Separation and Purification Technology最新文献

Ceramic-based graphene oxide/ultrafine activated carbon hybrid oil-water separation membrane 陶瓷基氧化石墨烯/超细活性炭杂化油水分离膜

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.2026.137006

Anwen Chen , Dong Zhan , Razium A. Soomro , Ning Qiao , Xiaojie Zhang , Bin Xu

Graphene oxide (GO)-based membranes have brought great research interest and wide application prospects in the field of oil-in-water emulsion separation by virtue of their unique properties. However, the rational design of the rough structure of the membrane surface and the exploration of the stability of the prepared membranes are still insufficient, which greatly limits the possibility of their survival in practical use. In this study, GO with larger lamellar size, ultrafine activated carbon (UAC) particles, and polyvinyl alcohol (PVA) as adhesive were compounded to form a membrane on the (3-aminopropyl) triethoxysilane (APTES) pretreated ceramic support by vacuum filtration. The composite membrane exhibits superb oil-repellent properties (underwater oil contact angle up to 162.6°) and very low oil adhesion underwater, while providing better mechanical strength and stability than porous polymer-supported membranes. After the GO sheets cover the UAC particles and form the membrane, the GO sheets generate micron-scale bumps with UAC spatial contours and nanoscale secondary folds due to the bending deformation of the GO sheets. The good combination of these structures endows the membrane with an excellent graded rough surface structure. On the surface of the membrane, it is possible to prepare two rough structures using only one material, the GO sheet. The intercalation of UAC particles resulted in a 72.6-fold increase in pure water flux to 94.38 L·m⁻²·h⁻¹ compared to pure GO membranes, while providing excellent separation performance and resistance to contamination (14.6% flux decline ratio and 95.7% flux recovery ratio while maintaining >99% emulsion removal). Moreover, adding PVA provided better mechanical strength and anti-swelling properties for the membrane, and the ceramic support pretreated with APTES had better bonding strength with the GO laminate. This study inspires the surface microscopic design of GO-based oil-in-water emulsion separation membranes and new ideas for preparing GO-based membranes with practical prospects, high throughput, and good antifouling properties.

氧化石墨烯膜以其独特的性能在油水乳液分离领域引起了极大的研究兴趣和广阔的应用前景。然而，对膜表面粗糙结构的合理设计和对所制备膜稳定性的探索仍然不足，这极大地限制了其在实际应用中生存的可能性。本研究将层状尺寸较大的氧化石墨烯与超细活性炭（UAC）颗粒、聚乙烯醇（PVA）作为粘合剂复合，通过真空过滤在（3-氨基丙基）三乙氧基硅烷（APTES）预处理陶瓷载体上形成膜。复合膜具有优异的拒油性能（水下油接触角高达162.6°）和极低的水下油附着力，同时具有比多孔聚合物支撑膜更好的机械强度和稳定性。当氧化石墨烯薄片覆盖在UAC颗粒上形成膜后，由于氧化石墨烯薄片的弯曲变形，氧化石墨烯薄片会产生具有UAC空间轮廓的微米尺度凸起和纳米尺度的二次褶皱。这些结构的良好结合使膜具有优异的梯度粗糙表面结构。在膜的表面，仅使用一种材料，氧化石墨烯片，就可以制备两个粗糙的结构。与纯氧化石墨烯膜相比，UAC颗粒的插入使纯水通量增加了72.6倍，达到94.38 L·m−2·h−1，同时具有优异的分离性能和抗污染能力（通量下降率为14.6%，通量回收率为95.7%，同时保持99%的乳液去除率）。此外，PVA的加入使膜具有更好的机械强度和抗膨胀性能，APTES预处理的陶瓷支架与氧化石墨烯层压板的结合强度更好。本研究为氧化石墨烯基水包油乳化液分离膜的表面微观设计提供了新的思路，为制备具有实用前景、高通量、良好防污性能的氧化石墨烯基分离膜提供了新的思路。

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引用次数: 0

Synergistic effect of filler sieving and polymer rigidification for selective C2H4/C2H6 separation 填料筛分和聚合物固化对C2H4/C2H6选择性分离的协同作用

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-07 DOI: 10.1016/j.seppur.2026.137196

