Separation and Purification Technology最新文献_第10页

Engineering a nanofiltration membrane with high mono-/divalent anion selectivity and antifouling properties via L-histidine incorporation 通过l -组氨酸掺入，设计一种具有高单/二价阴离子选择性和防污性能的纳滤膜

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136851

Ruohan Liang , Dongsheng Zhao , Fangming Jin , Jun Xu , Guicai Liu

The limited mono−/divalent anion selectivity and inadequate antifouling properties of polyamide (PA) nanofiltration (NF) membranes restrict their use in water treatment. Herein, L-histidine (L-His)-modified NF membranes were prepared through interfacial polymerization on a polyethersulfone porous substrate. The aqueous-phase comonomers were piperazine and L-His, which contain both amino and carboxyl groups, while the organic-phase monomer was trimesoyl chloride. Compared with the NF0 membrane without addition of L-His, all of the L-His-modified membrane was characterized by a higher surface roughness, a thinner PA layer, greater hydrophilicity, a more negative surface charge and a larger mean pore size. Among them, the optimal NF0.5 membrane with the addition of 0.5% (w/v) L-His demonstrated a pure water permeability of 17.9 L/(m²·h·bar) and a 2.7-fold higher NaCl/Na₂SO₄ selectivity (up to 102.0). In particular, the NaCl/Na₂SO₄ selectivity improved with higher operating pressure, but decreased with increasing single-salt concentration or NaCl/Na₂SO₄ mass ratio in the feed solution. In addition, the NF0.5 membrane demonstrated superior resistance to protein fouling and outstanding long-term operational stability throughout a continuous 7-day filtration process. This study could provide valuable insights into the development of NF membranes with high mono−/divalent anion selectivity and excellent antifouling properties.

聚酰胺（PA）纳滤（NF）膜有限的单/二价阴离子选择性和不充分的防污性能限制了其在水处理中的应用。在聚醚砜多孔基质上，采用界面聚合法制备了l -组氨酸修饰的NF膜。水相单体为哌嗪和L-His，它们同时含有氨基和羧基，而有机相单体为三甲基氯。与未添加L-His的NF0膜相比，L-His修饰的膜表面粗糙度更高，PA层更薄，亲水性更强，表面负电荷更多，平均孔径更大。其中，添加0.5% (w/v) L- his的NF0.5膜的纯水渗透率为17.9 L/(m2·h·bar)， NaCl/Na2SO4选择性提高2.7倍（达102.0）。NaCl/Na2SO4的选择性随操作压力的增加而提高，但随进料溶液中单盐浓度或NaCl/Na2SO4质量比的增加而降低。此外，NF0.5膜在连续7天的过滤过程中表现出优异的抗蛋白质污染能力和出色的长期运行稳定性。该研究为开发具有高单/二价阴离子选择性和优异防污性能的纳滤膜提供了有价值的见解。

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引用次数: 0

Recovery of lead and fluorine from non-ferrous smelting acid sludge by synergistic leaching and stepwise precipitation 协同浸出-分步沉淀法回收有色冶炼酸泥中的铅和氟

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136793

Ziyuan Liu , Xiaoguang Zhang , Zhe Tan , De'an Pan , Guosai Jiang

Acid sludge, a hazardous waste from lead (Pb) and zinc (Zn) smelting process, commonly contains low-boiling-point elements such as Pb and fluorine (F). However, the complex phase composition of acid sludge typically results in low recovery efficiencies of Pb and F. Herein, we proposed an efficient recovery method for Pb and F through synergistic leaching using a solution containing aluminum ions (Al³⁺) and chloride ions (Cl⁻) followed by stepwise precipitation involving PbCl₂ cooling crystallization and cryolite formation. The single-factor experiment results showed the leaching efficiencies of 98.37% and 92.35% for Pb and F, respectively, which is superior to that of the separate leaching of Pb or F process, due to the intermingle structure of Pb and F phases in acid sludge. The precipitation efficiencies reached 94.44% for Pb and 97.88% for F, and the obtained PbCl₂ and cryolite products meet national standards. Density functional theory (DFT) calculations revealed the chemical states of Al³⁺, calcium ion (Ca²⁺), and F⁻ in leaching solution and their coexistence mechanism, and thermodynamic analysis clarified the preferential precipitation of cryolite with high quality. Further, the Life Cycle Assessment (LCA) and economic evaluation were conducted for the entire recovery process, indicating the significantly economic and environmental benefits with a cost of only ¥1.61 for treating 100 g of acid sludge. This study provides an efficient and sustainable method for recovering Pb and F from acid sludge, which not only mitigates environmental hazards but also enhances resource valorization, thereby supporting the development of a circular economy in the non-ferrous metal industry.

