xe adsorption capacity (2.22 mmol·g⁻¹) and Xe/Kr Ideal Adsorbed Solution Theory (IAST) selectivity (13.74) at 298 K and 1.0 bar. Furthermore, taking advantage of the strong coordination interactions between the pyrazole groups and metal nanoparticles, silver nanoparticles were successfully introduced to form the composite MOP-PZ-Ag, thereby improving the Xe/Kr separation capability. Under dilute conditions, MOP-PZ-Ag exhibited significantly higher IAST selectivity and Henry's coefficient for Xe compared with MOP-PZ. In dynamic breakthrough experiments, MOP-PZ-Ag showed better separation performance toward Xe/Kr, with the Xe adsorption capacity increasing from 3.79 mmol·kg⁻¹ to 4.91 mmol·kg⁻¹ under low concentration (400 ppm Xe and 40 ppm Kr in dry air). Besides, the superior separation performance of MOP-PZ-Ag can be well maintained over at least five adsorption-desorption cycles. Such experiment results revealed the potential of MOP-PZ-Ag for Xe/Kr separation in used nuclear fuel (UNF) off-gas management.

从气体混合物中分离氙（Xe）和氪（Kr）是一个关键但具有挑战性的工业过程，主要是由于固有的惰性和相似的物理化学性质。在此，我们报道了一种新型的吡唑基微孔有机聚合物的合成，用于Xe/Kr的高效分离。这种多孔有机聚合物具有丰富的氮位点和集中的微孔网络，孔径主要集中在4-6 Å范围内。该材料在298 K和1.0 bar下具有良好的Xe吸附量（2.22 mmol·g−1）和Xe/Kr理想吸附溶液理论（IAST）选择性（13.74）。此外，利用吡唑基团与金属纳米粒子之间的强配位相互作用，成功地引入了银纳米粒子，形成了复合的MOP-PZ-Ag，从而提高了Xe/Kr的分离能力。在稀释条件下，MOP-PZ- ag对Xe的选择性和Henry’s系数显著高于MOP-PZ。在动态突破实验中，MOP-PZ-Ag对Xe/Kr表现出较好的分离性能，在低浓度（400 ppm Xe和40 ppm Kr）条件下，对Xe的吸附量从3.79 mmol·kg−1增加到4.91 mmol·kg−1。此外，MOP-PZ-Ag优异的分离性能可以在至少5个吸附-解吸循环中保持。这些实验结果揭示了mopp - pz - ag在乏燃料（UNF）废气管理中Xe/Kr分离的潜力。

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引用次数: 0

Three-dimensional CFD–PBM insights into bubble dynamics and interfacial momhentum transfer in bubble columns 三维CFD-PBM对气泡动力学和气泡柱界面动量传递的见解

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136527

Jin Liang, Haochuan Xiong, Zhehao Hu, Dihao Xie, Honggang Zhang, Zhanghao Wan

Bubble columns are widely used gas-liquid contactors in chemical and biochemical processes, where complex interfacial forces necessitate an investigation of multiphase hydrodynamics along with bubble coalescence and breakup phenomena. This work analyzes the dependence of mesoscopic bubble behavior and microscopic forces on fluid properties under a nonlinear turbulence using an Eulerian-Eulerian model coupled with a population balance model (PBM). This model incorporates drag and other interfacial momentum exchange mechanisms. Following quantitative validation, the bubble dynamics and interfacial momentum transfer within the bubble column are numerically investigated with respect to the effects of superficial gas velocity, surface tension, and initial bubble inlet diameter. The results reveal a strong temporal coupling between the instantaneous drag variation and the periodic oscillation of the bubble plume. An inverse relationship is observed between bubble diameter and drag force together with the vertical drag component exceeding horizontal components by nearly two orders of magnitude during plume stabilization. Increasing surface tension suppresses bubble breakup and reduces turbulent kinetic energy (TKE), leading to a more stable plume structure. An initial bubble diameter of 2.35 mm achieves optimal liquid velocity and TKE. By explicitly resolving the temporal evolution of interfacial forces and the coupling with plume dynamics, this study provides new insights into the nonlinear nature of momentum transfer in bubble-driven flows under varying fluid properties.