Linxuan Han, Yutao Liu, Dongxiao Yang, Jian Tan, Chao Zhi, Yang Chen, Jinping Li, Libo Li

Membrane separation technology on account of low energy consumption shows great potential for energy-intensive C₂H₄/C₂H₆ separation. Mixed matrix membranes (MMMs), fabricated by embedding sieving functional fillers within polymer, are expected to improve the separation performance of conventional polymer. However, most MMMs fail to deliver the anticipated gains in C₂H₄/C₂H₆ separation selectivity. Sieving fillers typically have ultra-small pores that may impose higher entry barriers on polarizable hydrocarbons than the dynamic free-volume elements of polymers. Thus, focus should extend beyond the filler itself to the structural variations of the polymer matrix upon filler incorporation. In this work, we incorporated an C₂H₄/C₂H₆ sieving metal-organic framework material, Cu(BF₄)₂(4-DPDS)₂, into 6FDA-DAM to fabricate MMMs for C₂H₄/C₂H₆ separation. It is found that the size sieving ability of Cu(BF₄)₂(4-DPDS)₂ contributes partially to the improved C₂H₄/C₂H₆ diffusion selectivity. Additionally, the rigidification of 6FDA-DAM molecular chains induced by the strong interfacial interaction markedly hinders C₂H₆ transport. These two factors act synergistically to effectively enhance the C₂H₄/C₂H₆ diffusion selectivity. For an equimolar gas mixture, the filler-optimized MMMs exhibit a C₂H₄ permeability of 13.35 barrer and a C₂H₄/C₂H₆ selectivity of 7.02, exceeding the separation upper bound reported in 2013 and representing the highest selectivity reported for sieving-filler-based MMMs. This work provides valuable insights for the rational design of high-performance MMMs for ethylene/ethane separation.

膜分离技术由于能耗低，在高耗能的C2H4/C2H6分离中显示出巨大的潜力。混合基质膜（MMMs）是通过在聚合物中嵌入筛分功能填料来制备的，有望改善传统聚合物的分离性能。然而，大多数mm无法提供C2H4/C2H6分离选择性的预期增益。筛分填料通常具有超小的孔隙，与聚合物的动态自由体积元素相比，可能对极化碳氢化合物施加更高的进入障碍。因此，重点应超越填料本身延伸到填料掺入后聚合物基体的结构变化。在这项工作中，我们将C2H4/C2H6筛选金属有机骨架材料Cu(BF4)2(4-DPDS)2加入到6FDA-DAM中，制备了用于C2H4/C2H6分离的MMMs。结果表明，Cu(BF4)2(4-DPDS)2的筛分能力是提高C2H4/C2H6扩散选择性的部分原因。此外，强界面相互作用诱导的6FDA-DAM分子链硬化明显阻碍了C2H6的转运。这两个因素协同作用，有效提高了C2H4/C2H6的扩散选择性。对于等摩尔气体混合物，填料优化的MMMs的C2H4渗透率为13.35，C2H4/C2H6选择性为7.02，超过了2013年报道的分离上限，代表了基于筛分填料的MMMs的最高选择性。这项工作为合理设计用于乙烯/乙烷分离的高性能mm材料提供了有价值的见解。

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引用次数: 0

Morphological impact of Ni-based electrodes (solid Ni sheets vs. Ni-assisted W meshes) on Lu(III) electrochemical behavior and efficient extraction mechanism in LiCl-KCl molten salts Ni基电极（固体Ni片vs. Ni辅助W网）形态对Lu（III）在LiCl-KCl熔盐中的电化学行为及有效萃取机理的影响

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.2026.137150

Jiacheng Li , Ji Wang , Peidong He , Junyang Shu , Jinshuo Yang , Wenlong Li , Xiangbiao Yin , Deqian Zeng , Qiang Wu , Yuezhou Wei

