Separation and Purification Technology最新文献_第10页

Recent progress in separation strategies for upgrading bio-oil: mechanisms, challenges and a way forward 生物油升级分离策略的最新进展：机制、挑战和前进方向

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137146

Akhil Mohan , Åsa Emmer , Klas Engvall , Mats Jonsson

Due to the presence of high content of oxygenated compounds (aldehydes, alcohols, carboxylic acids, esters, ethers, furfurals, ketones, lignin-derived compounds, phenols, and sugars), bio-oil has inferior oil properties compared to petroleum-derived oils. This creates numerous technological challenges in downstream separation processes. The present study outlines recent research trends on various separation strategies for upgrading crude biogenic pyrolysis oil for the production of valuable commodities. The present study mainly focuses on the various separation strategies, such as column chromatography, distillation, membrane filtration, crystallization, solvent extraction, electrosorption, and fractional condensation with respect to principles of operation, efficiency, economy and environmental concerns. Phase separation using solvent and adsorbent was found to be the best separation strategy compared to others due to lower capital investment and energy expenditure. However, there are various technological challenges with separation strategies for scale-up in industries. A comparative analysis of various separation strategies with the application of various bio-oil fractions from aqueous phases of bio-oil is summarized to understand the possible pathways for utilization in various industries. A brief section on technoeconomic analysis with existing pilot and semi-pilot pyrolysis plants is presented to understand the economic feasibility of pyrolysis and upgrading strategies. In the end, a circular economy perspective of pyrolysis-separation and its integration with a machine learning model, are briefly outlined.

由于含氧化合物（醛类、醇类、羧酸类、酯类、醚类、糠醛类、酮类、木质素衍生化合物、酚类和糖）含量高，与石油衍生油相比，生物油的油性能较差。这给下游分离过程带来了许多技术挑战。本研究概述了各种分离策略的最新研究趋势，以提高原油生物热解油的生产价值。本文主要从操作原理、效率、经济和环境等方面对柱层析、蒸馏、膜过滤、结晶、溶剂萃取、电吸附和分馏冷凝等分离策略进行了研究。采用溶剂和吸附剂相分离是一种较好的分离方法，具有较低的资金投入和能源消耗。然而，在工业规模扩大的分离策略中存在各种技术挑战。本文对生物油水相中不同馏分的分离策略及应用进行了比较分析，以了解其在不同行业的应用途径。简要介绍了现有中试和半中试热解装置的技术经济分析，以了解热解和升级策略的经济可行性。最后，简要概述了热解分离的循环经济视角及其与机器学习模型的集成。

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引用次数: 0

Capacitive deionization based on Ti2P2O9: symmetrical electrode and synergistic removal mechanism of thallium and fluoride 基于Ti2P2O9的电容去离子：对称电极及协同除氟机制

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137151

Yupeng Li, Lei Huang, Zhu Xiong, Gaosheng Zhang

Electroplating and mining wastewater contain important pollutants such as thallium and fluoride. Capacitive deionization technology is the current cutting-edge technology for treatment. This study prepares titanium-based phosphate crystal material Ti₂P₂O₉ using the hydrothermal method, and the material particles exhibit a spherical morphology. Ti, P, and O elements are uniformly distributed on the material surface, with a specific surface area of 87.94 m²/g and capacitance of 30.54 F/g. The material demonstrates efficient removal of Tl(I) under different pH conditions and achieves efficient removal of fluoride ions in strong acidic environments. The maximum adsorption capacity of Ti₂P₂O₉ for thallium under neutral conditions, as determined from the Langmuir isotherm adsorption curve fitting results, is 526.96 mg/g, and the maximum adsorption capacity for fluoride under acidic conditions is 51.27 mg/g. The material exhibits excellent regenerative performance, achieving regeneration effects of 90.4% and 69.9% for the removal of thallium and fluoride ions, respectively, after multiple regenerations under electrochemical methods. After DFT simulation calculation, the energy barriers are ordered from high to low as: Ti₂P₂O₉-F, Ti₂P₂O₉-HF, Ti₂P₂O₉-Tl. This paper investigates the efficiency of this material for capacitive deionization in removing thallium and fluoride pollution under multi-factor conditions. The micro-mechanisms of the material during electroadsorption are discussed, that combined with theoretical calculations. It provides guidance for research on electroadsorption-assisted pollutant removal.

