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Sulfonamides extraction from environmental water using natural hydrophobic deep eutectic solvent: COSMO-RS calculations and ANN-GA optimization 天然疏水深共熔溶剂从环境水中提取磺胺类化合物:cosmos - rs计算和ANN-GA优化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137213
Jiacao Wu , Yi Kuang , Shengxiang Yang, Xu Han, Yiyu Qi
To address the challenge of efficiently removing sulfonamides (SAs) from environmental water, a vortex-assisted liquid-liquid microextraction method using an L-menthol-based natural hydrophobic deep eutectic solvent (NaHDES), combined with ultra-performance liquid chromatography, was employed. The single-factor experiments, response surface methodology, and artificial neural network coupled with genetic algorithm (ANN-GA) were applied to optimize the key extraction parameters. Under the optimized conditions, the method exhibited excellent linearity (1.67–500 μg·L−1), low limits of detection (0.42–0.77 μg·L−1), relative standard deviations of 0.23–4.27%, and negligible matrix effects, as evaluated using real water samples from different sources. The extraction mechanism of SAs by the NaHDES was investigated using the conductor-like screening model for real solvents (COSMO-RS). Moreover, the validated method was successfully applied to environmental water samples. Finally, the results from three green chemistry assessment tools, including AGREE, AGREEprep and ComplexGAPI, demonstrated the greenness of the method. Overall, the proposed method is dispersant-free, simple, time-saving, environmentally friendly, and highly efficient, making it well suited for the analysis of SAs in different water samples.
为了解决从环境水中高效去除磺胺类化合物(SAs)的难题,采用基于l-薄荷醇的天然疏水深共晶溶剂(NaHDES)的涡流辅助液-液微萃取法,结合超高效液相色谱法。采用单因素实验、响应面法、人工神经网络结合遗传算法(ANN-GA)对关键提取参数进行优化。在优化条件下,该方法具有良好的线性关系(1.67 ~ 500 μg·L−1),低检出限(0.42 ~ 0.77 μg·L−1),相对标准偏差为0.23 ~ 4.27%,基质效应可忽略。采用真实溶剂类导体筛选模型(cosmos - rs)研究了NaHDES萃取SAs的机理。此外,该方法还成功地应用于环境水样。最后,通过三种绿色化学评价工具(AGREE、AGREEprep和ComplexGAPI)验证了该方法的环保性。总体而言,该方法无分散剂、简单、省时、环保、高效,适用于不同水样中SAs的分析。
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引用次数: 0
Green and synergistic process for high-efficiency recycling and valorization of nickel smelting slag 镍冶炼渣高效回收与增值的绿色协同工艺
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-11 DOI: 10.1016/j.seppur.2026.137205
Xiaoyu Tan , Liang Zhou , Yuchun He , Min Chen , Xingbang Wan
Nickel smelting slag is an important secondary resource since its nickel content often exceeds that of certain primary ores. In this study, a novel process of recycling valuable metals from nickel slag was developed and experimentally verified, which can help Ni, Cu, and Co selectively separated from the slag. Under optimal conditions (650 °C, 90 min, 5%SO2–20%O2–75%Ar atmosphere, and Na2SO4/slag mass ratio of 0.5,1), the water-leaching efficiencies of Ni, Cu, and Co reached 96.5%, 99.7%, and 81.4%, respectively, whereas most Fe, Si, and other impurities were retained in the solid residue. Moreover, the reaction and catalysis mechanism were experimentally investigated and concluded. It was found that controlled gas atmosphere and temperature can achieve the selective sulfation of Ni, Cu, and Co into soluble sulfates, while Fe and Si remained as stable oxides, and the formation of nickel ferrite (NiFe2O4) was identified as a major inhibitory phase that limited Ni recovery. The addition of Na2SO4 promoted the generation of a low-melting-point salt (NaMgFe(SO4)3), which effectively suppressing NiFe2O4 formation and improving overall recovery efficiency. Furthermore, this process could utilize industrial SO2 off-gases as the sulfur source, and a ‘waste-treats-waste’ approach that converts harmful emissions into reactive agents was then established. This study provides a green, acid-free, and economically viable pathway for the comprehensive utilization of nickel slag and offers valuable guidance for the sustainable recovery of valuable metals from metal-bearing secondary resources.