Spent nuclear fuel dry reprocessing demands efficient recovery of valuable rare-earth elements, yet its extraction from complex LiCl-KCl molten salt matrices remains challenging. This study investigates the electrochemical behaviors and underlying mechanism of Lu(III) in LiCl-KCl molten salts, with a focus on its efficient extraction via Ni-based systems. The electrochemical behavior of Lu(III) on W and Ni-assisted W electrodes using various electrochemical methods was studied. On W electrodes, cyclic voltammetry (CV), square wave voltammetry (SWV), and chronopotentiometry (CP) measurements yielded the diffusion coefficient of Lu(III) in the salt, while comparison with the Scharifker-Hill model confirmed that Lu nucleation follows a three-dimensional instantaneous mechanism, and thermodynamic data of Lu(III)/Lu(0) were calculated. For Ni-assisted W electrodes, different techniques identified LuNi intermetallic compounds, with subsequent computation of the thermodynamic parameters of LuNi alloys. A comparative extraction efficiency of Lu across cathode configurations showed that the Ni-assisted W electrodes exhibited the highest efficiency, attributed to their larger specific surface area. XRD and SEM-EDS analysis were conducted on the alloy products.

乏燃料干式后处理要求有效回收有价值的稀土元素，但从复杂的LiCl-KCl熔盐基质中提取仍具有挑战性。本研究研究了Lu（III）在LiCl-KCl熔盐中的电化学行为和潜在机理，重点研究了ni基体系对Lu（III）的高效萃取。采用不同的电化学方法研究了Lu（III）在W和ni辅助W电极上的电化学行为。在W电极上，通过循环伏安法（CV）、方波伏安法（SWV）和时间电位法（CP）测量得到了Lu（III）在盐中的扩散系数，并与Scharifker-Hill模型进行了对比，证实了Lu(III)/Lu(0)的三维瞬时成核机制，计算了Lu(III)/Lu(0)的热力学数据。对于ni辅助W电极，采用不同的技术鉴定了LuNi金属间化合物，并计算了LuNi合金的热力学参数。不同阴极结构对Lu的萃取效率的比较表明，ni辅助W电极由于其更大的比表面积而表现出最高的萃取效率。对合金制品进行了XRD和SEM-EDS分析。

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引用次数: 0

Advancements in solar still performance enhancement through heat pipes, evacuated tubes, and pulsating heat pipes: a comprehensive review 通过热管、真空管和脉动热管提高太阳能蒸馏器性能的进展：综合综述

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.2026.137159

Jay R. Patel, Y. Naresh

Addressing water scarcity and improving the quality of life in arid and semi-arid regions necessitates the development of sustainable freshwater production technologies. Among them, solar stills offer a simple and eco-friendly solution by converting saline water into potable water using only solar radiation. However, their productivity remains significantly lower compared to conventional desalination methods, prompting extensive research into performance enhancement strategies. Various augmentation techniques—including nanofluids, phase change materials (PCMs), sensible heat storage, and heat pipes—have been investigated to overcome these limitations. The novelty of this review lies in its comprehensive bibliometric and in-depth technical analysis of heat pipe-assisted solar stills over a 25-year period (2000–2025), integrating both evacuated tube and pulsating heat pipe configurations. Unlike earlier reviews, this study quantitatively correlates research trends with system-level advancements—particularly in energy storage, phase change material integration, and hybrid enhancement techniques—to establish a clear roadmap for the next generation of high-performance solar desalination systems. The analysis highlights year-wise publication growth, geographical and journal-wise contributions, and keyword co-occurrence networks, where emerging themes include energy storage, heat exchanger, water depth, and phase change material. Recent advances in evacuated tube-based collectors and their performance under varying operating parameters are systematically examined, along with detailed discussions on pulsating heat pipe (PHP)-integrated solar stills. Furthermore, the review outlines the comparative benefits, limitations, and challenges of these technologies, offering critical insights to guide the development of next-generation solar desalination systems with improved efficiency, reliability, and economic feasibility.

