首页 > 最新文献

Separation and Purification Technology最新文献

英文 中文
Novel heterojunction catalyst for the sustainable degradation of amoxicillin and propyl-2-thiourea: Ecotoxicity evaluation and mechanistic insights 可持续降解阿莫西林和丙基-2-硫脲的新型异质结催化剂:生态毒性评价和机理见解
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136853
Lalruatkima Ralte , Nehala Sona Payanthoth , Hmingsangzuali , Jinho Jung , Diwakar Tiwari
The occurrence of pharmaceutical and agrochemical residues such as amoxicillin (AMX) and propyl-2-thiourea (PTU) in aquatic environments poses significant environmental and health risks. The present study introduces a green route to synthesize a non-ferrous Fenton-like (NFFL) catalyst, ZY@C1C2, by incorporating cerium and copper nanoparticles into zeolite Y using Carica papaya leaf extract. Comprehensive characterization confirmed well-dispersed nanoparticles, enhanced surface properties, reduced band gap, and superior electron transfer capability. The catalyst demonstrated outstanding performance in degrading AMX and PTU under light irradiation, with efficiencies exceeding 90% within 120 min at near-neutral pH. Kinetic evaluation followed pseudo-first-order behavior, while LC-MS and DFT analyses elucidated radical-mediated oxidative pathways involving •OH radical attacks, stepwise bond cleavage, and progressive mineralization into CO2 and H2O. Total organic carbon removal further confirmed substantial mineralization of the contaminants. Furthermore, the experimental toxicity test using D. magna and prediction using ECOSAR, revealed that both the catalyst and intermediates exhibited low environmental toxicity. The ZY@C1C2 retained high activity after multiple reuse cycles, and its performance in natural spring water validated real-world applicability. The work highlights the promising utilization of the nanocatalysts as eco-friendly and scalable alternatives to conventional iron-based systems for the sustainable elimination of micropollutants from wastewater.
水生环境中阿莫西林(AMX)和丙基-2-硫脲(PTU)等药物和农用化学品残留物的出现构成了重大的环境和健康风险。本研究介绍了以番木瓜叶提取物为原料,将铈和铜纳米颗粒掺入Y沸石中合成非铁类芬顿(NFFL)催化剂ZY@C1C2的绿色途径。综合表征证实了分散良好的纳米颗粒,增强了表面性能,减小了带隙,并具有优越的电子转移能力。该催化剂在光照射下降解AMX和PTU的性能优异,在接近中性的ph下,在120分钟内效率超过90%。动力学评价遵循准一级行为,而LC-MS和DFT分析阐明了自由基介导的氧化途径,包括•OH自由基攻击,逐步裂解键,逐步矿化成CO2和H2O。总有机碳的去除进一步证实了污染物的大量矿化。此外,用D. magna进行的毒性实验和ECOSAR预测结果表明,催化剂和中间体均表现出较低的环境毒性。ZY@C1C2在多次重复使用后仍保持了较高的活性,其在天然泉水中的性能验证了其在现实世界中的适用性。这项工作强调了纳米催化剂作为传统铁基系统的环保和可扩展替代品的应用前景,以可持续地消除废水中的微污染物。
{"title":"Novel heterojunction catalyst for the sustainable degradation of amoxicillin and propyl-2-thiourea: Ecotoxicity evaluation and mechanistic insights","authors":"Lalruatkima Ralte ,&nbsp;Nehala Sona Payanthoth ,&nbsp;Hmingsangzuali ,&nbsp;Jinho Jung ,&nbsp;Diwakar Tiwari","doi":"10.1016/j.seppur.2026.136853","DOIUrl":"10.1016/j.seppur.2026.136853","url":null,"abstract":"<div><div>The occurrence of pharmaceutical and agrochemical residues such as amoxicillin (AMX) and propyl-2-thiourea (PTU) in aquatic environments poses significant environmental and health risks. The present study introduces a green route to synthesize a non-ferrous Fenton-like (NFFL) catalyst, ZY@C<sub>1</sub>C<sub>2</sub>, by incorporating cerium and copper nanoparticles into zeolite Y using <em>Carica papaya</em> leaf extract. Comprehensive characterization confirmed well-dispersed nanoparticles, enhanced surface properties, reduced band gap, and superior electron transfer capability. The catalyst demonstrated outstanding performance in degrading AMX and PTU under light irradiation, with efficiencies exceeding 90% within 120 min at near-neutral pH. Kinetic evaluation followed pseudo-first-order behavior, while LC-MS and DFT analyses elucidated radical-mediated oxidative pathways involving •OH radical attacks, stepwise bond cleavage, and progressive mineralization into CO<sub>2</sub> and H<sub>2</sub>O. Total organic carbon removal further confirmed substantial mineralization of the contaminants. Furthermore, the experimental toxicity test using <em>D. magna</em> and prediction using ECOSAR, revealed that both the catalyst and intermediates exhibited low environmental toxicity. The ZY@C<sub>1</sub>C<sub>2</sub> retained high activity after multiple reuse cycles, and its performance in natural spring water validated real-world applicability. The work highlights the promising utilization of the nanocatalysts as eco-friendly and scalable alternatives to conventional iron-based systems for the sustainable elimination of micropollutants from wastewater.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"389 ","pages":"Article 136853"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975450","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
