Separation and Purification Technology最新文献_第8页

Carbon-based catalysts for CO2 hydrogenation to C1 products: mechanisms, materials, and prospects 二氧化碳加氢制C1产物的碳基催化剂：机理、材料及前景

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-06 DOI: 10.1016/j.seppur.2026.137175

Han Yan , Zejin Zhao , Rui Han , Lifei Wei , Gaoqi Han , Yuhan Ba , Chunfeng Song , Qingling Liu

Carbon-based catalysts have received much attention in the field of catalysis due to their excellent electrical conductivity, high specific surface area, good chemical stability, and thermal conductivity, particularly for CO₂ conversion. Carbon materials as catalyst supports enhance CO₂ hydrogenation by leveraging their excellent electrical/thermal conductivity to facilitate electron transfer and heat dispersion. At the same time, their high specific surface area and porous structure provide abundant active sites. They also maintain stable mechanical properties under harsh conditions, synergistically boosting conversion efficiency and product selectivity. This review examines the use of carbon materials as catalytic supports for the thermal hydrogenation of CO₂ to C1 products. Initially, we elucidate the mechanism by which carbon-based support promotes the CO₂ hydrogenation reaction. Subsequently, the synthesis method of various carbon-based catalyst composites designed for the thermal hydrogenation of CO₂ was summarised. Furthermore, we provide a comprehensive comparison of the catalytic activity and selectivity of carbon-supported catalysts, offering insights into how different dimensions of carbon-based carriers influence the catalytic performance toward the production of methane, methanol, formic acid, and carbon monoxide. Lastly, the paper highlights the current challenges and prospective research directions for the research of carbon-based catalysts in CO₂ conversion reactions, paving the way for innovative strategies to address global carbon neutrality and sustainable energy conversion through advanced CO₂ utilisation technologies.

碳基催化剂因其优异的导电性、高的比表面积、良好的化学稳定性和良好的导热性，特别是在CO2转化方面受到了催化领域的广泛关注。碳材料作为催化剂，通过利用其优异的电导率/导热性来促进电子传递和热量分散，从而支持增强二氧化碳的氢化。同时，它们的高比表面积和多孔结构提供了丰富的活性位点。它们还在恶劣条件下保持稳定的机械性能，协同提高转化效率和产品选择性。本文综述了碳材料作为二氧化碳热加氢制C1产物的催化载体的应用。首先，我们阐明了碳基载体促进CO2加氢反应的机理。随后，总结了各种用于CO2热加氢的碳基催化剂复合材料的合成方法。此外，我们提供了碳负载催化剂的催化活性和选择性的全面比较，提供了不同尺寸的碳基载体如何影响甲烷，甲醇，甲酸和一氧化碳的催化性能的见解。最后，本文重点介绍了碳基催化剂在二氧化碳转化反应中的研究面临的挑战和未来的研究方向，为通过先进的二氧化碳利用技术解决全球碳中和和可持续能源转化的创新战略铺平了道路。

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引用次数: 0

Strategic gradient Zn incorporation into PdZrO2 to engineer Pd-Zn-Zr interfaces: Exploring the synergism between PdZn alloy and ZnZrOx in shaping plasma-catalytic CO2 hydrogenation routes 在PdZrO2中战略性梯度加入Zn以设计Pd-Zn-Zr界面：探索PdZn合金和ZnZrOx在塑造等离子体催化CO2加氢路线中的协同作用

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-11 DOI: 10.1016/j.seppur.2026.137231

Boqiong Jiang , Jingying Chen , Zhengxuan Wu , Haoyu Yang , Jingyi Han , Yi Zhang , Ting Wang , Shaocai Yu , Yuhai Sun