要解决干旱和半干旱地区的缺水问题和提高生活质量，就必须发展可持续的淡水生产技术。其中，太阳能蒸馏器提供了一种简单而环保的解决方案，它只利用太阳辐射将盐水转化为饮用水。然而，与传统的海水淡化方法相比，它们的生产率仍然明显较低，这促使人们对性能增强策略进行了广泛的研究。各种增强技术——包括纳米流体、相变材料（PCMs）、显热存储和热管——已经被研究以克服这些限制。这篇综述的新颖之处在于它对热管辅助太阳能蒸馏器进行了全面的文献计量和深入的技术分析，超过25年的时间（2000-2025），整合了真空管和脉动热管配置。与之前的综述不同，本研究定量地将研究趋势与系统级进步联系起来，特别是在能量存储、相变材料集成和混合增强技术方面，为下一代高性能太阳能海水淡化系统建立了清晰的路线图。该分析强调了年度出版物增长、地理和期刊贡献以及关键词共现网络，其中新兴主题包括能源储存、热交换器、水深和相变材料。系统地介绍了真空管集热器的最新进展及其在不同工作参数下的性能，并对脉动热管集成太阳能蒸馏器进行了详细的讨论。此外，该综述概述了这些技术的相对优势、局限性和挑战，为指导下一代太阳能脱盐系统的开发提供了重要的见解，这些系统具有更高的效率、可靠性和经济可行性。

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引用次数: 0

Co-ZIF sacrificial templates precisely fabricate MCo-LDH (M = Ni/Cu): Bimetallic synergy regulates PMS activation for synergistic As(III) oxidation-adsorption in complex waters Co-ZIF牺牲模板精确制备MCo-LDH (M = Ni/Cu)：双金属协同作用调节PMS活化，协同As（III）在复杂水体中的氧化吸附

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.2026.137235

Boyu Du, Xianjin Qi, Yongkui Li, Yijin Liu, Jiarui Xiao, Nianyi Zao, Haifeng Chen, Yonglei Bu

Developing novel catalysts for highly efficient activation of PMS is crucial for the purification of arsenic-containing wastewater. In this study, a Co-ZIF sacrificial template was employed to construct NiCo-LDH and CuCo-LDH catalysts with hollow nanocage and nanoflower structures respectively, via Ni²⁺/Cu²⁺ directional etching. The effects of Ni²⁺/Cu²⁺ doping levels on the catalyst's structure, composition, and performance were systematically investigated, identifying the optimal metal doping ratio as Ni²⁺ (1.50 mmol)/Cu²⁺ (1.25 mmol). More importantly, both NiCo-LDH and CuCo-LDH catalysts demonstrated outstanding PMS activation capabilities, removing 98.80% and 97.37% of total arsenic within 600 s, with total arsenic uptakes reaching 1500.00 mg/g and 1415.00 mg/g (following 24 h adsorption equilibrium), respectively. Mechanistic analyses indicate that NiCo-LDH continuously activates PMS through the Ni²⁺/Ni³⁺ and Co³⁺/Co²⁺ redox cycles, generating radicals (SO₄^•− and ^•OH) that participate in the oxidation process of As(III). In contrast, CuCo-LDH promotes radical generation through Cu²⁺/Cu⁺ cycles, while also suggesting the formation of non-radical species (¹O₂), thereby establishing a potential synergistic “radical+non-radical” oxidation pathway. As(V) generated through oxidation in both systems is removed through coordination exchange (M − O − As), ion exchange (interlayer NO₃⁻ substitution), and electrostatic attraction. Additionally, both systems exhibit excellent adaptability to a wide range of concentrations in actual wastewater. After treating low-concentration arsenic-containing wastewater (simulating groundwater), the residual arsenic concentration was below 10.00 μg/L, significantly lower than drinking water standards. In summary, this study proposes a novel strategy for treating arsenic-contaminated wastewater using a Co-ZIF derived LDH to activate PMS, demonstrating broad application prospects in practical arsenic pollution control.

