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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 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL 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
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 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL 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
Harnessing Photothermal graphene oxide interlayers for high-flux solar-driven pervaporation desalination 利用光热氧化石墨烯中间层进行高通量太阳能驱动的渗透蒸发脱盐
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-03 DOI: 10.1016/j.seppur.2026.137136
Cheng Tang, Jie Hu, Tingting Yue, Xiufeng Hu, Wei Yu, Hui Lei
Seawater desalination is a crucial approach to addressing global freshwater scarcity, especially in coastal and arid regions. Pervaporation (PV) offers high salt rejection and strong fouling resistance, but conventional PV membranes often suffer from limited permeate flow rates and temperature polarization. In this study, solar energy was integrated with PV by incorporating graphene oxide (GO) as a photothermal material to directly heat the membrane surface, thereby reducing energy consumption and enhancing permeation flux. The composite membrane comprises an electrospun polyacrylonitrile (PAN) support layer, a GO-based intermediate layer crosslinked with polyethyleneimine (PEI), and a sodium alginate (SA) selective top layer. The GO interlayer converts the solar energy into localized heat and enhances surface wettability, facilitating the development of a uniform and ultrathin SA separation layer, while concurrently enhancing the structural stability of the membrane. By optimizing GO loading and SA thickness, the membrane structure was tailored to increase permeate flux and maintain high salt rejection. The optimized SA(10)/PEI-GO(250)/PAN membrane delivered a stable water flux averaging 2.9–3.0 kg/m2·h, while maintaining a salt removal efficiency above 99.9%. Extended operational trials validated the long-term reliability of the system. These findings highlight the feasibility of solar-driven PV (SPV) composites as a low-energy and eco-friendly approach to saline water treatment.
海水淡化是解决全球淡水短缺的关键方法,特别是在沿海和干旱地区。渗透蒸发膜(PV)具有较高的阻盐性和较强的抗污性,但传统的PV膜往往存在渗透速率有限和温度极化的问题。在本研究中,通过将氧化石墨烯(GO)作为光热材料直接加热膜表面,将太阳能与光伏相结合,从而降低了能耗,提高了渗透通量。该复合膜包括电纺丝聚丙烯腈(PAN)支撑层、与聚乙烯亚胺(PEI)交联的氧化石墨烯基中间层和海藻酸钠(SA)选择性顶层。氧化石墨烯中间层将太阳能转化为局部热,增强了表面润湿性,有利于形成均匀超薄的SA分离层,同时增强了膜的结构稳定性。通过优化氧化石墨烯的负载和SA的厚度,定制膜结构,以增加渗透通量并保持高的阻盐性。优化后的SA(10)/PEI-GO(250)/PAN膜具有稳定的水通量,平均为2.9 ~ 3.0 kg/m2·h,同时除盐效率保持在99.9%以上。扩展的操作试验验证了系统的长期可靠性。这些发现强调了太阳能驱动PV (SPV)复合材料作为一种低能耗和环保的盐水处理方法的可行性。
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引用次数: 0
Biomass-derived hydrogel evaporators for interfacial solar steam generation: crosslinking chemistry, hierarchical network architecture, and device-level strategies for salt-tolerant desalination 用于界面太阳能蒸汽产生的生物质衍生水凝胶蒸发器:交联化学,分层网络结构和耐盐海水淡化的设备级策略
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-02 DOI: 10.1016/j.seppur.2026.137123
Chongjia Fang, Haixin Guo, Xinhua Qi
Solar-driven interfacial steam generation (ISSG) has emerged as an attractive option for decentralized desalination, as it localizes heat at the air-water interface, achieving high solar-to-vapor conversion efficiencies. Biomass-derived hydrogels are an intrinsically sustainable material. The combination of its rich functional groups, hierarchical porous structure, and water-polymer interactions leads to the formation of an extended three-dimensional evaporation interface, thereby enabling rapid capillary transport and active salt management. The present paper reviews the structure, properties, and performance of biomass hydrogel evaporators, establishing a framework that combines cross-linking chemistry (including physical cross-linking, covalent cross-linking, and dynamic covalent cross-linking) and network structures (including bi-networks, interpenetrating polymer networks (IPNs), and semi-IPNs) with the integration of device-level structures, such as bifacial, gradient, bionic, and micro-channel systems, as well as multilayer systems. This framework can be used to rationally target evaporation rate, energy efficiency, hypersaline tolerance and durability. We summarize how intrinsic functionalities, external functionalization (e.g. carboxylation, sulfonation and quaternization) and the careful addition of photothermal, ion-regulating and reinforcing fillers work together to increase spectral absorption, control ion transport via charge/porosity gradients and stabilize long-term operation. In addition to materials design, we identify the following bottlenecks: non-standardized testing, thermal accounting, and mechanical and chemical stability under extreme salinity and temperature. Based on these findings, we propose the following priorities: green, scalable fabrication; ‘strong’ dynamic bonds for adaptive resilience; and integrated modules that pair desalination with antibiofouling or photocatalytic polishing toward zero-liquid-discharge water management. This framework presents a feasible roadmap for developing robust, field-ready hydrogel evaporators by integrating sustainable chemistry with performance-guided architecture.