气泡柱是化学和生化过程中广泛使用的气液接触器，其复杂的界面力要求研究气泡聚结和破裂的多相流体力学现象。本文采用欧拉-欧拉模型结合种群平衡模型（PBM）分析了非线性湍流条件下介观气泡行为和微观力对流体性质的依赖关系。该模型结合了阻力和其他界面动量交换机制。在定量验证之后，对气泡柱内的气泡动力学和界面动量传递进行了数值研究，考虑了表面气体速度、表面张力和初始气泡入口直径的影响。结果表明，瞬时阻力变化与气泡羽流的周期振荡之间存在较强的时间耦合。在羽流稳定过程中，气泡直径与阻力呈反比关系，且垂直阻力分量超过水平阻力分量近两个数量级。表面张力的增加抑制了气泡破裂，降低了湍流动能（TKE），导致羽流结构更加稳定。初始气泡直径为2.35 mm时，液体流速和TKE最佳。通过明确地解析界面力的时间演化以及与羽流动力学的耦合，本研究为不同流体性质下气泡驱动流动中动量传递的非线性特性提供了新的见解。

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引用次数: 0

Spray pyrolysis for effective detoxification of organotin waste and in situ synthesis of high-purity SnO₂ nanoparticles 喷雾热解有效解毒有机锡废物和原位合成高纯度SnO纳米颗粒

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136551

Zijian Su , Qijie Guo , Bin Lei , Qiuyu Li , Wei Lv , Peng Du , Yuanbo Zhang

Organotin waste (OTW) comprises refractory, tin-bearing hazardous materials with high biotoxicity, yet its tin content often exceeds that of primary ores, presenting an opportunity for resource recovery. In this study, a novel spray pyrolysis process was developed to enable the economical and efficient treatment of OTW. The transformation behavior and detoxification mechanisms of hazardous elements (C, N, and S) were systematically investigated. The results demonstrated that the pyrolysis of OTW was accelerated at higher pyrolysis temperatures and under an optimized air excess ratio (AER), which promoted the removal of C, N, and S. After optimization, carbon was completely oxidized to CO₂, while hazardous SO₂ and NOₓ emissions were relatively low. Furthermore, the residual C, N, and S in the solid products were reduced to <0.002 wt%, achieving almost complete elimination. The recovery rate and purity of SnO₂ nanoparticles (average size: 35 nm) formed in situ via the vapor–solid (VS) mechanism reached 99.46 % and 99.17 %, respectively, achieving high-purity tin recovery.

有机锡废物（OTW）是一种具有高生物毒性的难降解、含锡危险物质，但其锡含量往往超过原生矿石，为资源回收提供了机会。为了经济高效地处理OTW，本研究开发了一种新型的喷雾热解工艺。系统地研究了有害元素C、N、S的转化行为和解毒机制。结果表明，在较高的热解温度和优化的空气过剩比（AER）下，OTW的热解速度加快，促进了C、N和s的去除。优化后，碳被完全氧化为CO 2，而有害的SO 2和NOₓ排放量相对较低。固体产物中C、N、S的残留量降至0.002 wt%，几乎完全消除。通过气固（VS）机制原位生成的SnO₂纳米颗粒（平均尺寸为35 nm）的回收率和纯度分别达到99.46%和99.17%，实现了高纯度锡的回收。

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引用次数: 0

E-peroxone synergizes membrane distillation for treatment of organic-laden RO concentrate: Molecular weight-dependent fouling control and process stability e -过氧酮协同膜蒸馏处理含有机反渗透浓缩物：分子量依赖性污染控制和过程稳定性

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136544

Huijiao Wang , Haolin Li , Yanyu Cui , Weiwang Liu , Zhilin Zhang , Qiang Guo , Ruiping Liu , Erzhuo Zhao