Ionic liquids for the removal of pharmaceutical contaminants of emerging concern: a systematic review of extraction and purification strategies 离子液体用于去除新兴关注的药物污染物:提取和纯化策略的系统综述
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136836
Eduardo Villarroel-Utreras , Eduardo Vyhmeister , Juan Carlos Vidal , René Cabezas-Cornejo , Esteban Quijada-Maldonado , Lorenzo Reyes-Bozo
Emerging pollutants, particularly pharmaceuticals and endocrine-disrupting compounds, are a growing global concern due to their persistence, toxicity, and limited removal in conventional wastewater treatment systems. Ionic liquids (ILs) have emerged as versatile solvents and functional media with the potential to overcome these limitations. This review aims to provide an overview of the state of the art regarding the use of ILs to purify, extract, or facilitate the elimination of pharmacological components from various media. Covering the period 2021-2025, this work systematically maps advances in IL applications, classifying them by structural families (imidazolium, pyridinium, pyrrolidinium, ammonium, cholinium, phosphonium, sulfonium, and others); by pharmaceutical groups (antibiotics, NSAIDs, hormones, CNS drugs, cardiovascular drugs, anticancer agents, and other bioactives); and by purification processes (extraction, absorption, permeation, separation, and other applications). Imidazolium- and ammonium-based ILs dominate current studies, while cholinium ILs stand out as greener, biocompatible alternatives, and functionalized ILs offer niche applications. Despite these advances, challenges remain regarding toxicity, cost, and scalability. Overall, ILs demonstrate strong potential for the sustainable management of pharmaceutical pollutants, with opportunities for task-specific design and alignment with green chemistry principles.
新出现的污染物,特别是药物和干扰内分泌的化合物,由于其持久性、毒性和在传统废水处理系统中去除有限而日益受到全球关注。离子液体(ILs)作为一种多功能溶剂和功能介质已经出现,具有克服这些限制的潜力。这篇综述的目的是提供关于使用il来纯化、提取或促进从各种介质中消除药理成分的最新技术的概述。涵盖2021-2025年期间,本工作系统地绘制了IL应用的进展,并按结构族(咪唑、吡啶、吡咯吡啶、铵、胆、磷、磺胺等)对其进行了分类;药物组(抗生素、非甾体抗炎药、激素、中枢神经系统药物、心血管药物、抗癌药物和其他生物活性药物);并经纯化工艺(萃取、吸收、渗透、分离等应用)。咪唑类和氨类il在目前的研究中占主导地位,而胆碱类il则是更环保、生物相容性更好的替代品,而功能化的il则提供了小众应用。尽管取得了这些进步,但在毒性、成本和可扩展性方面仍然存在挑战。总体而言,ILs显示了药物污染物可持续管理的强大潜力,有机会进行特定任务的设计并与绿色化学原则保持一致。
{"title":"Ionic liquids for the removal of pharmaceutical contaminants of emerging concern: a systematic review of extraction and purification strategies","authors":"Eduardo Villarroel-Utreras ,&nbsp;Eduardo Vyhmeister ,&nbsp;Juan Carlos Vidal ,&nbsp;René Cabezas-Cornejo ,&nbsp;Esteban Quijada-Maldonado ,&nbsp;Lorenzo Reyes-Bozo","doi":"10.1016/j.seppur.2026.136836","DOIUrl":"10.1016/j.seppur.2026.136836","url":null,"abstract":"<div><div>Emerging pollutants, particularly pharmaceuticals and endocrine-disrupting compounds, are a growing global concern due to their persistence, toxicity, and limited removal in conventional wastewater treatment systems. Ionic liquids (ILs) have emerged as versatile solvents and functional media with the potential to overcome these limitations. This review aims to provide an overview of the state of the art regarding the use of ILs to purify, extract, or facilitate the elimination of pharmacological components from various media. Covering the period 2021-2025, this work systematically maps advances in IL applications, classifying them by structural families (imidazolium, pyridinium, pyrrolidinium, ammonium, cholinium, phosphonium, sulfonium, and others); by pharmaceutical groups (antibiotics, NSAIDs, hormones, CNS drugs, cardiovascular drugs, anticancer agents, and other bioactives); and by purification processes (extraction, absorption, permeation, separation, and other applications). Imidazolium- and ammonium-based ILs dominate current studies, while cholinium ILs stand out as greener, biocompatible alternatives, and functionalized ILs offer niche applications. Despite these advances, challenges remain regarding toxicity, cost, and scalability. Overall, ILs demonstrate strong potential for the sustainable management of pharmaceutical pollutants, with opportunities for task-specific design and alignment with green chemistry principles.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"389 ","pages":"Article 136836"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975628","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
Efficient removal of ibuprofen by a new electro-peroxone process via OH− separation in non-conductive membrane divided electrolytic cell: Performance and mechanisms 在非导电膜电解池中OH -分离电-过氧酮法高效去除布洛芬:性能和机理