电镀和采矿废水中含有重要的污染物，如铊和氟化物。电容去离子技术是目前治疗的前沿技术。本研究采用水热法制备钛基磷酸盐晶体材料Ti2P2O9，材料颗粒呈球形形貌。Ti、P、O元素均匀分布在材料表面，比表面积为87.94 m2/g，电容为30.54 F/g。该材料在不同pH条件下均能有效去除Tl(I)，在强酸性环境下也能有效去除氟离子。Langmuir等温吸附曲线拟合结果表明，Ti2P2O9在中性条件下对铊的最大吸附容量为526.96 mg/g，在酸性条件下对氟的最大吸附容量为51.27 mg/g。该材料表现出优异的再生性能，经多次电化学再生后，对铊离子和氟离子的去除率分别达到90.4%和69.9%。经DFT模拟计算，能垒由高到低依次为：Ti2P2O9-F、Ti2P2O9-HF、Ti2P2O9-Tl。研究了该材料在多因素条件下电容去离子去除铊和氟污染的效率。结合理论计算，讨论了材料电吸附过程的微观机理。为电吸附辅助去除污染物的研究提供了指导。

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引用次数: 0

Excellent sieving separation of methanol from water and ethanol by ultramicroporous molecular-sieving UTSA-280 and cage-like Cu-Tria 超微孔分子筛UTSA-280和笼状Cu-Tria对甲醇与水和乙醇的分离效果良好

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137142

Xiaoqing Zheng , Fahui Xiang , Hongyu Lin , Lei He , Shengchang Xiang , Zhangjing Zhang

High-purity methanol is in high global demand due to its critical role in chemical synthesis and energy production. However efficiently separating methanol from the impurities such as water and ethanol with low energy consumption remains a key challenge. Here two ultramicroporous MOFs (molecular-sieving UTSA-280 and cage-like Cu-Tria) are investigated for methanol purification. The results show excellent water/methanol separation performance in both MOFs. But in a single adsorption cycle from a 16/84 water/methanol mixture, Cu-Tria achieved a markedly higher methanol productivity of 23.24 mmol/g (98% purity) than that of UTSA-280 (3.63 mmol/g) with a higher water/methanol separation factor of 46.00. Moreover, methanol/ethanol mixture can be separated only by Cu-Tria, benefiting from the enhancing sieving effect of the cage-window structure. Adsorption enthalpies, diffusional time constants measurements and grand canonical Monte Carlo (GCMC) simulations demonstrate that the selective separation of water/methanol mixture in UTSA-280 is mainly ascribed to the kinetic mechanism by the faster transport of water over methanol in the confined channels. But the balance between high water adsorption capacity and high water/methanol separation selectivity in Cu-Tria is achieved by the synergistic effect of thermodynamic and kinetic mechanisms originating from its cage-window structure.

由于其在化学合成和能源生产中的关键作用，高纯度甲醇在全球的需求量很大。然而，如何以低能耗将甲醇从水和乙醇等杂质中高效分离出来仍然是一个关键的挑战。本文研究了两种超微孔mof（分子筛UTSA-280和笼状Cu-Tria）用于甲醇净化。结果表明，两种MOFs均具有优异的水/甲醇分离性能。但在16/84水/甲醇混合物的单次吸附循环中，Cu-Tria的甲醇产率为23.24 mmol/g（98%纯度），显著高于UTSA-280 (3.63 mmol/g)，水/甲醇分离系数为46.00。此外，由于笼窗结构的增强筛分作用，甲醇/乙醇混合物只能通过Cu-Tria进行分离。吸附焓、扩散时间常数测量和大正则蒙特卡罗（GCMC）模拟表明，水/甲醇混合物在UTSA-280中的选择性分离主要归因于水在受限通道中快速通过甲醇的动力学机制。Cu-Tria的高水吸附能力和高水/甲醇分离选择性之间的平衡是由其笼窗结构引起的热力学机制和动力学机制的协同作用实现的。