太阳能驱动的界面蒸汽产生(ISSG)已经成为分散海水淡化的一个有吸引力的选择,因为它将热量集中在空气-水界面,实现了高的太阳能-蒸汽转换效率。生物质衍生的水凝胶是一种本质上可持续的材料。其丰富的官能团、分层多孔结构和水-聚合物相互作用的结合,形成了一个扩展的三维蒸发界面,从而实现了快速的毛细管输送和有效的盐管理。本文综述了生物质水凝胶蒸发器的结构、性能和性能,建立了一个将交联化学(包括物理交联、共价交联和动态共价交联)和网络结构(包括双网络、互穿聚合物网络(IPNs)和半IPNs)与设备级结构(如双面、梯度、仿生和微通道系统)集成在一起的框架。以及多层系统。该框架可用于合理目标蒸发速率,能源效率,高盐耐受性和耐久性。我们总结了内在官能化,外部官能化(例如羧基化,磺化和季铵化)以及光热,离子调节和增强填料的精心添加如何共同作用,以增加光谱吸收,通过电荷/孔隙梯度控制离子传输并稳定长期运行。除了材料设计之外,我们还确定了以下瓶颈:非标准化测试,热计算以及极端盐度和温度下的机械和化学稳定性。基于这些发现,我们提出以下优先事项:绿色,可扩展的制造;适应弹性的“强”动态纽带;将海水淡化与抗生素污垢或光催化抛光相结合的集成模块,实现零液体排放水管理。该框架通过将可持续化学与性能导向结构相结合,为开发强大的、现场可用的水凝胶蒸发器提供了可行的路线图。
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引用次数: 0
Sodium alginate sustained magnetic vanadate hydr(oxide) hydrogel beads for robust, selective, and record-high uptake of tetracycline from waters 海藻酸钠持续磁性钒酸氢(氧化物)水凝胶珠稳健,选择性和创纪录的高四环素从水中摄取
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-02 DOI: 10.1016/j.seppur.2026.137132
Kamatchi Rubini, Triveni Rajashekhar Mandlimath
This study mainly focuses on the development of magnetic vanadium oxide (IVO) reinforced by sodium alginate (Alg) to form hydrogel beads. The as-prepared hydrogel beads were characterized before and after the adsorption of tetracycline (TC) by several spectro-analytical techniques, including powder XRD, FE-SEM, TGA, and XPS. The maximum adsorption densities of 3.254 mmol/g on IVO@Alg hydrogel beads were calculated by a non-linear Langmuir adsorption isotherm. This value is one of the record-high adsorption densities among the materials reported in the literature. The chemical interaction between the adsorbent and adsorbate was confirmed by the kinetic models. The IVO@Alg hydrogel beads were independent of the pH conditions, and they could be used in the extensive pH range from 3 to 12 and were highly selective in the coexistence of binary organic solutions. After seven repeated cycle studies, the studied material showed excellent stability, confirmed by PXRD and FE-SEM analysis. The XPS analysis of TC adsorbed on IVO@Alg hydrogel beads revealed the presence of N-is the indication of successful adsorption of TC onto the IVO@Alg hydrogel beads. The material was also tested with the waters collected from the fields and found that the material is highly selective and suitable for practical applications. This adsorbent stands out as the optimal choice for eliminating TC with high stability from water, due to its remarkable adsorption capacity and simplicity of separation, attributed to its distinctive characteristics.