开发高效活化PMS的新型催化剂对含砷废水的净化至关重要。在本研究中，采用Co-ZIF牺牲模板，通过Ni2+/Cu2+定向刻蚀，分别构建了具有空心纳米笼和纳米花结构的NiCo-LDH和CuCo-LDH催化剂。系统考察了Ni2+/Cu2+掺杂水平对催化剂结构、组成和性能的影响，确定了最佳金属掺杂比例为Ni2+ (1.50 mmol)/Cu2+ (1.25 mmol)。更重要的是，NiCo-LDH和CuCo-LDH催化剂均表现出出色的PMS活化能力，在600 s内脱除了98.80%和97.37%的总砷，总砷吸收率分别达到1500 mg/g和1415.00 mg/g （24 h吸附平衡）。机理分析表明，NiCo-LDH通过Ni2+/Ni3+和Co3+/Co2+氧化还原循环持续激活PMS，产生参与As（III）氧化过程的自由基（SO4•−和•OH）。相反，CuCo-LDH通过Cu2+/Cu+循环促进自由基生成，同时也提示非自由基（1O2）的形成，从而建立了潜在的协同“自由基+非自由基”氧化途径。两种体系中氧化产生的As(V)通过配位交换（M−O−As）、离子交换（层间NO3−取代）和静电吸引去除。此外，这两种系统都表现出对实际废水中各种浓度的良好适应性。低浓度含砷废水（模拟地下水）处理后，残留砷浓度低于10.00 μg/L，显著低于饮用水标准。综上所述，本研究提出了一种利用Co-ZIF衍生的LDH活化PMS处理砷污染废水的新策略，在实际砷污染控制中具有广阔的应用前景。

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引用次数: 0

Sustainable fabrication of cellulose beads supported CoFe2O4 and ag-CoFe2O4 catalysts for enhanced tetracycline degradation via PMS activation 纤维素微球负载CoFe2O4和ag-CoFe2O4催化剂的制备及其在四环素降解中的应用

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-01 DOI: 10.1016/j.seppur.2026.137119

Brahim El Allaoui , Hanane Benzeid , Ali Ouhssain , Issam Meftah Kadmiri , Nadia Zari , Abou el kacem Qaiss , Tao Wu , Cheng Heng Pang , Rachid Bouhfid

This study presents a heterogeneous advanced oxidation process (AOP) for antibiotic removal using fibrous cellulose beads (CB) as sustainable catalyst supports. The CB were fabricated from biomass through a green, mechanical approach that avoids cellulose dissolution, preserving their native fibrous structure. Two catalysts, CoFe₂O₄@CB and Ag-CoFe₂O₄@CB, were synthesized via co-precipitation and in situ silver doping. Structural analyses confirmed the spinel CoFe₂O₄ phase, successful Ag incorporation, uniform nanoparticle dispersion, and strong interfacial coupling involving mixed-valence Co/Fe species, Ag-related surface species, and multiple oxygen environments. Under identical optimal conditions identified by Response Surface Methodology (RSM) using a Box–Behnken Design (BBD) (0.40 g L⁻¹ catalyst, 0.50 g L⁻¹ peroxymonosulfate (PMS), 20 mg L⁻¹ tetracycline (TC), 50 min), Ag-CoFe₂O₄@CB achieved 96.18% TC degradation with a higher apparent pseudo-first-order rate constant (k = 0.0690 min⁻¹) than CoFe₂O₄@CB (93.35%, k = 0.0568 min⁻¹), corresponding to ∼43% lower residual TC after 50 min. The enhancement is attributed to Ag-mediated promotion of ROS generation and interfacial electron-transfer processes, while also imparting rapid antibacterial activity against Escherichia coli and Staphylococcus aureus. The fibrous CB architecture further improved catalyst stability, reusability, and mass transfer. The dissolution-free fibrous CB platform enables a scalable, bio-based, and multifunctional catalyst architecture for PMS-driven antibiotic abatement and microbial control in water treatment.

本研究提出了一种以纤维纤维素珠（CB）为可持续催化剂载体的非均相高级氧化法（AOP）去除抗生素。炭黑是由生物质通过绿色，机械的方法，避免纤维素溶解，保留其原有的纤维结构制造的。通过共沉淀法和原位银掺杂法制备了CoFe2O4@CB和Ag-CoFe2O4@CB两种催化剂。结构分析证实了尖晶石CoFe2O4相，成功的银结合，均匀的纳米颗粒分散，以及混合价Co/Fe物种，Ag相关表面物种和多种氧环境的强界面耦合。在采用Box-Behnken设计（BBD）的响应面法（RSM）确定的相同最佳条件下（0.40 g L−1催化剂，0.50 g过氧单硫酸根（PMS）， 20 mg L−1四环素（TC）， 50 min）， Ag-CoFe2O4@CB的TC降解率为96.18%，表观伪一阶速率常数（k = 0.0690 min−1）高于CoFe2O4@CB (93.35%, k = 0.0568 min−1)，对应于50 min后残留TC降低约43%。这种增强是由于ag介导的ROS生成和界面电子转移过程的促进，同时也赋予了对大肠杆菌和金黄色葡萄球菌的快速抗菌活性。纤维状炭黑结构进一步提高了催化剂的稳定性、可重用性和传质性。无溶解纤维CB平台为pms驱动的抗生素减少和水处理中的微生物控制提供了可扩展的、生物基的多功能催化剂结构。