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引用次数: 0

Chitosan aerogel beads embedded with CoFe layered double hydroxide for peroxymonosulfate activation 壳聚糖气凝胶珠包埋fe层状双氢氧化物用于过氧单硫酸盐活化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137149

Wenjun Zeng , Yidan Luo , Shujuan He , Huiyin Ye , Yueyang Xiao , Shuohan Yu , Yu Xie , Mingshan Xue , Zuozhu Yin , Zugen Liu , Bin Gao

In the development of efficient catalysts for antibiotic degradation, catalyst recovery has long been a major challenge. Immobilizing advanced oxidation catalysts within porous biopolymer supports such as chitosan beads can effectively address this issue, but their cyclic stability remains a key focus of research. In this study, a novel chitosan aerogel microsphere embedded with cobalt‑iron layered double hydroxide (CS/CoFe LDH) was synthesized to efficiently activate peroxymonosulfate (PMS) to degrade tetracycline (TC). The CS/CoFe LDH aerogel microspheres constructed a three-dimensional porous network and contained abundant functional groups, thereby enhancing TC removal and facilitating catalyst recovery. Under optimal conditions, the CS/CoFe/PMS system achieved near-complete degradation of TC. The catalyst maintained high activity at pH 3–11 and in real water environments, with TC removal efficiency remaining above 82% even after five reuse cycles.

Mechanistic investigations revealed that TC degradation was predominantly governed by a non-radical oxidation pathway, with superoxide radicals (·O₂⁻) playing an auxiliary role, while hydroxyl radicals (·OH) and sulfate radicals (·SO₄⁻) contributed to a lesser extent, indicating the coexistence of multiple oxidative pathways. The surface redox cycling of Co²⁺/Co³⁺ and Fe²⁺/Fe³⁺ was identified as the key mechanism for continuous PMS activation. Combined with liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) analysis, key intermediate products were identified, and degradation pathways involving demethylation, hydroxylation, ring cleavage, etc., were proposed. Toxicity predictions indicated that these intermediates were generally less harmful than TC, confirming the safety of the mineralization process. This work provides valuable mechanistic insights and demonstrates the application potential of aerogel-encapsulated LDH catalysts for water remediation and antibiotic removal.

在开发高效的抗生素降解催化剂的过程中，催化剂的回收一直是一个主要的挑战。在壳聚糖珠等多孔生物聚合物载体中固定化高级氧化催化剂可以有效地解决这一问题，但其循环稳定性仍是研究的重点。本研究合成了一种新型壳聚糖气凝胶微球，包埋钴-铁层状双氢氧化物（CS/CoFe LDH），以高效激活过氧单硫酸盐（PMS）降解四环素（TC）。CS/CoFe LDH气凝胶微球构建了三维多孔网络，含有丰富的官能团，从而增强了TC的去除能力，促进了催化剂的回收。在最优条件下，CS/CoFe/PMS体系实现了TC的近乎完全降解。该催化剂在pH值 3-11和真实水环境中保持了较高的活性，即使重复使用5次，TC的去除率仍保持在82%以上。机理研究表明，TC的降解主要由非自由基氧化途径控制，超氧自由基（·O2−）起辅助作用，羟基自由基（·OH）和硫酸盐自由基（·SO4−）的作用较小，表明多种氧化途径并存。Co2+/Co3+和Fe2+/Fe3+的表面氧化还原循环是PMS持续活化的关键机制。结合液相色谱-质谱（LC-MS）和密度泛函理论（DFT）分析，确定了关键中间产物，并提出了降解途径，包括去甲基化、羟基化、环裂解等。毒性预测表明，这些中间体的危害一般小于TC，证实了矿化过程的安全性。这项工作提供了有价值的机理见解，并证明了气凝胶封装LDH催化剂在水修复和抗生素去除方面的应用潜力。