本研究主要研究海藻酸钠(Alg)增强磁性氧化钒(IVO)形成水凝胶珠的方法。采用粉末XRD、FE-SEM、TGA、XPS等多种光谱分析技术对制备的水凝胶珠吸附四环素前后进行了表征。采用非线性Langmuir吸附等温线计算得到IVO@Alg水凝胶珠的最大吸附密度为3.254 mmol/g。该值是文献报道的材料中吸附密度最高的值之一。动力学模型证实了吸附剂和吸附物之间的化学相互作用。IVO@Alg水凝胶珠不受pH条件的影响,可以在3 ~ 12的广泛pH范围内使用,并且对二元有机溶液的共存具有很高的选择性。经过7次重复循环研究,材料的稳定性得到了PXRD和FE-SEM的证实。吸附在IVO@Alg水凝胶珠上的TC的XPS分析表明,n的存在表明IVO@Alg水凝胶珠上成功吸附了TC。该材料还与从田间收集的水进行了测试,发现该材料具有很高的选择性,适合实际应用。该吸附剂具有显著的吸附能力和简单的分离特性,是去除水中高稳定性TC的最佳选择。
{"title":"Sodium alginate sustained magnetic vanadate hydr(oxide) hydrogel beads for robust, selective, and record-high uptake of tetracycline from waters","authors":"Kamatchi Rubini, Triveni Rajashekhar Mandlimath","doi":"10.1016/j.seppur.2026.137132","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137132","url":null,"abstract":"This study mainly focuses on the development of magnetic vanadium oxide (IVO) reinforced by sodium alginate (Alg) to form hydrogel beads. The as-prepared hydrogel beads were characterized before and after the adsorption of tetracycline (TC) by several spectro-analytical techniques, including powder XRD, FE-SEM, TGA, and XPS. The maximum adsorption densities of 3.254 mmol/g on IVO@Alg hydrogel beads were calculated by a non-linear Langmuir adsorption isotherm. This value is one of the record-high adsorption densities among the materials reported in the literature. The chemical interaction between the adsorbent and adsorbate was confirmed by the kinetic models. The IVO@Alg hydrogel beads were independent of the pH conditions, and they could be used in the extensive pH range from 3 to 12 and were highly selective in the coexistence of binary organic solutions. After seven repeated cycle studies, the studied material showed excellent stability, confirmed by PXRD and FE-SEM analysis. The XPS analysis of TC adsorbed on IVO@Alg hydrogel beads revealed the presence of N-is the indication of successful adsorption of TC onto the IVO@Alg hydrogel beads. The material was also tested with the waters collected from the fields and found that the material is highly selective and suitable for practical applications. This adsorbent stands out as the optimal choice for eliminating TC with high stability from water, due to its remarkable adsorption capacity and simplicity of separation, attributed to its distinctive characteristics.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"44 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101345","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
Integrated oxygen-limited sequencing batch biofilm reactor (SBBR) process coupled with iron‑carbon micro-electrolysis: Simultaneous nitrogen and phosphorus removal performance and mechanism 铁碳微电解一体化限氧序批式生物膜反应器(SBBR)工艺:同时脱氮除磷性能及机理
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-02 DOI: 10.1016/j.seppur.2026.137042
Juqing Lou, Jinhao Zhu, Mengru Han, Dong Che, Qi Su, Zihang Zhu, Jingxuan chen
To address sludge retention time (SRT) conflicts in traditional nitrogen/phosphorus removal, and low C/N ratio in wastewater, an iron‑carbon micro-electrolysis (IC-ME) coupled oxygen-limited sequencing batch biofilm reactor (SBBR) was developed. Using the synergistic growth of immobilized biofilm and suspended sludge, dual-SRT microorganisms were enriched, forming a nitrifiers-denitrifiers‑phosphorus accumulating organisms (PAOs) synergistic metabolic system. Results showed that under low C/N (2.5:1), dissolved oxygen (DO) = 1.6 ± 0.3 mg/L, total nitrogen (TN) and total phosphorus (TP) removal efficiencies stably exceeded 94.5% and 89%, respectively. IC-ME enhanced phosphorus removal via precipitates. The anaerobic ammonium-oxidizing bacteria (AnAOB) were promoted while nitrite-oxidizing bacteria (NOB) were inhibited. A spatial zoning of “outer nitrification-inner denitrification/anammox” with significantly increased abundance of iron-metabolizing genus Spirochaeta and Ignavibacterium was built. DO gradient and iron‑carbon microenvironment synergy drove functional bacteria dynamics, forming an efficient network. The results provide an innovative chemical-biological solution for simultaneous nitrogen/phosphorus removal in low-C/N municipal wastewater.