镍冶炼渣的镍含量往往超过某些原生矿石,是重要的二次资源。本研究开发了一种从镍渣中回收有价金属的新工艺,并进行了实验验证,该工艺有助于镍、铜、钴从渣中选择性分离。在最佳条件(650 ℃,90 min, 5%SO2-20%O2-75%Ar气氛,Na2SO4/渣质量比为0.5,1)下,Ni、Cu和Co的水浸效率分别达到96.5%、99.7%和81.4%,大部分Fe、Si等杂质保留在固体渣中。并对反应机理和催化机理进行了实验研究和总结。结果表明,控制气体气氛和温度可以使Ni、Cu和Co选择性硫酸化成可溶性硫酸盐,而Fe和Si保持稳定的氧化物状态,镍铁氧体(NiFe2O4)的形成是限制Ni回收的主要抑制相。Na2SO4的加入促进了低熔点盐(NaMgFe(SO4)3)的生成,有效抑制了NiFe2O4的生成,提高了整体回收率。此外,该工艺可以利用工业二氧化硫废气作为硫源,并建立了一种将有害排放物转化为活性物质的“废物处理废物”方法。本研究为镍渣的综合利用提供了一条绿色、无酸、经济可行的途径,为含金属二次资源中有价金属的可持续回收提供了有价值的指导。
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引用次数: 0
Zeolite P synthesis based on dephosphorized ash and its adsorption of Cd (II) ions 脱磷灰合成P型沸石及其对Cd (II)离子的吸附
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-05 DOI: 10.1016/j.seppur.2026.137154
Cheng Chen , Lihua Wang , Fei Wang , Nan Xu
Dephosphorized ash (DA) retains considerable potential for zeolite synthesis due to its inherent silicon and aluminum content after phosphorus extraction. In this study, a one-step alkaline hydrothermal method was employed to promote the formation of zeolite P, and its adsorption performance toward Cd (II) ions in aqueous solution was systematically investigated. The presence of OH ions in the alkaline environment effectively facilitates the dissolution and hydrolysis of the original DA structure. An appropriate hydrothermal temperature (150 °C) and sufficient reaction time (9 h) ensure that zeolite P is the dominant crystalline product. The synthesized zeolite P exhibits an optimal Cd (II) adsorption capacity of 33.08 mg/g at pH 5, which is associated with its negatively charged surface as indicated by zeta potential analysis. The adsorption behavior of Cd (II) is well described by the Langmuir isotherm model and pseudo-second-order kinetic model. Mechanistic analysis suggests that Cd (II) adsorption on zeolite P involves ion exchange and surface complexation via dehydration–condensation reactions. Furthermore, density functional theory (DFT) calculations indicate that Cd (II) preferentially binds to AlO sites to form CdO bonds, owing to the stronger interaction at Al-associated hydroxyl groups compared with Si-associated sites. Overall, this study provides a feasible strategy for converting DA into zeolite P and offers insights into its application for Cd (II) removal, which can realize a waste to waste utilization pathway.
除磷灰(DA)在除磷后,由于其固有的硅和铝含量而保留了相当大的合成沸石的潜力。本研究采用一步法碱性水热法促进P沸石的形成,并系统研究了其对水溶液中Cd (II)离子的吸附性能。碱性环境中OH−离子的存在有效地促进了原始DA结构的溶解和水解。适当的水热温度(150°C)和充足的反应时间(9 h)确保沸石P是主要的结晶产物。zeta电位分析表明,合成的P沸石在pH为5时对Cd (II)的最佳吸附容量为33.08 mg/g,这与P沸石表面带负电荷有关。Langmuir等温模型和拟二级动力学模型很好地描述了Cd (II)的吸附行为。机理分析表明,P沸石吸附Cd (II)涉及离子交换和表面脱水缩合反应。此外,密度泛函理论(DFT)计算表明,由于al相关羟基上的相互作用比si相关位点更强,Cd (II)优先与AlO位点结合形成CdO键。综上所述,本研究提供了一种可行的将DA转化为P沸石的策略,并为其在Cd (II)去除中的应用提供了见解,实现了废到废的利用途径。
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引用次数: 0
Rapid ag and Pb extraction and high-purity material regeneration from silver-containing waste via selective reduction, leaching, and precipitation 通过选择性还原、浸出和沉淀从含银废物中快速提取银、铅和高纯材料再生
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-09 DOI: 10.1016/j.seppur.2026.137204
Yang Zhao , Weifeng Liu , Baiqi Sun , Duchao Zhang , Lin Chen , Tianzu Yang , Qunli Zhou
Noble antimony chloride leaching residue represents an important silver-bearing secondary resource that also contains Pb, Sb, and trace Au. However, existing processes predominantly focus on silver extraction and are constrained by excessive reagent consumption, limited selectivity, and low overall recovery. In this study, a novel ligand-free and integrated process was developed, comprising alkaline dechlorination, H2O2–HNO3 synergistic oxidative leaching, stepwise precipitation, and direct hydrazine reduction, enabling the efficient recovery of silver together with the selective separation of associated metals. Thermodynamic analysis demonstrated that the alkaline reduction–synergistic leaching strategy facilitates preferential dissolution of Ag and Pb while enriching Au and Sb in the residue. Under optimal conditions, the leaching efficiencies of Ag and Pb reached 99.2% and 79.4%, respectively, with effective suppression of NO2 emission. Subsequent sulfate and chloride precipitation yielded high-purity products, including ultrafine Ag powder (99.7%) and PbSO4 (99.3%). The overall direct recoveries of Ag and Pb were 98.9% and 78.6%, while the remaining residue was upgraded to a high-grade AuSb concentrate (Au 2.92%, Sb 23.8%). The process was successfully validated at an industrial scale in an antimony smelter, enabling annual recovery of 1.62 t Au and 1.4 t Ag, with reductions of 57% in reagent cost and 72.9% in wastewater discharge. This work provides a sustainable, low-emission, and industrially scalable route for the comprehensive valorization of high-Ag chloride residues.