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引用次数: 0

One-step hydrothermal synthesis of Zn/Co MOF for efficiently activating PMS to degrade organic pollutants in water: The reaction kinetics and mechanism 一步水热合成Zn/Co MOF高效活化PMS降解水中有机污染物的反应动力学及机理

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137127

Ming Zhang , Jiacheng Li , Lijun Wu , Tian Liang , Jian Liu , Lu Wang

Acetamiprid (ACE) can accumulate in the environment through the food chain, potentially endanger human health. In this experiment, zinc‑cobalt bimetallic metal organic framework (Zn/Co MOF) was synthesized and used to activate peroxymonosulfate (PMS) for the removal of ACE from water. The degradation efficiency of ACE could achieve approximately 96.93% after 90 min. Through the synergistic effect of Zn and Co bimetallic sites, ACE was degraded via a Fenton-like reaction, while reactive oxygen species (SO₄^·-, ·OH, O₂^·-, and ¹O₂) participated in the process. The high catalytic activity of Zn/Co MOF led to the degradation of ACE through the formation of a series of low-toxicity intermediates, and partial mineralization to CO₂ and H₂O. In addition, Zn/Co MOF remained effective under broad pH conditions (pH 5–11) and temperatures (5–45 °C). This system had excellent degradation effects in actual water, with degradation rates of 95.42% and 95.18% after 90 min in the Pai River and Liren Lake, respectively. With its high catalytic performance, the Zn/Co MOF is expected to become an ideal catalyst that could be used to remove pesticide residues in water.

对乙酰米虫啉（ACE）可通过食物链在环境中积累，潜在地危害人体健康。本实验合成了锌-钴双金属有机骨架（Zn/Co MOF），并将其用于活化过氧单硫酸盐（PMS）去除水中的ACE。90 min后，ACE的降解效率可达96.93%左右。通过Zn和Co双金属位点的协同作用，ACE通过类芬顿反应被降解，而活性氧（SO4·-、·OH、O2·-和1O2）参与了这一过程。Zn/Co MOF的高催化活性通过形成一系列低毒中间体，部分矿化为CO2和H2O，导致ACE的降解。此外，Zn/Co MOF在较宽的pH条件（pH 5-11）和温度（5-45°C）下仍然有效。该系统在实际水体中具有良好的降解效果，在排河和立人湖中，90 min后降解率分别为95.42%和95.18%。Zn/Co MOF具有良好的催化性能，有望成为去除水中农药残留的理想催化剂。

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引用次数: 0

Freeze-thaw switched diverse singlet oxygen initiation for prevailing the dual-substrate synergistic decontamination in textile wastewater 冻融切换多种单线态氧引发法对纺织废水进行双底物协同除污

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-04 DOI: 10.1016/j.seppur.2026.137097

Peng Zhang, Yongyi Mo, Yanqiu Li, Xiao Wang, Zhen Zhang, Yang Sun, Liang Tang

With gradually increased concerning of water resources management, how to mitigate the serious impacts of both printing dyes and fallen fabrics in textile sewage on environmental quality and health risks are still challenging. Here we reported that the coexisted azo dyes and microplastics from fiber debris in printing and dyeing wastewater, such as methyl orange (MO) and polyvinyl chloride (PVC), can be concurrently decontaminated when assisting with the permonosulfate (PMS)-based nonradiative mediation under ambient and freezing conditions. Insights into the freeze-thaw effect on strengthening mutual collisions between MO/PVC and PMS are crucial for switching the diverse singlet oxygen (¹O₂) initiation imposed by the series of oxidative degradation (e.g., PMS dosage, thermal and pH effect, metal ions and natural organic matter) and reactive species identifications (e.g., radical quenching experiments, electron paramagnetic resonance and galvanic oxidation). Especially through in situ confocal Raman-microscope analysis on simulated winter freezing, the progressive freeze concentration could prevail the PMS activation with the chloride ion from PVC dehydrochlorination for further promoting the robust ¹O₂ generation and efficient dual-substrate (i.e., MO and PVC) degradation at low toxicity (i.e., intermediate monitor and ECOSAR program). This system with good resistance to water matrix provides a new possibility for exploring the synergistic decontamination of complex pollutants from textile wastewater in permafrost regions or under year-round all seasonal conditions.