为解决传统脱氮除磷过程中污泥停留时间(SRT)矛盾以及废水中碳氮比低的问题,研制了铁碳微电解(IC-ME)耦合限氧测序间歇式生物膜反应器(SBBR)。利用固定化生物膜与悬浮污泥协同生长,使双srt微生物富集,形成硝化-反硝化-聚磷生物(PAOs)协同代谢系统。结果表明:在低C/N(2.5:1)、溶解氧(DO) = 1.6 ± 0.3 mg/L条件下,总氮(TN)和总磷(TP)的去除率分别稳定在94.5%和89%以上;IC-ME通过沉淀物增强除磷。厌氧氨氧化菌(AnAOB)得到促进,亚硝酸盐氧化菌(NOB)得到抑制。建立了“外硝化-内反硝化/厌氧氨氧化”的空间分区,铁代谢属Spirochaeta和Ignavibacterium的丰度显著增加。DO梯度和铁碳微环境协同作用驱动功能性细菌动力学,形成一个高效的网络。研究结果为同时去除低碳/氮城市污水中的氮/磷提供了一种创新的化学-生物解决方案。
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引用次数: 0
Pyromellitic acid-coordinated Fe3O4 nanoparticles-mediated GO lamellar membranes for organic solvent nanofiltration and wastewater treatment 邻苯二甲酸配位Fe3O4纳米颗粒介导氧化石墨烯层状膜的有机溶剂纳滤及废水处理
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-02 DOI: 10.1016/j.seppur.2026.137105
Smrutiranjan Nayak, Wei-Kai Hung, T.M. Subrahmanya, Shalligito Habetamu Abebe, R.D. Hope T. Cayron, Hannah Faye M. Austria, Wei-Song Hung, Chien-Chieh Hu, Kueir-Rarn Lee, Juin-Yih Lai
The growing demand for sustainable chemical and pharmaceutical processes has increased the need for efficient organic solvent recovery and solute separation to minimize solvent waste and environmental impact. Graphene oxide (GO)-based lamellar membranes are promising candidates for organic solvent nanofiltration (OSN) due to their subatomic thickness, tunable nanochannels, and excellent molecular sieving capability. Nevertheless, pure GO membranes typically exhibit limited flux, excessive swelling, and structural instability in aggressive solvents. To overcome these limitations, this study developed a novel GP2Fe100 nanocomposite membrane through pressure driven self-assembly of pyromellitic acid (PMA)-coordinated Fe3O4 nanoparticles intercalated within GO lamellae. The synergistic coordination of Fe3O4 nanoparticles with PMA precisely tuned the d-spacing while suppressing hydration-induced swelling, imparting exceptional chemical and mechanical robustness. Under dead-end operation, the GP2Fe100 membrane exhibited good solvent flux together with dye removal efficiency above 97% for Congo red (CR) and Methyl blue (MB) in both aqueous and organic media. It also achieved high CR removal (≥ 94.30%) from harsh solvents like N, N-dimethylformamide (DMF) and N, N-dimethylpyrrolidone (NMP), and efficient separation of the pharmaceutical oxytetracycline dihydrate (OTC) from water and DMF. Long-term filtration (72 h) confirmed stable flux and consistent OTC (in water) and CR (in ethanol) rejection. In cross-flow mode, the membrane maintained CR and MB rejection above 98.80% with enhanced water flux and consistent OTC rejection of 97.16% across four conjugative cycles. Outstanding Pressure resistance both in dead end and cross flow filtration, and antifouling performance (flux recovery >96%) further highlights its durability. Overall, GP2Fe100 membrane provides a highly effective platform for OSN-based solvent recovery and pharmaceutical/dye removal.