A systematic investigation was conducted on a series of PdZn_αZrO_x catalysts with precisely tuned Zn concentration gradients (α = 0.1–0.9) for plasma-catalytic CO₂ hydrogenation. PdZn_0.3ZrO_x exhibited the highest CO₂ conversion of 51.5%, while PdZn_0.7ZrO_x achieved a maximum CO yield of 45.4% with a selectivity exceeding 95%. These performances were attained even under a high H₂/CO₂ molar ratio of 3:1, a condition typically favoring methanation. Characterizations revealed that the synergy between the PdZn alloy and ZnZrO_x was pivotal in dictating the reaction pathways. The PdZn alloy enhanced the PdZr interaction, generating abundant oxygen vacancies (O_v) that effectively activated CO₂ to form bi-CO₃²⁻. This intermediate preferred hydrogenation to bi-HCOO⁻, which would subsequently decompose into CO^⁎ or hydrogenate into CH₄. The PdZn alloy weakened the adsorption strength of CO^⁎, promoting its desorption and thereby increasing CO selectivity. When α > 0.3, excessive Zn interacted with Zr to form ZnZrO_x. This phase not only prevented excessive Zn from aggregating into ZnO that could cover O_v but also stabilized hydrogen spillover species from ZrO₂, suppressing the hydrogenation of bi-HCOO⁻ to CH₄ and steering the reaction towards CO production. By harnessing this synergistic effect, the PdZn_αZrO_x catalysts achieved over 40% CO₂ conversion with CO as the predominant product, presenting a novel plasma-catalytic strategy to overcome the traditional activity-selectivity trade-off in reverse water-gas shift reactions for CO₂ utilization.

系统地研究了精确调整Zn浓度梯度（α = 0.1 ~ 0.9）的pdzn - α zrox系列等离子体催化CO2加氢催化剂。PdZn0.3ZrOx的CO2转化率最高，达51.5%，而PdZn0.7ZrOx的CO收率最高，达45.4%，选择性超过95%。这些性能即使在H2/CO2的摩尔比为3:1的情况下也能得到，这是一个典型的有利于甲烷化的条件。表征表明，PdZn合金和ZnZrOx之间的协同作用是决定反应途径的关键。PdZn合金增强了PdZr相互作用，产生了丰富的氧空位（Ov），有效地激活了CO2形成bi-CO32−。这种中间体倾向于氢化成双hcoo−，而双hcoo−随后会分解成CO β或氢化成CH4。PdZn合金减弱了CO的吸附强度，促进了CO的解吸，从而提高了CO的选择性。当α >； 0.3时，过量的Zn与Zr相互作用形成ZnZrOx。该相不仅可以防止过量的Zn聚集成覆盖Ov的ZnO，还可以稳定ZrO2的氢溢出物质，抑制bi-HCOO−加氢成CH4，并使反应转向CO生成。通过利用这种协同效应，pdzn - α - zrox催化剂以CO为主要产物实现了40%以上的CO2转化率，提出了一种新的等离子体催化策略，克服了传统的水气倒转反应中对CO2利用的活性-选择性权衡。

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引用次数: 0

Titanium ion sieves utilize flow electrode capacitive deionization technology to achieve efficient lithium extraction 钛离子筛采用流动电极电容去离子技术，实现高效的锂提取

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-01-31 DOI: 10.1016/j.seppur.2026.137065

Zhaoyang Song , Xuewen Wu , Qiongqiong He , Junhan Huyan , Ruize Gao , Xiaoqi Wu , Zhenyong Miao

Lithium (Li) is an indispensable strategic resource for modern societal development. The advancement of efficient and synergistic lithium ion (Li⁺) extraction and separation technologies is of major strategic importance. This study employed flow-electrode capacitive deionization (FCDI) to enhance the Li⁺ adsorption performance of titanium ion sieve (HTO-650) for the first time. In alkaline solution, the electroadsorption behavior of HTO-650 was primarily governed by the capacitive deionization (CDI) effect, achieving an electroadsorption amount of 62.54 mg/g, which is 2.08 times that of static adsorption. Electrodialysis (ED) achieved preliminary separation of Li⁺/Na⁺ with a selectivity of 1.47, while subsequent CDI enhanced the selectivity to 5.00, enabling a two-stage separation process. The FCDI can be decoupled into two sub-processes: CDI and ED. During FCDI, Li⁺ migrates from the feed solution to the cathodic flow electrode (CFE) driven by ED, and is subsequently adsorbed into HTO-650 by CDI. A decrease in Li⁺ amount within the CFE (by 6.46 mg) indicated the predominance of the CDI effect, demonstrating the excellent electroadsorption performance of HTO-650 in the FCDI. Molecular dynamics simulations revealed that under an electric field, Li⁺ undergoes rapid dehydration, Li⁺/H⁺ exchange, and diffusion into the interlayers of HTO-650, resulting in a significant increase in its diffusion coefficient from 3.52 to 249 Å/ps. This integrated technology remarkably improves Li⁺ adsorption amount and provides a theoretical foundation for efficient Li⁺ separation.