随着人们对水资源管理的日益关注，如何减轻纺织废水中印染和落布对环境质量和健康风险的严重影响仍然是一个挑战。本文报道了印染废水中共存的偶氮染料和微塑料，如甲基橙（MO）和聚氯乙烯（PVC），在环境和冷冻条件下，在permonsulfate （PMS）为基础的非辐射介质的辅助下，可以同时去除甲基橙（MO）和聚氯乙烯（PVC）。了解冻融效应对加强MO/PVC和PMS之间相互碰撞的影响，对于改变一系列氧化降解（如PMS剂量、热和pH效应、金属离子和天然有机物）和反应物质鉴定（如自由基淬火实验、电子顺磁共振和电氧化）所施加的不同单线态氧（1O2）引发至关重要。特别是通过原位共聚焦拉曼显微镜对模拟冬季冻结的分析，渐进冻结浓度可以优于PMS与PVC脱氢氯化氯离子的激活，从而进一步促进在低毒性（即中间监测和ECOSAR程序）下稳定生成1O2和高效降解双底物（即MO和PVC）。该系统具有良好的抗水基质性能，为探索多年冻土区或全年全季节条件下纺织废水中复杂污染物的协同去污提供了新的可能性。

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引用次数: 0

Enhancing hydrogen sulfide removal through photoelectrochemistry with WO3 photoanodes under blue LED irradiation 蓝光LED照射下WO3光阳极光电化脱除硫化氢

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-03 DOI: 10.1016/j.seppur.2026.137138

Roberta Y.N. Reis , Alberto Rodríguez-Gómez , Caio V.S. Almeida , Lucia H. Mascaro , Manuel A. Rodrigo

Hydrogen sulfide (H₂S) is a highly toxic and corrosive gas commonly found in industrial emissions, posing serious environmental and operational risks. This work proposes an innovative photoelectrocatalytic strategy for the simultaneous degradation of gaseous H₂S and the generation of green hydrogen (H₂) under flux conditions. The system integrates gas-liquid absorption with electrochemical and photoelectrochemical oxidation, employing a WO₃ photoanode and a stainless steel cathode separated by a proton exchange membrane. The performance of the electrocatalytic and photoelectrocatalytic configurations was systematically evaluated regarding H₂S removal efficiency, hydrogen production, and energy consumption. The photoelectrocatalytic process exhibited superior activity, achieving a degradation of 8.2 mg S with a Coulombic efficiency of 3600 mg S Ah⁻¹ for H₂S oxidation and a Faradaic efficiency of 60% for H₂ evolution at an applied current density of 0.33 mA cm⁻². Illumination with a 10 W high-power blue LED significantly increased charge separation and reduced the cell potential, resulting in higher energy efficiency. Post-reaction characterization by X-ray photoelectron spectroscopy (XPS) demonstrated partial sulfur deposition on the WO₃ surface and the presence of oxidized sulfur species. Overall, the results demonstrate that photoelectrocatalysis under optimized conditions offers an efficient and sustainable route for simultaneous H₂S reduction and hydrogen generation, providing a promising dual-purpose platform for environmental remediation and renewable energy production.