对可持续化学和制药工艺的需求不断增长,增加了对高效有机溶剂回收和溶质分离的需求,以尽量减少溶剂浪费和对环境的影响。基于氧化石墨烯(GO)的层状膜由于其亚原子厚度、可调谐纳米通道和优异的分子筛分能力而成为有机溶剂纳滤(OSN)的有希望的候选者。然而,纯氧化石墨烯膜在腐蚀性溶剂中通常表现出有限的通量、过度膨胀和结构不稳定。为了克服这些限制,本研究通过在氧化石墨烯薄片中嵌入邻苯二甲酸(PMA)配位的Fe3O4纳米颗粒的压力驱动自组装,开发了一种新型的GP2Fe100纳米复合膜。Fe3O4纳米颗粒与PMA的协同配合精确调节了d-间距,同时抑制了水化引起的膨胀,赋予了优异的化学和机械鲁棒性。在无端操作下,GP2Fe100膜对刚果红(CR)和甲基蓝(MB)的去除率均在97%以上。对N, N-二甲基甲酰胺(DMF)和N, N-二甲基吡咯烷酮(NMP)等苛刻溶剂的CR去除率≥94.30%,对药物二水化土霉素(OTC)与水和DMF的有效分离。长期过滤(72小时)证实通量稳定,OTC(水中)和CR(乙醇中)的去除率一致。在交叉流动模式下,膜在四个共轭循环中保持CR和MB的截留率在98.80%以上,水通量增强,OTC截留率保持在97.16%。在死角和交叉流过滤中,优异的耐压性能和防污性能(通量回收率>;96%)进一步凸显了其耐用性。总体而言,GP2Fe100膜为基于osn的溶剂回收和药物/染料去除提供了一个高效的平台。
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引用次数: 0
Upcycled PET carbon dots build an S-scheme Fe2O3 heterojunction photocatalyst for visible-light degradation of tetracycline 升级后的PET碳点构建了S-scheme Fe2O3异质结光催化剂,用于四环素的可见光降解
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-01 DOI: 10.1016/j.seppur.2026.137122
Pandi Kalimuthu, Gopi Kalaiyarasan, Jinho Jung, Diwakar Tiwari
Polyethylene terephthalate-derived carbon dots (PET-CDs) were interfaced with Fe2O3 to develop a visible-light PET-CDs/Fe2O3 photocatalyst for tetracycline (TC) removal. Waste PET bottles were upcycled via a peroxide-free route, enabling oxidant-free operation. The photocatalyst forms a defect-rich, mesoporous carbon-dot network with uniformly dispersed Fe2O3 nanoparticles, enhancing adsorption and interfacial charge transport. This study demonstrates efficient TC removal at a relatively high initial concentration (C₀ = 100 mg L−1) under visible light (λ > 420 nm) without added oxidants. The optimized PET-CDs/Fe2O3 (0.4) reaches 98.2% TC removal. Kinetics follow a pseudo-first-order model, and blank tests confirm negligible photolysis and dark adsorption. The TOC and LC-MS results show rapid degradation followed by slower oxidation. Mineralization is substantial, with TOC decreasing from 100 to 34 mg L−1 at 4 h and reaching 89.6% removal at 10 h. The PET-CDs/Fe2O3 photocatalyst operates across pH 3–11. Phosphate reduces activity by competitive site blocking. At least 80% efficiency is retained over repeated cycles. Convergent evidence supports an S-scheme pathway rather than a type-II junction. DRS-Tauc analysis and band alignment indicate favorable energetic offsets and interfacial band bending. Steady-state PL shows selective quenching of PET-CDs emission with enhanced red Fe2O3 or interfacial emission. Transient photocurrent and EIS Nyquist plots reveal enhanced charge separation and reduced charge-transfer resistance. Scavenger tests and ESR identify h+ and •O2 as dominant species, with •OH secondary. LC-MS tracking shows early functional-group loss products at m/z 417 and 402, followed by lower-mass fragments (m/z 301–231 and 189–72), confirming stepwise oxidation toward mineralization.