贵金属氯化锑浸出渣是一种重要的含银二次资源,它还含有Pb、Sb和微量Au。然而,现有的工艺主要集中在银的提取上,并且受到过多的试剂消耗、有限的选择性和低的总回收率的限制。在本研究中,开发了一种新的无配体集成工艺,包括碱性脱氯、H2O2-HNO3协同氧化浸出、分步沉淀和直接肼还原,实现了银的高效回收和伴生金属的选择性分离。热力学分析表明,碱还原-协同浸出有利于银和铅的优先溶解,同时富集了渣中的Au和Sb。在最佳浸出条件下,银和铅的浸出效率分别达到99.2%和79.4%,并能有效抑制NO2的排放。随后的硫酸盐和氯化物沉淀得到了高纯度的产品,包括超细银粉(99.7%)和PbSO4(99.3%)。银和铅的总直接回收率分别为98.9%和78.6%,剩余残渣升级为Au 2.92%、Sb 23.8%的高品位AuSb精矿。该工艺在一家锑冶炼厂的工业规模上得到了成功验证,每年可回收1.62 t Au和1.4 t Ag,试剂成本降低57%,废水排放量降低72.9%。这项工作为高氯化银残留物的综合增值提供了一条可持续、低排放和工业可扩展的途径。
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引用次数: 0
Controllable design of poly(ionic liquid) coatings for enhanced artemisinin purification 用于增强青蒿素纯化的聚离子液体涂层的可控设计
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-06 DOI: 10.1016/j.seppur.2026.137145
Xingxing Li , Jianing Qi , Mingjing Shi , Yuan Yao , Yingying Cao , Xue Wang , Hui Wang
Artemisinin is primarily derived from Artemisia annua L. However, due to the complex composition of its leaf extract, the purification and separation of artemisinin remain a significant challenge. In this work, various poly(ionic liquid)s (PILs) containing polar ester groups and non-polar long-chain alkyl groups were synthesized through radical polymerization. Subsequently, these PILs were made into coatings with controllable pore sizes and adjustable hydrophobicity. The ethyl octadecanoate based PIL coating showed excellent capability to intensify this purification process. The product purity could reach 96.8% after one crystallization step under the optimal conditions, approximately 30.8% higher than the traditional method. And the product purity could reach 99.9% after three sequential separation processes. In addition, the adsorption kinetics of wax oil on the PIL coating were studied, and the results indicated that it followed a pseudo-first-order kinetic model with a maximum adsorption capacity of 226.33 mg/g. Mechanism analysis demonstrated that hydrogen bonding and van der Waals forces between the wax oil (the main impurity in the extract) and PIL facilitated the adsorption of the wax oil, thereby increasing the purity of artemisinin.