锂是现代社会发展不可缺少的战略资源。高效、协同的锂离子萃取分离技术的发展具有重要的战略意义。本研究首次采用流动电极电容去离子（FCDI）技术提高钛离子筛（HTO-650）对Li+的吸附性能。在碱性溶液中，HTO-650的电吸附行为主要受电容去离子（CDI）效应支配，电吸附量为62.54 mg/g，是静态吸附量的2.08倍。电渗析（ED）实现了Li+/Na+的初步分离，其选择性为1.47，而随后的CDI将选择性提高到5.00，实现了两段分离过程。FCDI可解耦为两个子过程：CDI和ED。在FCDI过程中，Li+从进料溶液迁移到ED驱动的阴极流电极（CFE），随后被CDI吸附到HTO-650中。CFE内Li+的减少量为6.46 mg，表明CDI效应占主导地位，表明HTO-650在FCDI中具有良好的电吸附性能。分子动力学模拟结果表明，在电场作用下，Li+发生快速脱水、Li+/H+交换并扩散到HTO-650的层间，导致其扩散系数从3.52显著增加到249 Å/ps。该综合技术显著提高了锂离子吸附量，为高效分离锂离子提供了理论基础。

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引用次数: 0

Machine learning-driven doping optimization: Enhancing structural stability of Mn-based ion sieves for Lithium extraction from brine 机器学习驱动的掺杂优化：提高锰基离子筛从盐水中提取锂的结构稳定性

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137214

Zhiai Huang , Luri Bao , Xiaorong Qu , Ting Wei , Shu-Ying Sun

Manganese-based adsorbents are a key technology for lithium extraction from salt-lake brines, but they suffer from Mn dissolution. Conventional dopant screening relies on trial-and-error methods, which are both time-consuming and costly. Here, we develop a machine learning (ML) model to predict the effects of 16 metallic dopants on Li_1.6Mn_1.6O₄ adsorbents. To integrate literature data with our laboratory dataset, we employed the ComBat method to correct for batch effects, thereby enabling robust predictions based on limited data. SHAP analysis reveals that electronegativity (En), dopant loading (ratio), and melting point (m.p.) are the key features governing Mn dissolution. Experiments confirmed that Sr and Nd doping reduced the Mn dissolution rate to 1.27% and 1.03%, respectively, and the modified adsorbent maintained excellent cycling stability after 6 cycles. This data-driven workflow accelerates the screening of dopants and provides actionable guidance for mitigating Mn dissolution issues

锰基吸附剂是盐湖卤水提锂的关键技术，但锰基吸附剂存在锰溶解的问题。传统的掺杂剂筛选依赖于反复试验的方法，既耗时又昂贵。在这里，我们开发了一个机器学习（ML）模型来预测16种金属掺杂剂对Li1.6Mn1.6O4吸附剂的影响。为了将文献数据与我们的实验室数据集整合，我们采用ComBat方法来校正批处理效应，从而实现基于有限数据的稳健预测。SHAP分析表明，电负性（En）、掺杂量（比率）和熔点（m.p）是影响锰溶解的关键特征。实验证实，Sr和Nd的掺杂使Mn的溶解率分别降低到1.27%和1.03%，改性吸附剂在6次循环后仍保持良好的循环稳定性。这种数据驱动的工作流程加速了掺杂剂的筛选，并为减轻锰溶解问题提供了可行的指导

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引用次数: 0

Construction of long-lived Ti/TiN/RuO2/PbO2 anode with a heterogeneous interlayer for efficient electro-oxidative degradation of metformin 具有非均相中间层的Ti/TiN/RuO2/PbO2长寿命阳极的构建用于二甲双胍的高效电氧化降解

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137218

Changbin Tang , Shihua Wang , Wei Li , Zhigang Li , Lihua Yu , Juanqin Xue , Xiangyang Yin , Nan Zheng