酸性污泥是铅（Pb）和锌（Zn）冶炼过程产生的危险废物，通常含有低沸点元素，如Pb和氟(F)。然而，酸性污泥的复杂相组成通常导致Pb和F的回收效率较低。为此，我们提出了一种高效的Pb和F回收方法，即使用含有铝离子（Al3+）和氯离子（Cl−）的溶液进行协同浸出，然后通过PbCl2冷却结晶和冰晶石形成的逐步沉淀。单因素试验结果表明，由于酸性污泥中Pb和F相的混合结构，Pb和F的浸出效率分别为98.37%和92.35%，优于单独浸出Pb或F的工艺。Pb的沉淀效率为94.44%，F的沉淀效率为97.88%，所得的PbCl2和冰晶石产品均达到国家标准。密度泛函理论（DFT）计算揭示了浸出液中Al3+、钙离子（Ca2+）和F−的化学态及其共存机理，热力学分析明确了高质量冰晶石的优先沉淀。对整个回收过程进行了生命周期评价（LCA）和经济评价，表明处理100 g酸污泥的成本仅为1.61元，具有显著的经济效益和环境效益。本研究为从酸性污泥中回收铅和F提供了一种高效、可持续的方法，既减轻了环境危害，又提高了资源价值，从而支持有色金属工业循环经济的发展。

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引用次数: 0

Highly stable SiO2-ZrO2 hollow fiber membrane via phase-transformation derived α-Al2O3 interlayer for nanofiltration under extreme conditions 高稳定的SiO2-ZrO2中空纤维膜通过相变衍生α-Al2O3中间层用于极端条件下的纳滤

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136849

Beibei Liu, Zhigang Wang, Xiaoyao Tan

Compared to organic nanofiltration (NF) membranes, ceramic NF membranes exhibit higher stability under harsh conditions such as extreme pH and elevated temperatures. γ-Al₂O₃ is commonly employed as an interlayer in multilayer ceramic NF membranes, but it is restricted to relatively mild conditions. In this study, on a macroporous alumina hollow fiber support, a boehmite sol coating is transformed from γ-Al₂O₃ to α-Al₂O₃ at a reduced phase-transformation temperature under the induction of TiO₂, forming a uniform ultrafiltration interlayer for the fabrication of SiO₂-ZrO₂ separation layer in a single step. By dual regulating the TiO₂ doping content in boehmite sol and sintering temperatures, the resulting SiO₂-ZrO₂/α-Al₂O₃ NF membrane with a pore size of 1.4 nm demonstrates extended stability across a wide pH range of 1–13 under elevated temperatures. During the long-term dynamic textile wastewater treatment test, it maintains stable permeance and selectivity for over 24 h at pH 2/12 under 60 °C, significantly outperforming γ-Al₂O₃-supported SiO₂-ZrO₂ membranes. Meanwhile, it displays a permeance of up to 18 LMH/bar and superior dye desalination performance (CR: 99.23%, NaCl <12%). This optimization strategy not only enhances the stability of SiO₂-ZrO₂ NF membranes with the aid of an α-Al₂O₃ interlayer but also provides a simplified route for their fabrication.

与有机纳滤（NF）膜相比，陶瓷纳滤膜在极端pH值和高温等恶劣条件下表现出更高的稳定性。γ-Al2O3通常用作多层陶瓷NF膜的中间层，但仅限于相对温和的条件。在本研究中，在大孔氧化铝中空纤维支架上，在TiO2的诱导下，薄水铝石溶胶涂层在降低的相变温度下由γ-Al2O3转变为α-Al2O3，形成均匀的超滤中间层，一步制备SiO2-ZrO2分离层。通过对薄水铝石溶胶中TiO2掺杂量和烧结温度的双重调节，得到了孔径为1.4 nm的SiO2-ZrO2/α-Al2O3滤膜，在较高的温度下，在1-13的pH范围内具有较好的稳定性。在长期的纺织废水动态处理试验中，在60°C下，在pH 2/12条件下，它保持了超过24 h的稳定的渗透和选择性，明显优于γ- al2o3负载的SiO2-ZrO2膜。同时，它具有高达18 LMH/bar的渗透性能和优异的染料脱盐性能（CR: 99.23%, NaCl <12%）。该优化策略不仅提高了α-Al2O3中间层SiO2-ZrO2 NF膜的稳定性，而且为其制备提供了简化的途径。