青蒿素主要来源于黄花蒿(Artemisia annua L.),但由于黄花蒿叶提取物成分复杂,其纯化和分离仍然是一个重大挑战。本文采用自由基聚合的方法合成了多种含有极性酯基和非极性长链烷基的聚离子液体(pil)。随后,将这些pil制成孔径可控、疏水性可调的涂层。十八烷酸乙酯基PIL涂层对这一净化过程有很好的强化作用。在最佳工艺条件下,单步结晶后产品纯度可达96.8%,比传统方法提高约30.8%。经3次顺序分离,产品纯度可达99.9%。此外,研究了蜡油在PIL涂层上的吸附动力学,结果表明其符合准一级动力学模型,最大吸附量为226.33 mg/g。机理分析表明,蜡油(提取物中的主要杂质)与PIL之间的氢键和范德华力有利于蜡油的吸附,从而提高了青蒿素的纯度。
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引用次数: 0
Synergetic Zn doping and KOH etching of CeO2 for enhanced H2S oxidation via electronic structure reconstruction 协同Zn掺杂和KOH蚀刻CeO2通过电子结构重建增强H2S氧化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137207
Honghong Yi , Kai Chen , Hongkun Ni , Yiming Ma , Xiaolong Tang , Qingjun Yu , Fengyu Gao , Shunzheng Zhao
This study employs a synergistic strategy of Zn doping and KOH etching to precisely regulate the physicochemical properties of CeO2, significantly enhancing its H2S catalytic oxidation performance. Experimental results indicate that Zn doping induces lattice expansion of CeO2, while KOH etching further removes Zn, increases Ce3+ and oxygen vacancy concentrations, thereby optimizing surface acidity-basicity and redox capability. The obtained E-Zn/CeO2 material exhibits excellent H2S conversion, reaction and kinetics, while promoting the selective formation of SO2. Mechanistic studies reveal that H2S undergoes adsorption and dissociation via μ2-OH/–COOH groups on the material surface, with the oxidation process following the MvK mechanism, where oxygen vacancies play a key role in adsorption and lattice oxygen transfer. Theoretical calculations further demonstrate that the synergistic modification induces reconstruction of the electronic structure of CeO2, including weakened covalency of CeO bonds and a spin-state transition of O2p orbitals, which significantly reduces the oxygen vacancy formation energy (as low as −1.47 eV) and enhances structural stability. This work provides both experimental and theoretical foundations for the rational design of highly efficient H2S catalytic materials.
本研究采用Zn掺杂和KOH蚀刻协同策略,精确调控CeO2的理化性质,显著提高其H2S催化氧化性能。实验结果表明,掺杂Zn引起CeO2晶格膨胀,而KOH腐蚀进一步去除Zn,增加Ce3+和氧空位浓度,从而优化表面酸碱度和氧化还原能力。制备的E-Zn/CeO2材料表现出优异的H2S转化、反应和动力学,同时促进了SO2的选择性生成。机理研究表明,H2S在材料表面通过μ2-OH/ -COOH基团进行吸附和解离,氧化过程遵循MvK机制,其中氧空位在吸附和晶格氧转移中起关键作用。理论计算进一步表明,协同修饰导致CeO2的电子结构重构,包括CeO键的共价减弱和O2p轨道的自旋态跃迁,显著降低了氧空位形成能(低至- 1.47 eV),增强了结构稳定性。本工作为合理设计高效H2S催化材料提供了实验和理论基础。
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引用次数: 0
Critical reviews on recovery of valuable metals from spent petroleum catalysts 从废石油催化剂中回收有价金属的研究进展
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137206
Haotian Gan , Baohuai Zhao , Qing Liu , Xuefeng He , Zhisheng Shi , Shuai Han , Kezhi Li , Bo Liu , Shengen Zhang , Yunji Ding
Catalysts play a significant role in oil refining field. Reforming catalysts, hydrogenation catalysts and fluid catalytic cracking catalysts (FCC catalysts) are extensively employed in the petroleum refining, which account for over 90% of total catalysts. Consequently, large amounts of spent catalysts are generated once they lose the effectiveness and end of life. Spent catalysts are classified as hazardous waste and their disposal has become a great concern for the refineries. Recovery of spent catalysts has attracted great attention due to the environmental issues and economic benefits as containing valuable metals (such as Pt, Pd, Co, Mo, Ni, V, rare earth metals) as well. This review summarized the recycling technologies on the recovery of valuable metals from spent petroleum catalysts, as well as the latest achievements of the authors' group. More recycling technologies with less environmental impacts have been developed in recent years. For instance, pyrometallurgical enrichment of valuable metals have become the research focus for recovery of spent reforming catalysts and hydrogenation catalysts. Hydrometallurgical leaching and alkali roasted methods are the main recycling technologies, which were widely used in industry. The comparison of different technologies has been provided and the existing challenges have also been put forward. Finally, with the aim to promote the sustainable development of petroleum industry, several considerations for highly and efficiently recovery of valuable metals from spent petroleum catalyst have been proposed.