Industrial reverse osmosis concentrate (ROC) from coal chemical wastewater is typically laden with refractory organic contaminants, especially humic substances, posing a major bottleneck for zero liquid discharge. This study systematically evaluated three pretreatment processes (electro-oxidation (E), ozonation (O₃), and the E-peroxone (EP)) to remove these organics from ROC and mitigate membrane fouling during subsequent membrane distillation (i.e., E-MD, O₃-MD, and EP-MD). Results show that pretreatment strategies significantly influenced the performance and fouling behavior of subsequent MD. Due to the ineffective removal of total organic carbon (TOC, 6 % after 3 h electro-oxidation), E-MD witnessed 75 % water flux decline at a water recovery rate of 78 %. O₃-MD suffered from a sharp flux decline shortly after initiation because of the ineffective ozonation of organics with low molecular weight (MW). In contrast, by effectively degrading organics across a wide MW range, the EP-MD process exhibited the highest water flux (3.5–5.9 times of other processes) and the shortest time (22.5 h vs. 30–34 h) to achieve 78 % water recovery, demonstrating the most effective membrane fouling control. Further characterization and theoretical analysis elucidated the MW-dependent fouling mechanisms, that is, higher-MW organics are prone to form porous fouling layer, while lower-MW fractions preferentially complex with scaling ions to form blocky crystal-organic fouling. Finally, cycle tests demonstrate that the EP-MD system, complemented by periodic HCl cleaning, maintained robust stability over five cycles, highlighting its great potential as a viable and efficient strategy for integrated ROC treatment and resource recovery.

煤化工废水的工业反渗透浓缩物通常含有难降解的有机污染物，特别是腐殖质物质，是实现零液体排放的主要瓶颈。该研究系统地评估了三种预处理工艺(电氧化（E)、臭氧化（O₃）和E-过氧酮（EP））从ROC中去除这些有机物，并在随后的膜蒸馏（即E- md、O3-MD和EP- md）中减轻膜污染。结果表明，预处理策略对后续MD的性能和污染行为有显著影响。由于电氧化3 h后总有机碳（TOC, 6%）去除效果不显著，E-MD的水通量下降75%，水回收率为78%。由于低分子量有机物的臭氧化效果不佳，O3-MD在启动后不久通量急剧下降。相比之下，EP-MD工艺通过在较宽的MW范围内有效降解有机物，表现出最高的水通量（是其他工艺的3.5-5.9倍）和最短的时间（22.5 h对30-34 h），达到78%的水回收率，证明了最有效的膜污染控制。进一步的表征和理论分析阐明了分子量依赖的结垢机理，即高分子量有机物容易形成多孔结垢层，而低分子量有机物优先与结垢离子络合形成块状结晶有机结垢。最后，循环测试表明，EP-MD系统，辅以定期的HCl清洗，在五个循环中保持了强大的稳定性，突出了其作为综合ROC处理和资源回收的可行和有效策略的巨大潜力。

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引用次数: 0

Ulva biochar-anchored ZnO/ZnFe2O4 heterojunctions for enhanced piezoelectric degradation of PFOA for water remediation Ulva生物炭锚定ZnO/ZnFe2O4异质结增强压电降解PFOA的水修复

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136548

Hua Jing, Haojia Zhu, Yafei Pei, Daoqiong Zheng, Ke Zhang

Harnessing mechanical energy for environmental remediation via piezo-catalysis offers a promising pathway, yet challenges like insufficient reactive oxygen species (ROS) generation, low mass transfer efficiency, and poor recovery rates remain. Herein, a novel Z-scheme piezo-catalyst, ZnO/ZnFe₂O₄@UBC, was successfully constructed by confining ZnO/ZnFe₂O₄ heterojunctions within the hierarchical porous structure of Ulva biochar (UBC). Under ultrasonic vibration, ZnO/ZnFe₂O₄@UBC achieved 96.7 % degradation of PFOA within 4 h. Importantly, the catalyst maintained stable piezo-catalytic performance across a wide pH range (2.68–10.68) and in the presence of common inorganic anions (Cl⁻, HCO₃⁻, NO₃⁻, HPO₃²⁻, SO₃²⁻) as well as natural organic matter (humic acid). Even under complex water matrices, ZnO/ZnFe₂O₄@UBC exhibited excellent durability and reusability, maintaining a high PFOA removal efficiency of 72.7 % after ten consecutive cycles, alongside facile magnetic separation. This study highlights the potential of Ulva biochar confined heterojunctions for efficient PFOA degradation, providing a sustainable strategy for remediating a representative persistent PFAS pollutant in realistic aqueous environments.