硫化氢（H2S）是一种剧毒腐蚀性气体，常见于工业排放中，具有严重的环境和操作风险。这项工作提出了一种创新的光电催化策略，用于在通量条件下同时降解气态H2S和生成绿色氢（H2）。该系统将气液吸收与电化学和光电化学氧化相结合，采用WO3光阳极和由质子交换膜分离的不锈钢阴极。系统地评估了电催化和光催化构型对H2S的去除效率、产氢量和能耗。光电催化过程表现出优异的活性，在0.33 mA cm−2的电流密度下，H2S氧化的库仑效率为3600 mg S Ah−1，降解8.2 mg S，氢气析出的法拉第效率为60%。10 W高功率蓝色LED的照明显著增加了电荷分离，降低了电池电位，从而提高了能源效率。反应后的x射线光电子能谱（XPS）表征表明，WO3表面有部分硫沉积，并且存在氧化硫。综上所述，优化条件下的光电催化为同时还原H2S和制氢提供了一条高效、可持续的途径，为环境修复和可再生能源生产提供了一个有前景的双用途平台。

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引用次数: 0

Influence of fiber microstructure on particle dynamic deposition and macroscopic filtration performance in nonwoven fiber filter media 纤维微观结构对非织造纤维过滤介质中颗粒动态沉积及宏观过滤性能的影响

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-03 DOI: 10.1016/j.seppur.2026.137143

Hao Jin , Chenxuan Wang , Gangcheng Peng , Jiahua Chai , Qiang Zhang , Zhenyu Wu , Xiaoyu Zhu , Xuegang Wang , Changgeng Gui , Fan Geng , Shihang Li

Multilayer nonwoven fiber filter media are critical components in separation and purification processes for efficient fine particulate matter removal from airflow. However, there is a lack of in-depth understanding of how fiber microstructure dictates the dynamic evolution of particle deposition and, consequently, the macroscopic filtration performance. Understanding this mechanism is important for designing a new generation of filters characterized by high efficiency, low pressure drop, and prolonged lifespan. This paper investigates the influence of key structural parameters of fiber filter media, such as fiber packing density and fiber diameter, on particle deposition characteristics using the Discrete Element Method-Computational Fluid Dynamics (DEM-CFD) coupling simulation method. The results indicate that the timing of the dynamic transition from deep filtration to surface filtration of the filter media is regulated by the fiber microstructural parameters. Specifically, increasing fiber packing density or decreasing fiber diameter can improve filtration efficiency, but it lead to the concentration of deposited particles in the shallow filter media, resulting in a rapid increase in pressure drop and a decrease in quality factor. Conversely, reduced packing density and increased fiber diameters can facilitate particles penetrating deep into the filter media and achieving uniform deposition, thereby maintaining high filtration efficiency while delaying the increase in pressure drop and enhancing the quality factor, and extending the purification unit's service life. The research outcomes can offer theoretical guidance for the rational design, structural optimization, and performance enhancement of advanced nonwoven filter media.

多层非织造纤维过滤介质是分离和净化过程中有效去除气流中细颗粒物的关键部件。然而，人们对纤维微观结构如何决定颗粒沉积的动态演变以及宏观过滤性能缺乏深入的了解。了解这一机制对于设计新一代过滤器具有高效率、低压降和长寿命的特点非常重要。本文采用离散元法-计算流体力学（DEM-CFD）耦合模拟方法，研究了纤维滤料关键结构参数如纤维堆积密度和纤维直径对颗粒沉积特性的影响。结果表明，过滤介质从深层过滤到表面过滤的动态过渡时间受纤维微观结构参数的调控。具体而言，增大纤维堆积密度或减小纤维直径可以提高过滤效率，但会导致沉积颗粒在浅层过滤介质中的浓度增加，导致压降迅速增大，质量因子降低。反之，降低填料密度，增加纤维直径，有利于颗粒深入过滤介质，达到均匀沉积，从而保持较高的过滤效率，同时延缓压降的增大，提高质量系数，延长净化装置的使用寿命。研究成果可为先进无纺布滤料的合理设计、结构优化和性能提升提供理论指导。