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引用次数: 0

Two-dimensional Mg-ZIF nanosheets loaded with multistage porous carbon for efficient ammonia nitrogen adsorption via interfacial hydrogen bonding 负载多级多孔碳的二维Mg-ZIF纳米片通过界面氢键高效吸附氨氮

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136814

Xingyu Yang , Xu Liu , Boxing An , Hanwen Cui , Handong Leng , Penghui Wu , Ziyan Wang , Keke Li , Kangjun Wang , Yushan Li

A novel zeolite adsorbent with high ammonia nitrogen (NH₄⁺-N) adsorption capacity was successfully prepared by in situ growth of zeolite imidazole framework (ZIF) on oil sludge pyrolysis carbon(OSPC) residue as the carrier. Static experiments demonstrated that the adsorbent achieved a maximum adsorption capacity of 216.9 mg·g⁻¹ at pH = 8.0, which is significantly superior to that of conventional adsorbents. The adsorption mechanism was systematically investigated using Zeta potential, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT), revealing a multi-layer adsorption process involving electrostatic attraction, hydrogen bonding, and van der Waals forces. Combined with kinetic and thermodynamic analysis, the dynamic adsorption behavior of the material under different initial NH₄⁺-N concentration, ion interference, dosage and temperature was elucidated. Furthermore, Aspen modeling was employed to optimize practical process parameters. This study not only realizes the high-value utilization of petroleum pyrolysis residue through multi-dimensional structural and functional design but also provides a theoretical foundation and technical support for developing advanced metal-organic framework (MOF) composite materials with high adsorption performance. The work effectively addresses the challenge of NH₄⁺-N pollution removal while pioneering an innovative pathway for designing high-performance environmental adsorption materials.

以油泥热解碳（OSPC）渣为载体，原位生长咪唑骨架（ZIF）分子筛，成功制备了一种具有高氨氮（NH4+-N）吸附能力的新型沸石吸附剂。静态实验表明，在pH = 8.0时，该吸附剂的最大吸附量为216.9 mg·g−1，明显优于常规吸附剂。利用Zeta电位、x射线光电子能谱（XPS）和密度泛函理论（DFT）对吸附机理进行了系统研究，揭示了一个涉及静电吸引、氢键和范德华力的多层吸附过程。结合动力学和热力学分析，阐明了材料在不同初始NH4+-N浓度、离子干扰、投加量和温度下的动态吸附行为。利用Aspen模型对实际工艺参数进行优化。本研究不仅通过多维度的结构和功能设计实现了石油热解渣油的高价值利用，而且为开发具有高吸附性能的先进金属-有机骨架（MOF）复合材料提供了理论基础和技术支持。该工作有效地解决了NH₄+-N污染去除的挑战，同时开拓了设计高性能环境吸附材料的创新途径。

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引用次数: 0

Efficient PM1 removal by bipolar pulsed electric agglomeration using dual-channel wire-wire electrodes 双通道导线电极双极脉冲电团聚高效去除PM1

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2025.136528

Zhenyu Yan, Zhen Liu, Keping Yan

Ultrafine particles (PM₁), one of the primary pollutants detrimental to human health and ecosystem integrity, present significant challenges for direct capture by conventional electrostatic precipitators (ESPs)due to their minute size and low saturation charge. This study introduces an innovative dual-channel rope-type wire-to-wire charger employing bipolar microsecond pulsed charging to enhance PM₁ removal via electric agglomeration. We systematically compared the charging performance and particle loss between direct current (DC) and pulsed modes. Particle Image Velocimetry (PIV) was also employed to visualize the flow field dynamics within the agglomeration zone at a gas velocity of 0.6 m/s. Results demonstrate that pulsed charging drastically enhances the charge of PM₁ by nearly an order of magnitude while reducing charge loss by over 20% compared to DC charging. Under optimal bipolar pulse conditions (+18 kV/−23.4 kV), the number concentration of 0.043 μm particles decreased by more than 23%, and the mass fraction of 1.3 μm particles increased by 15.9%. Scanning Electron Microscopy (SEM) analysis revealed three dominant agglomeration mechanisms for oily aerosols. Furthermore, the flow field in the agglomeration zone exhibited streamlines convergence and low-velocity sedimentation regions. By integrating this pulsed bipolar agglomeration technique with a downstream ESP, the removal efficiency of PM₁ was significantly enhanced, in particular for 0.043 μm particles from 78% to over 94%.