利用机械能通过压电催化进行环境修复提供了一条很有前景的途径，但仍存在活性氧（ROS）生成不足、传质效率低、回收率低等挑战。本文通过将ZnO/ZnFe2O4异质结限制在Ulva生物炭（UBC）的层次化多孔结构内，成功构建了一种新型Z-scheme压电催化剂ZnO/ZnFe2O4@UBC。在超声振动下，ZnO/ZnFe2O4@UBC在4 h内对PFOA的降解率达到96.7 %。重要的是，该催化剂在较宽的pH范围（2.68-10.68）和常见无机阴离子（Cl−,HCO3−,NO3−,HPO32−,SO32−）以及天然有机物（腐植酸）存在下保持稳定的压电催化性能。即使在复杂的水基质下，ZnO/ZnFe2O4@UBC也表现出优异的耐久性和可重复使用性，在连续10次循环后保持72.7 %的PFOA去除效率，同时易于磁分离。本研究强调了Ulva生物炭约束异质结对PFOA有效降解的潜力，为修复现实水环境中具有代表性的持久性PFAS污染物提供了一种可持续的策略。

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引用次数: 0

In situ construction of metal–phenolic networks in chitosan/polyvinyl alcohol (CS/PVA) hydrogel beads for efficient tetracycline hydrochloride removal with recyclability from complex water systems 壳聚糖/聚乙烯醇（CS/PVA）水凝胶珠中金属-酚网络的原位构建及其在复杂水系统中高效脱除盐酸四环素的可回收性

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136567

Jiahao Wu, Huiping Zeng, Fanhao Meng, Yating Zhao, Dong Li, Jie Zhang

The widespread occurrence of antibiotic residues in aquatic environments has become a major water pollution concern, posing ecological risks and accelerating antimicrobial resistance. Metal–phenolic networks (MPNs), eco-friendly functional materials formed via coordination between natural polyphenols and metal ions, exhibit broad application potential in environmental remediation. In this study, a novel composite adsorbent (FTN@CS/PVA) was fabricated by uniformly immobilizing MPN structures within a three-dimensional porous chitosan/polyvinyl alcohol (CS/PVA) gel beads through the in situ coordination of Fe³⁺ and tannic acid (TA). The resulting material exhibited excellent adsorption performance toward tetracycline hydrochloride (TCH), achieving a maximum adsorption capacity of 95.5 mg/g at 298 K and pH 3. The adsorption process followed the pseudo-second-order kinetic model (R² = 0.9963) and the Redlich–Peterson isotherm model (R² = 0.9736). The primary adsorption mechanisms involved synergistic physicochemical interactions, including hydrogen bonding, Fe single bond

O coordination, and electron transfer. Notably, FTN@CS/PVA also exhibited high adsorption efficiency toward various dyes and maintained excellent competitive and selective adsorption performance even in a TC–MB binary system. Furthermore, FTN@CS/PVA retained high TCH removal efficiency in real water matrices (lake water, domestic wastewater, and secondary effluent from a wastewater treatment plant) and in complex systems containing various coexisting anions or humic acid (HA), demonstrating superior interference resistance and environmental adaptability. In addition, FTN@CS/PVA demonstrated structural stability and excellent regenerability, maintaining over 80 % of its adsorption capacity after three adsorption–desorption cycles in the presence of humic acid (HA). This study provides a novel design strategy and theoretical foundation for developing highly stable and selective MPN-based composite adsorbents for the efficient removal of antibiotic contaminants.