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引用次数: 0

Bio-metal-organic framework with Nano-window traps for ultra-selective thorium separation 生物金属-有机框架与纳米窗陷阱超选择性钍分离

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.2026.137179

Maroof Ahmad Khan , Shaohui Huang , Xinfeng Du, Yongjie Yang, Yan Li, Yihui Yuan, Ning Wang

Selective separation of Th(IV) from chemically similar actinides and rare-earth ions remains a critical barrier to advancing thorium-based nuclear technologies. Here we report a bio-derived dual-ligand MOF platform in which uridine triphosphate and auxiliary N-donor linkers cooperatively assemble O/N-rich nano-window traps that enable precise Th(IV) discrimination. The engineered pore architecture enhances site accessibility, while confined coordination environments promote strong inner-sphere Th-O/N binding and adsorption-induced electronic reorganization. The nano-window confinement and electronic coupling govern precise Th(IV) discrimination. These synergistic structural and mechanistic features yield exceptional selectivity against 17 competing ions as well as high capacity of 553 mg g⁻¹ at pH 3.0. Our findings establish a rational strategy for designing biologically inspired MOFs capable of robust, high-fidelity Th(IV) capture, offering a viable route toward sustainable nuclear-fuel processing and radionuclide remediation.

钍（IV）与化学性质相似的锕系元素和稀土离子的选择性分离仍然是推进钍基核技术的关键障碍。在这里，我们报道了一个生物衍生的双配体MOF平台，其中三磷酸尿苷和辅助n -供体连接剂协同组装富O/ n的纳米窗口陷阱，从而实现精确的Th（IV）识别。工程孔结构增强了位点的可达性，而有限的配位环境促进了球内Th-O/N的强结合和吸附诱导的电子重组。纳米窗口约束和电子耦合控制了精确的Th（IV）判别。这些协同的结构和机制特点产生了对17种竞争离子的卓越选择性，以及在pH 3.0下553 mg g - 1的高容量。我们的研究结果为设计具有强大、高保真Th（IV）捕获能力的生物启发mof建立了合理的策略，为可持续核燃料处理和放射性核素修复提供了可行的途径。

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引用次数: 0

Understanding the adsorption trilemma: Achieving load, level, and selectivity for the removal of pharmaceuticals with zeolites 理解吸附的三难选择：实现沸石去除药物的负荷、水平和选择性

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.2026.137086

Jakob Brauer , Parisa Mahdavi , Jorg Thöming , Michael Fischer

The persistence and ecotoxic effects of pharmaceuticals in aquatic environments demand their removal from wastewater treatment plant effluents. Adsorbents for this purpose must combine high uptake at low concentration levels and a high adsorption load (capacity) with strong selectivity over competing wastewater constituents. Yet, a systematic strategy to address this trilemma remains elusive. Here, we present such an approach using commercial zeolites, which are promising candidates for selective removal owing to the strong influence of molecular shape–topology relationships on interaction energies. The removal of carbamazepine (CBZ) and diclofenac (DCF) with maximum capacities and affinities of 59.71 mg/g and 3.37 L/mg, as well as 104.28 mg/g and 0.21 L/mg, respectively, could be maintained for CBZ adsorption in a secondary-treated municipal wastewater effluent (WWTP effluent), while the adsorption of DCF was significantly reduced. Thermodynamic interpretation of the experimental isotherm parameters showed an excellent quantitative agreement with free energy perturbation simulations, yielding consistent free adsorption energies for CBZ across all zeolites. This confirms that for structurally rigid pollutants, mostly consisting of annulated ring structures, the shape-topology fit is the dominant and predictive factor for adsorption, providing a clear design principle for the targeted selection of zeolites. In contrast, the deviations observed for the DCF molecule with a more flexible structure, consisting of two rings that can more freely arrange with respect to each other, highlight that for non-rigid, more complex pollutants, dynamic conformational effects and guest-guest interactions can become critically important. This study reveals the zeolite topology as a determinant of selective pharmaceutical uptake from wastewater and paves the way for contaminant-specific selection.