超细颗粒（PM1）是危害人类健康和生态系统完整性的主要污染物之一，由于其微小的尺寸和低饱和电荷，对传统静电除尘器（esp）的直接捕获提出了重大挑战。本研究介绍了一种创新的双通道绳式线对线充电器，采用双极微秒脉冲充电，通过电团聚来增强PM 1的去除。我们系统地比较了直流模式和脉冲模式下的充电性能和粒子损耗。采用粒子图像测速技术（PIV）对气体流速为0.6 m/s时凝聚区内的流场动态进行了可视化。结果表明，与直流充电相比，脉冲充电可大幅提高PM 1的电荷量，同时减少20%以上的电荷损失。在最佳双极脉冲条件下（+18 kV/−23.4 kV）， 0.043 μm颗粒的数量浓度下降了23%以上，1.3 μm颗粒的质量分数增加了15.9%。扫描电镜（SEM）分析揭示了油性气溶胶的三种主要团聚机制。团聚带的流场表现为流线收敛区和低速沉降区。通过将脉冲双极团聚技术与下游ESP集成，PM1的去除率显著提高，特别是对0.043 μm颗粒的去除率从78%提高到94%以上。

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引用次数: 0

GREEN extraction of antioxidant carotenoids from fresh ORANGE PEEL USING CO₂-expanded ethanol 用二氧化碳膨胀乙醇从新鲜橘子皮中提取抗氧化类胡萝卜素

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2026.136808

Merichel Plaza , María Luisa Marina

Carotenoids are valuable bioactive pigments widely used in the food, pharmaceutical, and cosmetic industries due to their potent antioxidant properties. The growing demand for sustainable extraction processes has driven interest in valorizing agro-industrial by-products, such as orange peel, which is particularly rich in carotenoids. Traditional extraction methods typically rely on toxic organic solvents and energy-intensive procedures, raising environmental and safety concerns. In this study, a green and efficient method based on CO₂-expanded ethanol (CXE) was developed for the extraction of antioxidant carotenoids from fresh orange peel waste. To the best of our knowledge, this is the first report exploring CXE for carotenoid recovery from citrus by-products. A theoretical evaluation using Hansen solubility parameters (HSP) was conducted to predict the solubility behaviour of key carotenoids in CXE, guiding the selection of optimal solvent compositions. A D-optimal response surface design was employed to optimize key extraction parameters, including CO₂ molar fraction, temperature, pressure, and solvent flow rate. The optimized CXE process (57.6 °C, 6.3 MPa, 1 mL/min, and 50% v/v CO₂ in ethanol) achieved significantly higher carotenoid yields and antioxidant capacities (ABTS and DPPH assays) than conventional solid-liquid extraction using acetone, hexane, or ethanol. Notably, the CXE method enabled direct extraction from fresh peel, circumventing the need for a drying step and thereby preserving thermolabile compounds and reducing energy consumption. These results confirm the potential of CXE as a scalable and sustainable alternative for the recovery of high-value compounds from citrus waste, aligning with green chemistry principles and circular economy strategies.

类胡萝卜素是一种有价值的生物活性色素，由于其有效的抗氧化特性，被广泛应用于食品、制药和化妆品行业。对可持续提取工艺的需求不断增长，推动了对农业工业副产品的兴趣，如橘子皮，其中特别富含类胡萝卜素。传统的提取方法通常依赖于有毒的有机溶剂和能源密集型的过程，引起了环境和安全问题。研究了一种绿色高效的以CO₂膨胀乙醇（CXE）为原料提取新鲜橘皮废弃物中抗氧化类胡萝卜素的方法。据我们所知，这是探索柑橘副产品中类胡萝卜素的CXE回收的第一份报告。利用汉森溶解度参数（Hansen soluble parameters， HSP）进行理论评价，预测了关键类胡萝卜素在CXE中的溶解度行为，指导了最佳溶剂组成的选择。采用d -最优响应面设计，对co2摩尔分数、温度、压力、溶剂流速等关键提取参数进行优化。优化后的CXE工艺（57.6°C, 6.3 MPa, 1 mL/min， 50% v/v CO₂在乙醇中）比传统的丙酮、己烷或乙醇固液萃取法获得了更高的类胡萝卜素产量和抗氧化能力（ABTS和DPPH检测）。值得注意的是，CXE方法可以直接从新鲜果皮中提取，避免了干燥步骤的需要，从而保存了耐热性化合物并降低了能耗。这些结果证实了CXE作为从柑橘废弃物中回收高价值化合物的可扩展和可持续替代方案的潜力，符合绿色化学原则和循环经济战略。