抗生素残留在水生环境中的广泛存在已成为水污染的主要问题，造成生态风险并加速抗生素耐药性。金属-酚网络是天然多酚类物质与金属离子协同形成的环保功能材料，在环境修复中具有广阔的应用潜力。在本研究中，通过Fe3+和单宁酸（TA）的原位配位，在三维多孔壳聚糖/聚乙烯醇（CS/PVA）凝胶珠内均匀固定MPN结构，制备了一种新型复合吸附剂（FTN@CS/PVA）。所得材料对盐酸四环素（TCH）具有优异的吸附性能，在298 K和 3 pH条件下，最大吸附量为95.5 mg/g。吸附过程符合拟二级动力学模型（R2 = 0.9963）和Redlich-Peterson等温线模型（R2 = 0.9736）。主要吸附机制包括氢键、FeO配位和电子转移等物理化学协同作用。值得注意的是，FTN@CS/PVA对各种染料也表现出较高的吸附效率，即使在TC-MB二元体系中也保持了优异的竞争和选择性吸附性能。此外，FTN@CS/PVA在真实的水基质（湖水、生活废水和污水处理厂的二级出水）和含有多种阴离子或腐殖酸（HA）共存的复杂系统中保持了高TCH去除效率，表现出卓越的抗干扰性和环境适应性。此外，FTN@CS/PVA表现出结构稳定性和良好的可再生性，在腐植酸（HA）存在下，经过三次吸附-解吸循环后，其吸附容量保持在80% %以上。本研究为开发高稳定性、高选择性的mpn基复合吸附剂高效去除抗生素污染物提供了新的设计策略和理论基础。

{"title":"In situ construction of metal–phenolic networks in chitosan/polyvinyl alcohol (CS/PVA) hydrogel beads for efficient tetracycline hydrochloride removal with recyclability from complex water systems","authors":"Jiahao Wu, Huiping Zeng, Fanhao Meng, Yating Zhao, Dong Li, Jie Zhang","doi":"10.1016/j.seppur.2025.136567","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136567","url":null,"abstract":"The widespread occurrence of antibiotic residues in aquatic environments has become a major water pollution concern, posing ecological risks and accelerating antimicrobial resistance. Metal–phenolic networks (MPNs), eco-friendly functional materials formed via coordination between natural polyphenols and metal ions, exhibit broad application potential in environmental remediation. In this study, a novel composite adsorbent (FTN@CS/PVA) was fabricated by uniformly immobilizing MPN structures within a three-dimensional porous chitosan/polyvinyl alcohol (CS/PVA) gel beads through the in situ coordination of Fe3+ and tannic acid (TA). The resulting material exhibited excellent adsorption performance toward tetracycline hydrochloride (TCH), achieving a maximum adsorption capacity of 95.5 mg/g at 298 K and pH 3. The adsorption process followed the pseudo-second-order kinetic model (R2 = 0.9963) and the Redlich–Peterson isotherm model (R2 = 0.9736). The primary adsorption mechanisms involved synergistic physicochemical interactions, including hydrogen bonding, Fe<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O coordination, and electron transfer. Notably, FTN@CS/PVA also exhibited high adsorption efficiency toward various dyes and maintained excellent competitive and selective adsorption performance even in a TC–MB binary system. Furthermore, FTN@CS/PVA retained high TCH removal efficiency in real water matrices (lake water, domestic wastewater, and secondary effluent from a wastewater treatment plant) and in complex systems containing various coexisting anions or humic acid (HA), demonstrating superior interference resistance and environmental adaptability. In addition, FTN@CS/PVA demonstrated structural stability and excellent regenerability, maintaining over 80 % of its adsorption capacity after three adsorption–desorption cycles in the presence of humic acid (HA). This study provides a novel design strategy and theoretical foundation for developing highly stable and selective MPN-based composite adsorbents for the efficient removal of antibiotic contaminants.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":"136567"},"PeriodicalIF":8.6,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145801502","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

CaO2-integrated hydrogel with high O22− content and mechanical property for sustainable water disinfection 具有高O22−含量和高机械性能的水凝胶

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-18 DOI: 10.1016/j.seppur.2025.136549

Xiuling Li, Chaoran Zhang, Qiuju Zheng, Peng Wang, Guangwu Wen, Zhihui Niu, Xiaowei Li