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引用次数: 0

A novel pyrazolyl-pyridine N-donor ligand-based extraction system for the separation of trivalent actinides from lanthanides without lipophilic anions 一种新型的吡唑吡啶n给体萃取体系用于分离三价锕系元素和不含亲脂阴离子的镧系元素

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-03 DOI: 10.1016/j.seppur.2026.137147

Rui Li, Hang Zhou, Yiting Wang, Qiao Yu, Die Huang, Qiaoyin Huang, Songdong Ding

To address the challenges of poor lipophilicity and the reliance on synergistic extractants in pyrazolyl-pyridine N-donor ligands for separating trivalent actinides from lanthanides, four 2,6-bis(5-alkyl-1H-pyrazol-3-yl)pyridine (BPP) ligands with varying alkyl chains were designed and synthesized. An efficient extraction system was established using n-octanol/n-dodecane (50 vol%) as the diluent, requiring no synergistic extractant. Among the ligands, C8-BPP exhibits a higher extraction selectivity for Am³⁺ over trivalent lanthanide ions (Ln³⁺), with separation factors (SF_Am/Ln) ranging from 48 to 172. Slope analysis, UV–vis titration, and isothermal titration calorimetry (ITC) consistently confirmed a 2:1 ligand-to-metal complexation stoichiometry with Eu³⁺. Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) analyses verified the tridentate coordination mode of C8-BPP. Further studies using Raman spectroscopy and conductivity measurements revealed the bidentate coordination of NO₃⁻ ions and their coordination number in the inner sphere, while time-resolved laser fluorescence spectroscopy (TRLFS) confirmed a dehydrated inner coordination environment for Eu³⁺. Based on combined extraction and complexation results, a neutral complexation-based extraction model was proposed. The corresponding stability constants and thermodynamic parameters (ΔH, ΔS, ΔG) were also determined.

为解决吡唑吡啶n给体在分离镧系元素和三价锕系元素时亲脂性差和依赖协同萃取剂的难题，设计并合成了4种不同烷基链的2,6-二（5-烷基- 1h -吡唑-3-基）吡啶（BPP）配体。以正辛醇/正十二烷（50 vol%）为稀释液，建立了一种高效的萃取体系，无需增效萃取剂。其中，C8-BPP对Am3+的萃取选择性高于三价镧系离子（Ln3+），分离因子（SFAm/Ln）在48 ~ 172之间。斜率分析、紫外-可见滴定和等温滴定量热法（ITC）一致证实了Eu3+的配体-金属络合化学计量。傅里叶变换红外（FT-IR）和x射线光电子能谱（XPS）分析证实了C8-BPP的三叉配位模式。利用拉曼光谱和电导率测量进一步研究发现，NO3−离子的双齿配位及其在内球中的配位数，而时间分辨激光荧光光谱（TRLFS）证实了Eu3+的脱水内配位环境。结合萃取和络合的结果，提出了一种基于中性络合的萃取模型。测定了相应的稳定性常数和热力学参数（ΔH， ΔS， ΔG）。