将聚对苯二甲酸乙二醇酯衍生的碳点(PET-CDs)与Fe2O3相结合,制备了四环素(TC)脱除可见光PET-CDs/Fe2O3光催化剂。废弃PET瓶通过无过氧化物路线升级回收,实现无氧化剂操作。该光催化剂与均匀分散的Fe2O3纳米颗粒形成了富含缺陷的介孔碳点网络,增强了吸附和界面电荷传输。本研究表明,在可见光(λ >; 420 nm)下,在相对高的初始浓度(C 0 = 100 mg L−1)下,不添加氧化剂,可以有效地去除TC。优化后的PET-CDs/Fe2O3(0.4)的TC去除率达到98.2%。动力学遵循伪一级模型,空白试验证实可忽略光解和暗吸附。TOC和LC-MS结果显示,降解速度快,氧化速度慢。矿化效果显著,在4 h时TOC从100降低到34 mg L−1,在10 h时达到89.6%的去除率。PET-CDs/Fe2O3光催化剂在pH值 3-11范围内工作。磷酸盐通过竞争性位点阻断降低活性。在重复循环中至少保持80%的效率。趋同的证据支持s方案途径,而不是ii型连接。drs - tac分析和带对准表明有利的能量偏移和界面带弯曲。稳态PL显示出PET-CDs发射的选择性猝灭,红色Fe2O3或界面发射增强。瞬态光电流和EIS奈奎斯特图显示电荷分离增强和电荷转移电阻降低。清道夫试验和ESR鉴定h+和•O2−为优势种,•OH为次要种。LC-MS追踪显示,在m/z 417和402处有较早的官能团损失产物,其次是较低质量的碎片(m/z 301-231和189-72),证实了逐步氧化到成矿的过程。
{"title":"Upcycled PET carbon dots build an S-scheme Fe2O3 heterojunction photocatalyst for visible-light degradation of tetracycline","authors":"Pandi Kalimuthu, Gopi Kalaiyarasan, Jinho Jung, Diwakar Tiwari","doi":"10.1016/j.seppur.2026.137122","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137122","url":null,"abstract":"Polyethylene terephthalate-derived carbon dots (PET-CDs) were interfaced with Fe<sub>2</sub>O<sub>3</sub> to develop a visible-light PET-CDs/Fe<sub>2</sub>O<sub>3</sub> photocatalyst for tetracycline (TC) removal. Waste PET bottles were upcycled via a peroxide-free route, enabling oxidant-free operation. The photocatalyst forms a defect-rich, mesoporous carbon-dot network with uniformly dispersed Fe<sub>2</sub>O<sub>3</sub> nanoparticles, enhancing adsorption and interfacial charge transport. This study demonstrates efficient TC removal at a relatively high initial concentration (<em>C₀</em> = 100 mg L<sup>−1</sup>) under visible light (λ &gt; 420 nm) without added oxidants. The optimized PET-CDs/Fe<sub>2</sub>O<sub>3</sub> (0.4) reaches 98.2% TC removal. Kinetics follow a pseudo-first-order model, and blank tests confirm negligible photolysis and dark adsorption. The TOC and LC-MS results show rapid degradation followed by slower oxidation. Mineralization is substantial, with TOC decreasing from 100 to 34 mg L<sup>−1</sup> at 4 h and reaching 89.6% removal at 10 h. The PET-CDs/Fe<sub>2</sub>O<sub>3</sub> photocatalyst operates across pH 3–11. Phosphate reduces activity by competitive site blocking. At least 80% efficiency is retained over repeated cycles. Convergent evidence supports an S-scheme pathway rather than a type-II junction. DRS-Tauc analysis and band alignment indicate favorable energetic offsets and interfacial band bending. Steady-state PL shows selective quenching of PET-CDs emission with enhanced red Fe<sub>2</sub>O<sub>3</sub> or interfacial emission. Transient photocurrent and EIS Nyquist plots reveal enhanced charge separation and reduced charge-transfer resistance. Scavenger tests and ESR identify h<sup>+</sup> and •O<sub>2</sub><sup>−</sup> as dominant species, with •OH secondary. LC-MS tracking shows early functional-group loss products at <em>m</em>/<em>z</em> 417 and 402, followed by lower-mass fragments (m/z 301–231 and 189–72), confirming stepwise oxidation toward mineralization.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"8 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101347","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