To obtain long-lived titanium-based lead dioxide coating anodes for efficient electro-oxidative degradation of the emerging aquatic pollutant metformin (MET), Ti/TiN/RuO₂/PbO₂ anodes were fabricated by introducing a composite interlayer through loading a small amount of RuO₂ onto an arc-sprayed TiN surface. Comparative analyses of the structure, electrochemical performance, and stability of anodes with different RuO₂ loadings were conducted, followed by optimization of MET electro-oxidative degradation parameters and analysis of the underlying mechanisms. The fabricated Ti/TiN/RuO₂/PbO₂ anodes with a heterointerfacial structure exhibited excellent stability and a long service life (current density: 1 A/cm², 579 h), which was almost twice that of the Ti/TiN/PbO₂ anode and 16.1-fold higher than the Ti/PbO₂ anode without an interlayer. Most importantly, the Ti/TiN/RuO₂/PbO₂ anode effectively removed MET, achieving 72% electro-oxidative degradation of 300 mg/L MET within 3 h under optimal degradation conditions (temperature: 30 °C, pH 7, current density: 40 mA/cm²). The degradation rate was further enhanced to 77% in medium containing 7 mmol/L Cl⁻, indicating the anode's compatibility with Cl⁻ ions. Furthermore, electrochemical testing, electron paramagnetic resonance spectroscopy, and quenching experiments confirmed that highly reactive non-radical singlet oxygen (¹O₂) played a primary role in MET degradation. Superoxide radicals (O₂·⁻) and direct oxidation made secondary contributions, but involvement of hydroxyl radicals (HO) was negligible. The developed long-lasting, highly efficient anode has promise for electro-oxidative water treatment, and may facilitate degradative removal of MET and other pollutants.

为了获得长寿命的钛基二氧化铅涂层阳极，以高效电氧化降解新兴的水生污染物二甲双胍（MET），通过在电弧喷涂的TiN表面上加载少量RuO2，引入复合中间层制备Ti/TiN/RuO2/PbO2阳极。对比分析了不同RuO2负荷量的阳极的结构、电化学性能和稳定性，优化了MET电氧化降解参数，并分析了其机理。制备的具有异质界面结构的Ti/TiN/RuO2/PbO2阳极具有优异的稳定性和较长的使用寿命（电流密度：1 a /cm2, 579 h），几乎是Ti/TiN/PbO2阳极的两倍，比没有夹层的Ti/PbO2阳极高16.1倍。最重要的是，Ti/TiN/RuO2/PbO2阳极有效地去除了MET，在最佳降解条件（温度：30℃，pH: 7，电流密度：40 mA/cm2）下，3小时内对300 mg/L的MET进行了72%的电氧化降解。在含有7 mmol/L Cl−的介质中，降解率进一步提高到77%，表明阳极与Cl−离子的相容性。此外，电化学测试、电子顺磁共振波谱和淬火实验证实，高活性的非自由基单线态氧（1O2）在MET降解中起主要作用。超氧自由基（O2·−）和直接氧化是次要作用，而羟基自由基（HO）的作用可以忽略不计。所开发的长效、高效阳极有望用于电氧化水处理，并有助于降解去除MET和其他污染物。

{"title":"Construction of long-lived Ti/TiN/RuO2/PbO2 anode with a heterogeneous interlayer for efficient electro-oxidative degradation of metformin","authors":"Changbin Tang , Shihua Wang , Wei Li , Zhigang Li , Lihua Yu , Juanqin Xue , Xiangyang Yin , Nan Zheng","doi":"10.1016/j.seppur.2026.137218","DOIUrl":"10.1016/j.seppur.2026.137218","url":null,"abstract":"<div><div>To obtain long-lived titanium-based lead dioxide coating anodes for efficient electro-oxidative degradation of the emerging aquatic pollutant metformin (MET), Ti/TiN/RuO2/PbO2 anodes were fabricated by introducing a composite interlayer through loading a small amount of RuO2 onto an arc-sprayed TiN surface. Comparative analyses of the structure, electrochemical performance, and stability of anodes with different RuO2 loadings were conducted, followed by optimization of MET electro-oxidative degradation parameters and analysis of the underlying mechanisms. The fabricated Ti/TiN/RuO2/PbO2 anodes with a heterointerfacial structure exhibited excellent stability and a long service life (current density: 1 A/cm2, 579 h), which was almost twice that of the Ti/TiN/PbO2 anode and 16.1-fold higher than the Ti/PbO2 anode without an interlayer. Most importantly, the Ti/TiN/RuO2/PbO2 anode effectively removed MET, achieving 72% electro-oxidative degradation of 300 mg/L MET within 3 h under optimal degradation conditions (temperature: 30 °C, pH 7, current density: 40 mA/cm2). The degradation rate was further enhanced to 77% in medium containing 7 mmol/L Cl−, indicating the anode's compatibility with Cl− ions. Furthermore, electrochemical testing, electron paramagnetic resonance spectroscopy, and quenching experiments confirmed that highly reactive non-radical singlet oxygen (1O2) played a primary role in MET degradation. Superoxide radicals (O2·−) and direct oxidation made secondary contributions, but involvement of hydroxyl radicals (HO<img>) was negligible. The developed long-lasting, highly efficient anode has promise for electro-oxidative water treatment, and may facilitate degradative removal of MET and other pollutants.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137218"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172557","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