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引用次数: 0

Efficient and selective catalytic hydrogenation of nitroarenes catalyzed by two-dimensional Ni@Cu-MOF bimetallic nanosheets 二维Ni@Cu-MOF双金属纳米片催化硝基芳烃高效选择性加氢

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2026.136830

Yu-Xuan Zhang , Yi-Jie Ma , Hai-Ming Fei , Feng Zhang , Li-Juan Lan , Cai-Xia Yu , Xiao-Qiang Li , Lei-Lei Liu

Development of efficient non-noble metal catalysts for the chemoselective hydrogenation of nitroarenes under mild conditions remains a significant challenge. In this study, we harnessed the unique and distinctive merits of two-dimensional (2D) metal-organic frameworks (MOFs) to synthesize an ultrathin 2D Ni@Cu-MOF bimetallic system. By using the mild reducing agent NaBH₄, the 2D bimetallic catalyst achieved exceptional catalytic performance in the hydrogenation of 4-chloronitrobenzene, with nearly full conversion (99.9%) and outstanding selectivity (99.4%) at room temperature. Systematic experimental investigations further revealed the highly efficient catalytic performance of the catalyst in the hydrogenation for a broad substrate scope, including diverse nitroarenes with varying electronic properties and steric hindrance. The excellent catalytic activity of the 2D Ni@Cu-MOF bimetallic catalyst can be stemmed from its unique structural attributes. The bimetallic Ni-Cu system synergistically enhanced selectivity while preserving reactivity, achieving a balanced activity-chemoselectivity for nitroarene hydrogenation. Maximizing dispersed catalytic site utilization via atomic dispersion and optimized spatial arrangement in 2D MOFs significantly amplified the catalytic efficiency, ensuring rapid, selective catalysis under mild conditions. Moreover, the unique cavity structure on the Ni@Cu-MOF nanosheets provided a well-confined microenvironment, which not only stabilized the metal ions against aggregation but also created a tailored microenvironment that intensifies substrate-active site interactions, thereby enhancing reaction selectivity. The catalytic mechanism underwent in-depth investigation through techniques including Fourier transform infrared analysis, X-ray photoelectron spectroscopy, and theoretical calculations. These studies demonstrated that the interactions between metal active sites and substrate molecules within the cavities of MOF nanosheets contributed significantly to the catalytic hydrogenation.

开发在温和条件下用于硝基芳烃化学选择性加氢的高效非贵金属催化剂仍然是一个重大挑战。在这项研究中，我们利用二维（2D）金属有机框架（mof）的独特和独特的优点来合成超薄二维Ni@Cu-MOF双金属体系。采用温和还原剂NaBH4，二维双金属催化剂对4-氯硝基苯加氢反应具有优异的催化性能，室温下转化率接近100%(99.9%)，选择性优异（99.4%）。系统的实验研究进一步揭示了该催化剂在广泛的底物范围内的高效催化加氢性能，包括具有不同电子性质和位阻的多种硝基芳烃。二维Ni@Cu-MOF双金属催化剂的优异催化活性源于其独特的结构属性。双金属Ni-Cu体系在保持反应活性的同时协同增强了选择性，实现了硝基芳烃加氢的活性-化学选择性平衡。通过原子分散和优化二维mof的空间排列，最大化分散的催化位点利用，显著提高了催化效率，确保了在温和条件下的快速、选择性催化。此外，Ni@Cu-MOF纳米片上独特的空腔结构提供了一个良好的微环境，不仅稳定了金属离子的聚集，而且创造了一个定制的微环境，加强了底物-活性位点的相互作用，从而提高了反应的选择性。通过傅立叶变换红外分析、x射线光电子能谱和理论计算等技术对催化机理进行了深入研究。这些研究表明，MOF纳米片腔内金属活性位点与底物分子之间的相互作用对催化加氢有重要作用。

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引用次数: 0

Preparation of 5 N-grade high-purity tellurium via fractional vacuum distillation with mechanism of deep impurity removal 分级真空精馏深度除杂工艺制备5n级高纯碲