催化剂在炼油领域发挥着重要作用。重整催化剂、加氢催化剂和流化催化裂化催化剂(FCC)在石油炼制中应用广泛,占催化剂总量的90%以上。因此,一旦催化剂失去效力和寿命终止,就会产生大量的废催化剂。废催化剂被归类为危险废物,其处置已成为炼油厂关注的焦点。废催化剂中含有Pt、Pd、Co、Mo、Ni、V、稀土等贵重金属,由于其环境问题和经济效益,回收利用受到了广泛关注。综述了从废石油催化剂中回收有价金属的回收技术,以及本课课组的最新研究成果。近年来,越来越多对环境影响较小的回收技术得到了发展。例如,有价金属的火法富集已成为废重整催化剂和加氢催化剂回收的研究热点。湿法冶金浸出法和碱焙烧法是目前工业上广泛应用的主要回收技术。对不同技术进行了比较,并提出了存在的问题。最后,为了促进石油工业的可持续发展,提出了从废石油催化剂中高效回收有价金属的几点考虑。
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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 Pub Date : 2026-06-19 Epub 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
Fractionation of guaiacyl and syringyl- lignin units using organic solvent nanofiltration 用有机溶剂纳滤分离愈创木酰和紫丁香酰木质素单元
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-02 DOI: 10.1016/j.seppur.2026.137099
Tim Croes , Abhishek Dutta , Korneel Van Aelst , Bert Sels , Bart Van der Bruggen , Iris Cornet
A major obstacle to employing the full potential of lignin-based aromatics is the fractionation of the monomers present in lignin, specifically the separation of guaiacyl (G) and syringyl (S) units, which possess nearly identical molecular weights (196 Da versus 166 Da) and dimensions, and identical functional groups. Such similarities make their separation highly challenging using conventional techniques and are generally considered beyond the capabilities of size-based membrane processes. This study examines the feasibility of organic solvent nanofiltration for fractionation of guaiacyl and syringyl units, and how membrane and process parameters affect separation of these two molecules. Sixteen commercially available membranes were tested with methanol and ethyl acetate as solvents. The results demonstrate that, despite the extreme similarity of the solutes, selective separation is achievable and is primarily governed by membrane material and solvent selection rather than the pore size-based molecular weight cut-off. Polyimide-based solvent-resistant membranes exhibited the highest selectivity, with a maximum observed separation factor of 3.33 obtained using a DuraMem™ 500 membrane in methanol. These findings demonstrate the potential of nanofiltration to address previously unresolved separation challenges in lignin valorization and provide a basis for further process development.
利用木质素基芳烃的全部潜力的一个主要障碍是木质素中单体的分离,特别是愈创木酰基(G)和丁香基(S)单元的分离,它们具有几乎相同的分子量(196da对166da)和尺寸,以及相同的官能团。这种相似性使得它们的分离使用传统技术非常具有挑战性,并且通常被认为超出了基于尺寸的膜处理的能力。本研究考察了有机溶剂纳滤分离愈创木酰基和丁香基单元的可行性,以及膜和工艺参数对这两种分子分离的影响。以甲醇和乙酸乙酯为溶剂对16种市售膜进行了测试。结果表明,尽管溶质非常相似,但选择性分离是可以实现的,并且主要由膜材料和溶剂的选择决定,而不是基于孔径的分子量切断。聚酰亚胺基耐溶剂膜表现出最高的选择性,使用DuraMem™500膜在甲醇中获得的最大分离系数为3.33。这些发现证明了纳滤在解决木质素增值中以前未解决的分离挑战方面的潜力,并为进一步的工艺开发提供了基础。
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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 Pub Date : 2026-06-19 Epub 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。
{"title":"Capacitive deionization based on Ti2P2O9: symmetrical electrode and synergistic removal mechanism of thallium and fluoride","authors":"Yupeng Li,&nbsp;Lei Huang,&nbsp;Zhu Xiong,&nbsp;Gaosheng Zhang","doi":"10.1016/j.seppur.2026.137151","DOIUrl":"10.1016/j.seppur.2026.137151","url":null,"abstract":"<div><div>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 Ti<sub>2</sub>P<sub>2</sub>O<sub>9</sub> 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 m<sup>2</sup>/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 Ti<sub>2</sub>P<sub>2</sub>O<sub>9</sub> 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: Ti<sub>2</sub>P<sub>2</sub>O<sub>9</sub>-F, Ti<sub>2</sub>P<sub>2</sub>O<sub>9</sub>-HF, Ti<sub>2</sub>P<sub>2</sub>O<sub>9</sub>-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.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137151"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172418","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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