{"title":"A novel pyrazolyl-pyridine N-donor ligand-based extraction system for the separation of trivalent actinides from lanthanides without lipophilic anions","authors":"Rui Li, Hang Zhou, Yiting Wang, Qiao Yu, Die Huang, Qiaoyin Huang, Songdong Ding","doi":"10.1016/j.seppur.2026.137147","DOIUrl":"10.1016/j.seppur.2026.137147","url":null,"abstract":"<div><div>To address the challenges of poor lipophilicity and the reliance on synergistic extractants in pyrazolyl-pyridine N-donor ligands for separating trivalent actinides from lanthanides, four 2,6-bis(5-alkyl-1H-pyrazol-3-yl)pyridine (BPP) ligands with varying alkyl chains were designed and synthesized. An efficient extraction system was established using <em>n</em>-octanol/<em>n</em>-dodecane (50 vol%) as the diluent, requiring no synergistic extractant. Among the ligands, C8-BPP exhibits a higher extraction selectivity for Am<sup>3+</sup> over trivalent lanthanide ions (Ln<sup>3+</sup>), with separation factors (<em>SF</em><sub>Am/Ln</sub>) ranging from 48 to 172. Slope analysis, UV–vis titration, and isothermal titration calorimetry (ITC) consistently confirmed a 2:1 ligand-to-metal complexation stoichiometry with Eu<sup>3+</sup>. Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) analyses verified the tridentate coordination mode of C8-BPP. Further studies using Raman spectroscopy and conductivity measurements revealed the bidentate coordination of NO<sub>3</sub><sup>−</sup> ions and their coordination number in the inner sphere, while time-resolved laser fluorescence spectroscopy (TRLFS) confirmed a dehydrated inner coordination environment for Eu<sup>3+</sup>. Based on combined extraction and complexation results, a neutral complexation-based extraction model was proposed. The corresponding stability constants and thermodynamic parameters (Δ<em>H</em>, Δ<em>S</em>, Δ<em>G</em>) were also determined.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137147"},"PeriodicalIF":9.0,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110898","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

Interchain hydrogen bonding in one-dimensional benzimidazolone-based covalent organic frameworks: charge modulation for improved gold recovery efficiency 一维苯并咪唑酮基共价有机骨架中的链间氢键：电荷调制提高金回收率

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-02-03 DOI: 10.1016/j.seppur.2026.137144

Zhen-Wen Zhang , Cheng-Peng Niu , Sai-Jin Xiao , Hao-Xuan He , Qiang Shi , Zhi-Hao Xue , Bin Lin , Ru-Ping Liang , Li Zhang , Jian-Ding Qiu

One-dimensional covalent organic frameworks (1D COFs), as linear crystalline porous polymers, are highly promising materials for gold recovery due to their exceptional atomic utilization efficiency and fully exposed active sites. However, their development for gold adsorption is constrained by the lack of gold-specific organic building blocks and limited electronic regulation strategies. Herein, we introduce benzoimidazolone units into 1D COFs and design interchain hydrogen bond through molecular engineering to rationally modulate their charge distribution. The constructed 1D COF, featuring improved crystallinity/stability, enriched recognition sites, and enhanced protonation capability, demonstrates superior performance in gold recovery with rapid kinetics, excellent selectivity and a high adsorption capacity of 2900.56 mg g⁻¹. Theoretical calculations reveal the multiple and synergistic interactions between benzimidazolone and AuCl₄⁻, and elucidate the effect of hydrogen bonding on electron redistribution/transfer towards benzimidazolone, thereby promoting its protonation and significantly enhancing the adsorption and reduction capabilities for gold. This work highlights the significance of hydrogen bonding on charge modulation and develops a benzimidazolone-based 1D COFs for efficient gold recycling from electronic waste.

一维共价有机框架（1D COFs）作为一种线性晶体多孔聚合物，由于其优异的原子利用效率和充分暴露的活性位点，是一种非常有前途的金回收材料。然而，由于缺乏金特异性有机构件和有限的电子调节策略，它们在金吸附方面的发展受到限制。本文将苯并咪唑酮单元引入一维COFs中，通过分子工程设计链间氢键，合理调节其电荷分布。所构建的1D COF具有结晶度/稳定性提高、识别位点丰富、质子化能力增强等特点，具有快速的动力学、优异的选择性和2900.56 mg g−1的高吸附量，具有优异的金回收性能。理论计算揭示了苯并咪唑酮与AuCl4−之间的多重协同相互作用，并阐明了氢键对电子向苯并咪唑酮的再分配/转移的影响，从而促进了苯并咪唑酮的质子化，显著提高了对金的吸附和还原能力。这项工作强调了氢键在电荷调制中的重要性，并开发了一种基于苯并咪唑酮的1D COFs，用于从电子废物中高效回收金。

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引用次数: 0