药物在水生环境中的持久性和生态毒性作用要求将其从废水处理厂流出物中去除。用于此目的的吸附剂必须结合低浓度水平下的高吸收率和高吸附负荷（容量），并具有对竞争废水成分的强选择性。然而，解决这一三难困境的系统策略仍然难以捉摸。在这里，我们使用商业沸石提出了这种方法，由于分子形状-拓扑关系对相互作用能的强烈影响，商业沸石是有希望的选择性去除候选者。二级处理的城市污水出水对卡马西平（CBZ）和双氯芬酸（DCF）的最大去除率分别为59.71 mg/g和3.37 L/mg，亲和度分别为104.28 mg/g和0.21 L/mg，而对DCF的吸附明显降低。实验等温线参数的热力学解释与自由能摄动模拟非常吻合，得到了CBZ在所有沸石上一致的自由吸附能。这证实了对于结构刚性的污染物，主要由环状结构组成，形状-拓扑配合是吸附的主导因素和预测因素，为有针对性地选择沸石提供了明确的设计原则。相比之下，对于具有更灵活结构的DCF分子（由两个环组成，彼此之间可以更自由地排列）所观察到的偏差突出表明，对于非刚性，更复杂的污染物，动态构象效应和宾客相互作用可能变得至关重要。这项研究揭示了沸石拓扑结构作为从废水中选择性药物摄取的决定因素，并为污染物特异性选择铺平了道路。

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引用次数: 0

Coupling Ni exposure with interfacial oxygen on Zr-doped CeO₂ for stable dry reforming of methane zr掺杂CeO 2上Ni与界面氧耦合暴露对甲烷稳定干重整的影响

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-09 DOI: 10.1016/j.seppur.2026.137164

Qinghui Yu , Yuqin Cheng , Qiufan Qu , Xuanyu Ji , Yu Yang , Yang Su , Xin Yu , Lu Yang , Lin Chen , Xiong Zhou

Dry reforming of methane (DRM) co-converts CH₄ and CO₂ but is limited by Ni sintering and carbon deposition at high temperature. CeO₂-based supports with oxygen vacancies can mitigate these issues, and Zr doping further tunes defect chemistry and basicity, yet the combined roles of Zr content, Ni exposure and pore architecture in governing interfacial oxygen supply and stability remain unclear. Spherical CeO₂ with interconnected through-pores and narrow mesopores is used as a common scaffold to prepare 5Ni/Ce₁₋ₓZrₓO₂ catalysts (Zr = 0, 1, 3 and 7 mol%) at fixed Ni loading and morphology. XRD, Raman and XPS confirm homogeneous Ce₁₋ₓZrₓO₂ solid solutions and show that, within the investigated Zr range, 3 mol% Zr gives the highest Ce³⁺ fraction and defect related surface oxygen while maintaining a moderate Ni particle size. CO₂ TPD, O₂ TPD, H₂ TPR and H₂ TPD further indicate that medium strength basic sites, interfacial reducible oxygen and accessible Ni sites are best balanced at 3 mol% Zr among the studied compositions. Under DRM at 800 °C, 5Ni/Ce₀․₉₇Zr₀․₀₃O₂ shows the highest CH₄ and CO₂ conversions, the lowest apparent activation energy, an H₂/CO ratio near 1.0 and the lowest coke amount over 50 h. Post-reaction XRD, TG–DTG, Raman and SEM suggest reduced Ni sintering and a larger fraction of filamentous or weakly bound carbon. These results are consistent with the importance of the Ni–Ce–Zr–O interfacial structure in balancing Ni exposure and oxygen supply, enabling high activity with low coking.