A novel magnetic adsorption–coagulation system using lanthanum carbonate/Fe3O4 composite adsorbent for simultaneous efficient removal of turbidity and fluoride 采用碳酸镧/Fe3O4复合吸附剂的新型磁吸附-混凝系统可同时高效除浊除氟
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-01 DOI: 10.1016/j.seppur.2026.137125
Shan Wang, Xinyan Zhang, Changlong Yan, Yao Zhang, Kefeng Zhang, Baoyou Shi, Jinhu Liu, Haotian Hao, Xin Huang
The reduction of fluoride concentration in wastewater to ultra-low levels remains a significant challenge, as conventional aluminum-based coagulation suffers from low efficiency at trace levels and high chemical consumption. Herein, a novel magnetic adsorption-coagulation (MAC) process was developed in this study to address this limitation by integrating a lanthanum carbonate/Fe3O4 composite (LC-Fe3O4) as a magnetic seed with polyaluminum chloride (PAC). Sole LC-Fe3O4 adsorbent exhibited a high fluoride adsorption capacity of 215.3 mg F/g (pH 7, 298 K, 0.1 g/L, 24 h), fitting well with Langmuir and Freundlich models and following the pseudo-second-order kinetic model. It maintained robust performance across a wide pH range (5.0–9.0) and exhibiting strong selectivity toward fluoride even in the presence of competing HCO3, CO32−, SO42−, and NO3 anions, whereas PO43− significantly interfered. This study revealed that the mechanisms of fluoride removal during LC-Fe3O4 adsorption process mainly included ligand exchange, electrostatic attraction, and inner-sphere complexation with La3+ sites. When applied for treating real secondary effluent, this novel MAC process achieved simultaneous and efficient removal of both fluoride and turbidity. Under optimized conditions, fluoride and turbidity removal efficiencies reached 69.12% and 95.2%, respectively, significantly outperforming sole coagulation. This enhancement might be attributed to the synergistic effects of adsorption on the magnetic seeds and the formation of denser and separable flocs. Furthermore, the LC-Fe3O4 seed showed excellent regenerability and reusability over multiple cycles, underscoring the practical potential of the MAC strategy for advanced wastewater treatment.
将废水中的氟化物浓度降至超低水平仍然是一项重大挑战,因为传统的铝基混凝在痕量水平下效率低且化学品消耗高。为了解决这一问题,本研究开发了一种新的磁吸附-混凝(MAC)工艺,通过将碳酸镧/Fe3O4复合材料(LC-Fe3O4)作为磁性种子与聚氯化铝(PAC)相结合。单一LC-Fe3O4吸附剂对氟的吸附量为215.3 mg F/g (pH 7, 298 K, 0.1 g/L, 24 h),符合Langmuir和Freundlich模型,符合准二级动力学模型。它在较宽的pH范围(5.0-9.0)内保持稳定的性能,即使在竞争的HCO3−、CO32−、SO42−和NO3−阴离子存在时也表现出对氟的强选择性,而PO43−则明显干扰。研究表明,LC-Fe3O4吸附过程中除氟的机制主要包括配体交换、静电吸引和La3+的球内络合。应用于实际二级出水处理时,该新工艺实现了氟和浊度的同时高效去除。在优化条件下,氟和浊度的去除率分别达到69.12%和95.2%,显著优于单纯混凝。这种增强可能是由于吸附对磁性种子的协同作用和形成更致密和可分离的絮凝体。此外,LC-Fe3O4种子在多个循环中表现出良好的可再生性和可重复使用性,强调了MAC策略在高级废水处理中的实际潜力。
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引用次数: 0
Superbase based deep eutectic solvents for high-efficiency carbon capture and characterization-derived insights 用于高效碳捕获和表征的超碱型深共晶溶剂
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-01 DOI: 10.1016/j.seppur.2026.137080
Qiang Zheng, Qiong Sun, Fuxin Yang, Houzhang Tan, Xiaopo Wang