Currently, most of the nanomaterial-based disinfection technologies are highly dependent on the input of external energy. Developing convenient strategy with low energy consumption and high efficiency for sustainable water disinfection still remains challenging. Herein, a high-purity CaO₂ nanoparticle with ultra-high peroxide ion (O₂²⁻) content was synthesized by regulation and control of the synthesis process parameters. The modulation of O₂²⁻ content, stability and release kinetics was systematically investigaed. As a result, the purity of the synthesized CaO₂ was improved up to 99.04 %, with a yield as high as 99.1 %, which is extremely close to the maximum theoretical value. Compared to other reported metal peroxides, the as prepared CaO₂ exhibits the fastest H₂O₂ release kinetics (K = 0.01898) and superior antibacterial performance against multiple bacterial strains at low concentrations. CaO₂-integrated hydrogel (PSCS-CaO₂) was further designed with mechanical strength up to 1.68 MPa, which surpassed the values reported in literatures. PSCS-0.2CaO₂ (containing 0.2 %w/v CaO₂) maintained excellent disinfection efficacy even after 20 consecutive reuse cycles, demonstrating outstanding stability and reusability. Thus, this work provides a convenient and environmentally friendly strategy with low energy consumption and high efficiency for sustainable water disinfection.

目前，大多数基于纳米材料的消毒技术高度依赖外部能量的输入。开发低能耗、高效率、便捷的可持续水消毒策略仍然是一个挑战。本文通过对合成工艺参数的调控，合成了具有超高过氧化氢离子（O22−）含量的高纯氧化钙纳米颗粒。系统地研究了O22−含量的调节、稳定性和释放动力学。结果表明，合成的CaO2纯度提高到99.04%，收率高达99.1%，非常接近理论值最大值。与已有报道的其他金属过氧化物相比，制备的CaO2在低浓度下具有最快的H2O2释放动力学（K = 0.01898）和对多种细菌的良好抑菌性能。进一步设计了聚氧化钙水凝胶（PSCS-CaO2），其机械强度达到1.68 MPa，超过了文献报道的数值。PSCS-0.2CaO2（含0.2% w/v CaO2）在连续重复使用20次后仍保持良好的消毒效果，表现出出色的稳定性和可重复使用性。因此，本研究为水的可持续消毒提供了一种方便、环保、低能耗、高效率的策略。

{"title":"CaO2-integrated hydrogel with high O22− content and mechanical property for sustainable water disinfection","authors":"Xiuling Li, Chaoran Zhang, Qiuju Zheng, Peng Wang, Guangwu Wen, Zhihui Niu, Xiaowei Li","doi":"10.1016/j.seppur.2025.136549","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136549","url":null,"abstract":"Currently, most of the nanomaterial-based disinfection technologies are highly dependent on the input of external energy. Developing convenient strategy with low energy consumption and high efficiency for sustainable water disinfection still remains challenging. Herein, a high-purity CaO2 nanoparticle with ultra-high peroxide ion (O22−) content was synthesized by regulation and control of the synthesis process parameters. The modulation of O22− content, stability and release kinetics was systematically investigaed. As a result, the purity of the synthesized CaO2 was improved up to 99.04 %, with a yield as high as 99.1 %, which is extremely close to the maximum theoretical value. Compared to other reported metal peroxides, the as prepared CaO2 exhibits the fastest H2O2 release kinetics (K = 0.01898) and superior antibacterial performance against multiple bacterial strains at low concentrations. CaO2-integrated hydrogel (PSCS-CaO2) was further designed with mechanical strength up to 1.68 MPa, which surpassed the values reported in literatures. PSCS-0.2CaO2 (containing 0.2 %w/v CaO2) maintained excellent disinfection efficacy even after 20 consecutive reuse cycles, demonstrating outstanding stability and reusability. Thus, this work provides a convenient and environmentally friendly strategy with low energy consumption and high efficiency for sustainable water disinfection.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"48 1","pages":"136549"},"PeriodicalIF":8.6,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145801504","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