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2026.136838

Chaosong Meng , Xuan Cui , Jinxi Qiao , Zhipeng Xu , Qinghua Tian , Xueyi Guo

High-purity tellurium is an indispensable key material in semiconductor materials, new energy devices, and communications. This study employed fractional vacuum distillation to prepare 5 N-grade high-purity tellurium and proposes a technical route of “suppressing entrainment, segmented temperature control, and low-temperature selective volatilization” to deeply elucidate the migration behavior of tellurium and impurities. Single-stage vacuum distillation effectively removes low-volatility impurities such as Al, Fe, Ag, and Ni, achieving a total impurity removal rate of 69.15–78.04% and elevating tellurium purity from 99.9978% to 99.9995%, yet shows poor removal of medium- and high-volatility impurities including Bi, Se, Ca, Na, and Zn and even causes impurity enrichment. Two-stage vacuum distillation markedly lowers the content of these medium- and high-volatility impurities through selective volatilization, raising tellurium purity to 99.9998% with a total impurity removal rate of 91.16–93.49% and a direct yield of 93.51–94.84%. The study further indicates that tellurium exhibits two microscopic morphologies (smooth plate-like and raised granular) that depend on the temperature zone. This work demonstrates an environmentally sustainable and efficient strategy for high-purity tellurium preparation and offers valuable insights and practical implications for industrial applications.

高纯度碲是半导体材料、新能源器件、通信等领域不可缺少的关键材料。本研究采用分馏真空蒸馏法制备5n级高纯碲，提出了“抑制夹带、分段控温、低温选择性挥发”的技术路线，深入阐明了碲与杂质的迁移行为。单级真空蒸馏能有效去除Al、Fe、Ag、Ni等低挥发性杂质，总杂质去除率达到69.15 ~ 78.04%，将碲纯度从99.9978%提高到99.9995%，但对Bi、Se、Ca、Na、Zn等中、高挥发性杂质去除率较差，甚至会导致杂质富集。两级真空蒸馏通过选择性挥发，显著降低了中挥发性和高挥发性杂质的含量，将碲纯度提高到99.9998%，总杂质去除率为91.16 ~ 93.49%，直接收率为93.51 ~ 94.84%。研究进一步表明，碲在不同的温度区表现出两种微观形态（光滑的片状和凸起的颗粒状）。本研究为高纯度碲的制备提供了一种环境可持续和高效的策略，为工业应用提供了有价值的见解和实际意义。

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引用次数: 0

A dual-functional electrochemical system for versatile uranium recovery from acidic and organic-rich wastewaters 从酸性和富有机废水中回收铀的双功能电化学系统

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2026.136843

Jiaqi Chen , Jianzhang Gao , Yu Liu , Huitao Lv , Yongde Yan , Fuqiu Ma , Yun Xue , Xiangbiao Yin

Conventional methods struggle to treat two different types of nuclear wastewater (highly acidic and organic-rich uranium streams) within a single system. To address this, we developed an electro-synergy uranium recovery (ESUR) system that adaptively treats both wastewater types without reconfiguration. The ESUR system achieved high uranium removal from real and simulated wastewaters. At pH = 1.0, stirring improved removal rates by up to 4.98-fold (1 V) and 14.94-fold (4 V), while adding NaCl boosted efficiency to 99.9% within 1 h, which was 3.4-fold higher than without additives. And the uranium content was reduced below 30 μg/L within 3 h, meeting WHO standards. In real wastewater (pH ≈ 0.5), uranium removal efficiency reached 98%. The ESUR system also maintained over 90% uranium removal in simulated wastewater with organics (TBP, EDTA, HA, urea, PVA, THFA) and over 96% in real uranium-containing wastewater with high levels of organics and ammonia nitrogen. The characterization results demonstrate that uranium recovery from highly acidic wastewater was achieved via the synergistic coupling of three integrated processes in ESUR system. This work breaks from single-function electrochemical treatment paradigms, offering a versatile and efficient platform for managing diverse uranium-containing wastewaters and promoting sustainable uranium recovery.