甲烷（DRM）干法重整可将CH₄和CO₂共转化，但在高温下受Ni烧结和碳沉积的限制。含氧空位的ce2基支架可以缓解这些问题，Zr掺杂进一步调节缺陷的化学性质和碱度，但Zr含量、Ni暴露和孔隙结构在控制界面氧供应和稳定性中的综合作用尚不清楚。采用具有连通通孔和窄介孔的球形CeO₂作为普通支架，制备了固定Ni负载和形态下的5Ni/Ce₁（0、1、3和7 mol%）催化剂（Zr = 0、1、3和7）。XRD、Raman和XPS证实了Ce₁₁ₓZrₓO₂固溶体均相，并表明在所研究的Zr范围内，3 mol% Zr给出了最高的Ce3+分数和与缺陷相关的表面氧，同时保持了中等的Ni粒度。CO₂TPD、O₂TPD、H₂TPR和H₂TPD进一步表明，在3 mol% Zr时，所研究的组分中中等强度碱性位点、界面可还原氧位点和可接近Ni位点的平衡效果最好。在800 ℃的DRM条件下，5Ni/Ce₀。₉₇Zr₀。₀₃O₂转化率最高，表观活化能最低，H₂/CO比接近1.0，焦炭量最低，≥50 H。反应后的XRD， TG-DTG， Raman和SEM表明，Ni烧结还原，丝状或弱结合碳的比例较大。这些结果与Ni - ce - zr - o界面结构在平衡Ni暴露和氧供应方面的重要性相一致，从而实现高活性和低结焦。

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引用次数: 0

Finite-time thermodynamics study on solution thermal-regeneration for frost-free air source heat pump 无霜空气源热泵溶液热再生的有限时间热力学研究

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-06-19 Epub Date: 2026-02-09 DOI: 10.1016/j.seppur.2026.137203

Liutao Zhu , Zhikang Yu , Zhu Jiang , Xiaosong Zhang , Shifang Huang

The solution regeneration process in frost-free air-source heat pump (FFASHP) “imposes a substantial energy burden, directly influencing the overall system efficiency. Although various solution regeneration methods, including evaporation, distillation, and membrane distillation, have been studied extensively, their thermodynamic limits remain unclear. This study utilizes finite-time thermodynamics (FTT) to derive the expression for the minimum heat required in the solution thermal-regeneration process. A comprehensive parametric analysis reveals the interdependencies between solution concentration, regeneration ratio, heat source temperature, ambient temperature, heat transfer capacity-to-mass flow coefficient (θ), and internal reversibility coefficient in determining the minimum specific energy consumption (SEC). Under the basic parameters of this study, the system achieves SEC values of 74.08 kWh/t (thermal) and 16.78 kWh/t (mechanical) at the minimum θ. The θ are 2.12, 3.77, and 7.12 kJ/(kg·K) at thermodynamic second law efficiencies (η_II) of 0.95, 0.9, and 0.8, respectively. Life-cycle cost optimization identifies an economically optimal η_II value of 0.62, corresponding to a minimum total cost of $667.70 over a 20-year operational horizon in the case study. This study establishes theoretical benchmarks for regeneration energy consumption while providing actionable insights for balancing thermodynamic performance with economic viability in FFASHP solution regeneration system design.

无霜空气源热泵（FFASHP）的溶液再生过程造成了巨大的能源负担，直接影响系统的整体效率。尽管各种溶液再生方法，包括蒸发、蒸馏和膜蒸馏，已经得到了广泛的研究，但它们的热力学极限仍然不清楚。本研究利用有限时间热力学（FTT）推导了溶液热再生过程中所需的最小热量的表达式。综合参数分析表明，溶液浓度、再生比、热源温度、环境温度、换热能力-质量流量系数（θ）和内部可逆性系数是决定最小比能耗（SEC）的重要因素。在本研究的基本参数下，系统在最小θ时的SEC值分别为74.08 kWh/t（热）和16.78 kWh/t（机械）。在热力学第二定律效率ηII分别为0.95、0.9和0.8时，θ分别为2.12、3.77和7.12 kJ/（kg·K）。在案例研究中，生命周期成本优化确定经济上最优的η值为0.62，相当于在20年的运营期内，最低总成本为667.70美元。本研究建立了再生能源消耗的理论基准，同时为平衡FFASHP溶液再生系统设计的热力学性能和经济可行性提供了可行的见解。

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引用次数: 0