Boosting photothermal mineralization of toluene by Fe2O3/Co3O4 p-n heterojunctions: Accelerating activation of oxygen species through interfacial coupling effect Fe2O3/Co3O4 p-n异质结促进甲苯的光热矿化：通过界面耦合效应加速氧的活化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-08 DOI: 10.1016/j.seppur.2026.137166

Yi Liu , Guangmei Gan , Juyuan Xing, Junting Wang, Yuan Li, Gaoke Zhang

The effective activation of oxygen species through the interface coupling effect of catalysts to achieve photothermal toluene mineralization remains a major challenge. Herein, a p-n heterojunction catalyst composed of Co₃O₄ and Fe₂O₃ with strong interfacial coupling effect was rationally synthesized to overcome the intrinsic limitations, thereby achieving efficient photothermal mineralization of toluene. Under full-spectrum irradiation (350 mW/cm²), the Fe₂O₃/Co₃O₄ (0.15-FCO) p-n heterojunction achieved a toluene conversion rate of 99.72% and a CO₂ yield of 87.94%, outperforming individual oxides. Comprehensive structural analysis show that the heterojunction formation elongated and weakened the CoO bond induced by Fe₂O₃, thereby exposing Co³⁺ sites and promoting the generation of oxygen vacancies. Benefiting from interfacial coupling effect triggered by electronic modulation, 0.15-FCO enhances the adsorption and activation of O₂ and toluene as further corroborated by DFT calculations. Besides, the appropriate band potentials of the p-n heterojunction facilitated charge carrier migration and activation of molecular oxygen. The results of in-situ DRIFTS further demonstrate that the incorporation of Fe₂O₃ promotes the oxidative conversion of intermediates on Co₃O₄ through interfacial charge transfer and sustaining active oxygen species generation. Overall, this study highlights that strengthening interfacial coupling in oxide materials is a viable strategy for efficient photothermal VOCs oxidation.

如何通过催化剂的界面偶联效应有效活化氧来实现甲苯的光热矿化仍然是一个重要的挑战。本文合理合成了具有强界面耦合效应的Co3O4和Fe2O3组成的p-n异质结催化剂，克服了其固有的局限性，实现了甲苯的高效光热矿化。在350 mW/cm2全光谱辐照下，Fe2O3/Co3O4 (0.15-FCO) p-n异质结的甲苯转化率为99.72%，CO2产率为87.94%，优于单一氧化物。综合结构分析表明，异质结的形成拉长并削弱了Fe2O3诱导的CoO键，从而暴露了Co3+位点，促进了氧空位的生成。利用电子调制引发的界面耦合效应，0.15-FCO增强了对O2和甲苯的吸附和活化，DFT计算进一步证实了这一点。此外，适当的p-n异质结能带电位有利于载流子迁移和分子氧的活化。原位漂移的结果进一步表明，Fe2O3的加入通过界面电荷转移和维持活性氧的生成，促进了中间体在Co3O4上的氧化转化。总之，本研究强调了加强氧化物材料中的界面耦合是有效光热氧化VOCs的可行策略。

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引用次数: 0

Analysis of ion forces in the process of enhancing NH4+ recovery by magnetic flow electrode capacitive deionization (MF-FCDI) 磁流电极电容去离子（MF-FCDI）提高NH4+回收率过程中的离子力分析