To address the limitations of traditional amine absorbents for CO2 capture, this work prepared deep eutectic solvents (DESs) using 2,3,4,6,7,8-hexahydropyrrolo [1,2-a] pyrimidine (DBN) as hydrogen bond acceptor (HBA), and diaminoethane (DETA)/3-aminopropanol (AP) as hydrogen bond donors (HBDs). The CO2 absorption-desorption performance was investigated under varied molar ratios, temperatures, and water contents. Key physicochemical properties (thermal stability, density, viscosity) were characterized, and the absorption mechanism was elucidated via experimental techniques and density functional theory (DFT) calculations. These 2 types of DESs achieve maximum saturated absorption capacities of 0.234 and 0.199 g CO2/g DES at 313.15 K, respectively. They have distinct reaction pathways (carbamate for DBN-DETA based DESs and carbonate/bicarbonate for DBN-AP based DESs). Their regeneration energy consumption was 2.3437 and 1.9130 GJ/t CO2, much lower than that of the traditional aqueous amines, demonstrating promising potential as efficient, low-energy CO2 capture absorbents.
为了解决传统胺类吸收剂捕集CO2的局限性,本研究以2,3,4,6,7,8-六氢吡罗[1,2-a]嘧啶(DBN)为氢键受体(HBA),二氨基乙烷(DETA)/3-氨基丙醇(AP)为氢键供体(HBDs)制备了深度共晶溶剂(DESs)。考察了不同摩尔比、温度和含水量对CO2吸附解吸性能的影响。通过实验技术和密度泛函理论(DFT)计算,表征了其主要的物理化学性质(热稳定性、密度、粘度),并阐明了其吸附机理。在313.15 K下,这两种DES的最大饱和吸收容量分别为0.234和0.199 g CO2/g DES。它们具有不同的反应途径(氨基甲酸酯为DBN-DETA基DESs,碳酸盐/碳酸氢盐为DBN-AP基DESs)。其再生能耗分别为2.3437 GJ/t CO2和1.9130 GJ/t CO2,远低于传统水胺的再生能耗,作为高效、低能耗的CO2捕集吸收剂具有广阔的应用前景。
{"title":"Superbase based deep eutectic solvents for high-efficiency carbon capture and characterization-derived insights","authors":"Qiang Zheng, Qiong Sun, Fuxin Yang, Houzhang Tan, Xiaopo Wang","doi":"10.1016/j.seppur.2026.137080","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137080","url":null,"abstract":"To address the limitations of traditional amine absorbents for CO<sub>2</sub> capture, this work prepared deep eutectic solvents (DESs) using 2,3,4,6,7,8-hexahydropyrrolo [1,2-a] pyrimidine (DBN) as hydrogen bond acceptor (HBA), and diaminoethane (DETA)/3-aminopropanol (AP) as hydrogen bond donors (HBDs). The CO<sub>2</sub> absorption-desorption performance was investigated under varied molar ratios, temperatures, and water contents. Key physicochemical properties (thermal stability, density, viscosity) were characterized, and the absorption mechanism was elucidated via experimental techniques and density functional theory (DFT) calculations. These 2 types of DESs achieve maximum saturated absorption capacities of 0.234 and 0.199 g CO<sub>2</sub>/g DES at 313.15 K, respectively. They have distinct reaction pathways (carbamate for DBN-DETA based DESs and carbonate/bicarbonate for DBN-AP based DESs). Their regeneration energy consumption was 2.3437 and 1.9130 GJ/t CO<sub>2</sub>, much lower than that of the traditional aqueous amines, demonstrating promising potential as efficient, low-energy CO<sub>2</sub> capture absorbents.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101353","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
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Separation and Purification Technology
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