传统方法很难在一个系统内处理两种不同类型的核废水（高酸性和富有机铀流）。为了解决这个问题，我们开发了一种电协同铀回收（ESUR）系统，该系统可以自适应地处理两种废水类型，而无需重新配置。ESUR系统从真实和模拟废水中实现了高铀去除。在pH = 1.0时，搅拌可分别提高4.98倍（1 V）和14.94倍（4 V）的去除率，加入NaCl可在1 h内将去除率提高到99.9%，比未添加添加剂时提高3.4倍。3 h内铀含量降至30 μg/L以下，符合WHO标准。在实际废水（pH≈0.5）中，铀的去除率可达98%。ESUR系统在含有机物（TBP、EDTA、HA、尿素、PVA、THFA）的模拟废水中也保持了90%以上的铀去除率，在含高浓度有机物和氨氮的含铀废水中也保持了96%以上的铀去除率。表征结果表明，通过ESUR系统中三个集成过程的协同耦合，可以实现高酸性废水中铀的回收。这项工作打破了单一功能的电化学处理范式，为管理多种含铀废水和促进可持续铀回收提供了一个多功能和高效的平台。

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引用次数: 0

From prediction to synthesis: A combined machine learning and density functional theory approach for designing high-performance biochar and decoding codeine adsorption 从预测到合成：结合机器学习和密度功能理论设计高性能生物炭和解码可待因吸附的方法

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-08 DOI: 10.1016/j.seppur.2026.136840

Mao Ye , Shurui Cao , Jie Tian , Hongtao Su , Yao Tang , Zhiqiong Chen

A significant challenge in the rational design of biochar as an adsorbent for organic pollutants lies in the accurate prediction of adsorption performance. Machine learning (ML) offered a data-driven solution to identify key biochar parameters and underlying adsorption mechanism that are difficult to capture using conventional methods. This study combined ML with density functional theory (DFT) calculations fully decoded the adsorption process of codeine onto deep eutectic solvent (DES) modified biochar. Results demonstrated that XGBoost model showed the highest prediction performance with R² of 0.9237, RMSE of 0.3002, and MAE of 0.2222. SHAP and PDPs identified total pore volume (V_total) and specific surface area (S_BET), and N content as key material properties. In detail, V_total integrated the molecular accommodation and transference of different pores ranges, and S_BET modulated the abundance of active sites. N content regulated the quantity of N-containing functional groups (e.g., -NH₂, -NH₃⁺) on the biochar, thereby facilitating chemical interactions such as hydrogen bonding and electrostatic attraction. Guided by ML insights, a high-performance DES-doped biochar was successfully synthesized, achieving a notable codeine uptake capacity of 2659.69 μg/g. Kinetics and isotherm studies indicated hybrid physico-chemical adsorption process, while thermodynamics confirmed spontaneity and endothermicity. DFT calculations revealed MEA-based DES had the best adsorption performance with a stronger binding energy (−18.8 Kcal/mol), a lowest ∆E_gap (3.367 eV), and expanded negative electrostatic potential regions, due to the dual hydrogen bonding effect. This work demonstrated a data-enhanced strategy for developing functional biochar and elucidating contaminant removal mechanisms through an integrated ML–DFT framework.

合理设计生物炭作为有机污染物吸附剂的一个重大挑战在于准确预测其吸附性能。机器学习（ML）提供了一种数据驱动的解决方案，用于识别传统方法难以捕获的关键生物炭参数和潜在的吸附机制。本研究结合ML和密度泛函理论（DFT）计算，全面解析了可待因在深度共晶溶剂（DES）改性生物炭上的吸附过程。结果表明，XGBoost模型预测效果最佳，R2为0.9237，RMSE为0.3002，MAE为0.2222。SHAP和pdp将总孔隙体积（Vtotal）、比表面积（SBET）和N含量确定为材料的关键性能。Vtotal综合了不同孔隙范围的分子调节和转移，SBET调节了活性位点的丰度。N的含量调节了生物炭上含N的官能团（例如-NH₂，-NH₃+）的数量，从而促进了氢键和静电吸引等化学相互作用。在ML的指导下，成功合成了高性能的des掺杂生物炭，其可待因吸收量达到2659.69 μg/g。动力学和等温线研究表明吸附过程为物理-化学混合吸附过程，而热力学研究证实了吸附的自发性和吸热性。DFT计算结果表明，由于双氢键效应，mea基DES具有较强的结合能（- 18.8 Kcal/mol）、最低的∆Egap （3.367 eV）和较大的负静电势区，具有较好的吸附性能。这项工作展示了通过集成ML-DFT框架开发功能性生物炭和阐明污染物去除机制的数据增强策略。

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引用次数: 0