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-05 DOI: 10.1016/j.seppur.2026.137133

Mengyao Han , Xiaoxuan Chen , Jiayuan Zhang , Jianrui Niu , Situ Mu , Yongkun Shi , Jing Zhang , Chun Liu , Junjun Ma

Flow-electrode capacitive deionization (FCDI) is a promising technology for the energy-efficient recovery of valuable resources like NH₄⁺ from wastewater. While progress has been made using magnetic carbon (MC) electrodes, current research has predominantly focused on the magnetic manipulation of the MC particles themselves, largely neglecting the direct influence of the magnetic field on ion migration. Consequently, a systematic investigation into the optimization of magnetic field configurations, coupled with a quantitative force analysis of NH₄⁺ transport, remains notably absent. This gap hinders the development of strategies for precisely regulating ion trajectories to enhance system performance. Herein, we systematically investigate the influence of magnetic field orientation, position, and intensity on NH₄⁺ migration in a magnetic FCDI system (MF-FCDI). Our analysis reveals that the magnetic field, through the Lorentz force, synergistically acts with the electric field and the hydrodynamic drag force to modulate ion trajectories and accelerate migration. Under optimized conditions that 220 mT field applied centrally to the cathode side with MC (Fe:C = 1:1), the system achieved a superior average salt removal rate (ASRR) of 0.311 μmol·cm⁻² min⁻¹ and energy-normalized salt removal (ENRS) of 4.61 μmol·J⁻¹. This work presents a magnetically-assisted strategy that enables both efficient NH₄⁺ recovery and facile electrode separation.

流动电极电容去离子（FCDI）是一种有前途的高效回收废水中有价值资源如NH4+的技术。虽然磁性碳（MC）电极的研究取得了一定的进展，但目前的研究主要集中在磁性碳粒子本身的磁操纵上，而很大程度上忽略了磁场对离子迁移的直接影响。因此，对磁场结构优化的系统研究，以及对NH4+输运的定量力分析，仍然明显缺乏。这种差距阻碍了精确调节离子轨迹以提高系统性能的策略的发展。本文系统地研究了磁场方向、位置和强度对磁性FCDI系统（MF-FCDI）中NH4+迁移的影响。我们的分析表明，磁场通过洛伦兹力与电场和流体动力阻力协同作用，调节离子轨迹并加速迁移。在MC （Fe:C = 1:1）、220 mT电场集中施加于阴极侧的优化条件下，体系的平均脱盐率（ASRR）为0.311 μmol·cm−2 min−1，能量归一化脱盐率（ENRS）为4.61 μmol·J−1。这项工作提出了一种磁辅助策略，使有效的NH4+回收和易于电极分离。

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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 : 2026-06-19 Epub 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

Synthesis of sodium alginate composite aerogels for simultaneous adsorption of Cr(VI) and malachite green 同时吸附Cr（VI）和孔雀石绿的海藻酸钠复合气凝胶的合成

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-11 DOI: 10.1016/j.seppur.2026.137227

Bingxiang Wang , Ruiyu Mao , Hui Luan , Hang Lu , Jianze Feng , Yuzhong Niu , Hou Chen

Water contamination caused by heavy metal ions and organic dyes poses a serious threat to environmental safety and human health. The development of efficient adsorbents is critical for the remediation of water pollution through adsorption method. In this project, a series of amino and thiol-functionalized silica/graphene oxide/sodium alginate composite aerogels were constructed for simultaneous capturing Cr(VI) and malachite green (MG) from aqueous solutions. The aerogels exhibit low density, ultrahigh porosity, excellent mechanical properties and adsorption performance. The maximum adsorption capacity for Cr(VI) and MG are 61.73 mg·g⁻¹ (pH = 2, T = 25 °C and C₀ = 52.00 mg·L⁻¹) and 1111.11 mg·g⁻¹ (pH = 10, T = 25 °C and C₀ = 1000 mg·L⁻¹), respectively. The adsorption kinetic and isotherm process can be fitted by pseudo-second-order model and Langmuir model, respectively. The as-prepared composite aerogels can simultaneously remove Cr(VI) and MG from pure water and high saline environments. They also exhibit excellent adsorption selectivity toward Cr(VI) and MG. The as-prepared composite aerogels also display competitive adsorption and regeneration performance as compared with other adsorbents. The regeneration rates can maintain 91.43% and 89.85% after five adsorption-desorption cycles for Cr(VI) and MG. This study provides a promising strategy for the synthesis of novel adsorbents for the synergistical and efficient removal of Cr(VI) and MG from aqueous systems.

重金属离子和有机染料引起的水污染对环境安全和人体健康构成严重威胁。高效吸附剂的开发是利用吸附法修复水污染的关键。在本项目中，构建了一系列氨基和巯基功能化二氧化硅/氧化石墨烯/海藻酸钠复合气凝胶，用于同时捕获水溶液中的Cr（VI）和孔雀石绿（MG）。该气凝胶具有低密度、超高孔隙率、优异的力学性能和吸附性能。对Cr（VI）和MG的最大吸附量分别为61.73 MG·g−1 （pH = 2, T = 25℃，C0 = 52.00 MG·L−1）和1111.11 MG·g−1 （pH = 10, T = 25℃，C0 = 1000 MG·L−1）。吸附动力学和等温过程可分别用拟二阶模型和Langmuir模型拟合。所制备的复合气凝胶可以同时去除纯水和高盐环境中的Cr（VI）和MG。对Cr（VI）和MG也有很好的吸附选择性。与其他吸附剂相比，所制备的复合气凝胶具有较强的吸附和再生性能。经过5次吸附-解吸循环后，Cr（VI）和MG的再生率分别保持在91.43%和89.85%。本研究为新型吸附剂的合成提供了一个有希望的策略，以协同和有效地去除水系统中的Cr（VI）和MG。

{"title":"Synthesis of sodium alginate composite aerogels for simultaneous adsorption of Cr(VI) and malachite green","authors":"Bingxiang Wang , Ruiyu Mao , Hui Luan , Hang Lu , Jianze Feng , Yuzhong Niu , Hou Chen","doi":"10.1016/j.seppur.2026.137227","DOIUrl":"10.1016/j.seppur.2026.137227","url":null,"abstract":"<div><div>Water contamination caused by heavy metal ions and organic dyes poses a serious threat to environmental safety and human health. The development of efficient adsorbents is critical for the remediation of water pollution through adsorption method. In this project, a series of amino and thiol-functionalized silica/graphene oxide/sodium alginate composite aerogels were constructed for simultaneous capturing Cr(VI) and malachite green (MG) from aqueous solutions. The aerogels exhibit low density, ultrahigh porosity, excellent mechanical properties and adsorption performance. The maximum adsorption capacity for Cr(VI) and MG are 61.73 mg·g−1 (pH = 2, T = 25 °C and C0 = 52.00 mg·L−1) and 1111.11 mg·g−1 (pH = 10, T = 25 °C and C0 = 1000 mg·L−1), respectively. The adsorption kinetic and isotherm process can be fitted by pseudo-second-order model and Langmuir model, respectively. The as-prepared composite aerogels can simultaneously remove Cr(VI) and MG from pure water and high saline environments. They also exhibit excellent adsorption selectivity toward Cr(VI) and MG. The as-prepared composite aerogels also display competitive adsorption and regeneration performance as compared with other adsorbents. The regeneration rates can maintain 91.43% and 89.85% after five adsorption-desorption cycles for Cr(VI) and MG. This study provides a promising strategy for the synthesis of novel adsorbents for the synergistical and efficient removal of Cr(VI) and MG from aqueous systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137227"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153027","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

La-doped HKUST-1-derived catalysts for stable and selective CO2-to-CH4 conversion via Cu oxidation state stabilization la掺杂hkust -1衍生催化剂通过Cu氧化态稳定实现稳定和选择性的co2 - ch4转化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137210

Zekun Zhang, Jiqun Li, Luping Zhang, Xixue He, Hao Xu, Wei Yan

During the electrocatalytic CO₂ reduction (ECO₂R) process, the active oxidation states of Cu-based catalysts (e.g., Cu⁺) are unstable and prone to reduction to metallic Cu (Cu⁰), leading to decreased product selectivity and catalyst stability. To address this issue, this study proposed a catalyst design strategy involving lanthanum (La) doping to stabilize Cu oxidation states. Using typical Cu₃(BTC)₂ (HKUST-1) as a precursor, a series of x La/HKUST-1 materials with varying La doping levels were synthesized via a wet-chemical method, followed by electrochemical activation to obtain A-x La/HKUST-1 derived catalysts. Characterization revealed that appropriate La doping (Cu:La = 8:1) effectively modulated the electronic structure around Cu, suppressing its excessive reduction during the reaction and promoting the formation and stabilization of active Cu⁺ sites. Electrochemical performance tests in an H-cell demonstrated that A-0.1 La/HKUST-1 achieved a CH₄ Faradaic efficiency (FE_CH4) of 60.81% with a corresponding partial current density of −25.93 mA·cm⁻² at −1.37 V (vs. reversible hydrogen electrode (RHE)), significantly outperforming other catalysts. Furthermore, this catalyst exhibited excellent stability during a 24-h continuous test, maintaining an FE_CH4 above 55%. This research provides a novel material design concept and mechanistic insight for enhancing the CO₂ methanation pathway by stabilizing Cu oxidation states via rare-earth La doping.

在电催化CO2还原（ECO2R）过程中，Cu基催化剂（如Cu+）的活性氧化态不稳定，容易还原为金属Cu (Cu0)，导致产物选择性和催化剂稳定性下降。为了解决这一问题，本研究提出了一种涉及镧（La）掺杂的催化剂设计策略来稳定Cu的氧化态。以典型的Cu3(BTC)2 （HKUST-1）为前驱体，通过湿化学方法合成了一系列不同La掺杂水平的x La/HKUST-1材料，然后通过电化学活化得到a -x La/HKUST-1衍生催化剂。表征表明，适当的La掺杂（Cu:La = 8:1）可以有效调节Cu周围的电子结构，抑制其在反应过程中的过度还原，促进活性Cu+位点的形成和稳定。在h电池中的电化学性能测试表明，a -0.1 La/HKUST-1在−1.37 V（相对于可逆氢电极（RHE））下，CH4法拉第效率（FECH4）为60.81%，相应的分电流密度为−25.93 mA·cm−2，显著优于其他催化剂。此外，该催化剂在24小时连续测试中表现出优异的稳定性，将FECH4保持在55%以上。该研究为通过稀土La掺杂稳定Cu氧化态来增强CO2甲烷化途径提供了一种新的材料设计理念和机理见解。

{"title":"La-doped HKUST-1-derived catalysts for stable and selective CO2-to-CH4 conversion via Cu oxidation state stabilization","authors":"Zekun Zhang, Jiqun Li, Luping Zhang, Xixue He, Hao Xu, Wei Yan","doi":"10.1016/j.seppur.2026.137210","DOIUrl":"10.1016/j.seppur.2026.137210","url":null,"abstract":"<div><div>During the electrocatalytic CO2 reduction (ECO2R) process, the active oxidation states of Cu-based catalysts (e.g., Cu+) are unstable and prone to reduction to metallic Cu (Cu0), leading to decreased product selectivity and catalyst stability. To address this issue, this study proposed a catalyst design strategy involving lanthanum (La) doping to stabilize Cu oxidation states. Using typical Cu3(BTC)2 (HKUST-1) as a precursor, a series of x La/HKUST-1 materials with varying La doping levels were synthesized via a wet-chemical method, followed by electrochemical activation to obtain A-x La/HKUST-1 derived catalysts. Characterization revealed that appropriate La doping (Cu:La = 8:1) effectively modulated the electronic structure around Cu, suppressing its excessive reduction during the reaction and promoting the formation and stabilization of active Cu+ sites. Electrochemical performance tests in an H-cell demonstrated that A-0.1 La/HKUST-1 achieved a CH4 Faradaic efficiency (FECH4) of 60.81% with a corresponding partial current density of −25.93 mA·cm−2 at −1.37 V (vs. reversible hydrogen electrode (RHE)), significantly outperforming other catalysts. Furthermore, this catalyst exhibited excellent stability during a 24-h continuous test, maintaining an FECH4 above 55%. This research provides a novel material design concept and mechanistic insight for enhancing the CO2 methanation pathway by stabilizing Cu oxidation states via rare-earth La doping.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137210"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153688","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