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136822
Guoqiang Li, Runze Liu, Miaoqing Yang, Yiwei Zhao, Yimin Zhu, Lingen Wang, Long Huang, Yingke Fang, Yuan Li, Huiying Yang, Hongbin Xu
The persistent presence of recalcitrant micropollutants in aquatic environments poses significant environmental challenges. In this study, a porous polytetrafluoroethylene (PTFE) membrane was used to divide the traditional single-chamber Electro-peroxone (EP) process into a dual-chamber configuration (M/EP), and its pollutant degradation performance was systematically investigated. For ibuprofen (IBP) degradation, the M/EP process achieved a kinetic rate constant (kobs) of 0.215 min−1, which is markedly higher than those of the EP process (0.133 min−1) under the high alkaline conditions. This can be attributed to the fact that the •OH concentration generated in the M/EP process was 2 times higher than that in the EP process at initial pH 11. Quenching experiments revealed that •OH contributed the most to IBP degradation among the ROS. Meanwhile, the PTFE membrane prevents H2O2 migration and oxidation at the anode, resulting in 3 times higher H2O2 concentration in the cathodic chamber compared with the EP process. The kobs for the degradation of electron-deficient compounds was enhanced by 2.6–3.3 times compared to the EP process, while moderate improvements were also observed for neutral (1.7×) and electron-rich (1.15×) pollutants, along with a notable reduction in EE/O. Furthermore, degradation byproducts were identified via LC-MS to propose potential degradation pathways, and their toxicity was assessed. These findings demonstrate that the M/EP process offers a promising strategy for the degradation of trace organic micropollutants from water.
水生环境中顽固性微污染物的持续存在构成了重大的环境挑战。本研究采用多孔聚四氟乙烯(PTFE)膜将传统的单室电-过氧酮(EP)工艺划分为双室配置(M/EP),并对其污染物降解性能进行系统研究。高碱性条件下,M/EP法降解布洛芬(IBP)的动力学速率常数(kobs)为0.215 min−1,显著高于EP法(0.133 min−1)。这可以归因于在初始pH 11下,M/EP过程中产生的•OH浓度比EP过程高2倍。猝灭实验表明,在活性氧中,•OH对IBP的降解作用最大。同时,PTFE膜阻止了H2O2在阳极的迁移和氧化,导致阴极室中H2O2浓度比EP工艺高3倍。与EP工艺相比,缺乏电子化合物的降解效率提高了2.6-3.3倍,而中性(1.7倍)和富电子(1.15倍)污染物的降解效率也有适度提高,同时EE/O也显著降低。此外,通过LC-MS鉴定降解副产物,提出潜在的降解途径,并评估其毒性。这些发现表明,M/EP工艺为降解水中痕量有机微污染物提供了一种有前途的策略。
{"title":"Efficient removal of ibuprofen by a new electro-peroxone process via OH− separation in non-conductive membrane divided electrolytic cell: Performance and mechanisms","authors":"Guoqiang Li, Runze Liu, Miaoqing Yang, Yiwei Zhao, Yimin Zhu, Lingen Wang, Long Huang, Yingke Fang, Yuan Li, Huiying Yang, Hongbin Xu","doi":"10.1016/j.seppur.2026.136822","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.136822","url":null,"abstract":"The persistent presence of recalcitrant micropollutants in aquatic environments poses significant environmental challenges. In this study, a porous polytetrafluoroethylene (PTFE) membrane was used to divide the traditional single-chamber Electro-peroxone (EP) process into a dual-chamber configuration (M/EP), and its pollutant degradation performance was systematically investigated. For ibuprofen (IBP) degradation, the M/EP process achieved a kinetic rate constant (<em>k</em><sub>obs</sub>) of 0.215 min<sup>−1</sup>, which is markedly higher than those of the EP process (0.133 min<sup>−1</sup>) under the high alkaline conditions. This can be attributed to the fact that the •OH concentration generated in the M/EP process was 2 times higher than that in the EP process at initial pH 11. Quenching experiments revealed that •OH contributed the most to IBP degradation among the ROS. Meanwhile, the PTFE membrane prevents H<sub>2</sub>O<sub>2</sub> migration and oxidation at the anode, resulting in 3 times higher H<sub>2</sub>O<sub>2</sub> concentration in the cathodic chamber compared with the EP process. The <em>k</em><sub>obs</sub> for the degradation of electron-deficient compounds was enhanced by 2.6–3.3 times compared to the EP process, while moderate improvements were also observed for neutral (1.7×) and electron-rich (1.15×) pollutants, along with a notable reduction in EE/O. Furthermore, degradation byproducts were identified via LC-MS to propose potential degradation pathways, and their toxicity was assessed. These findings demonstrate that the M/EP process offers a promising strategy for the degradation of trace organic micropollutants from water.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"46 1","pages":"136822"},"PeriodicalIF":8.6,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145961912","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
Study on the hydrogen production mechanism of the MnCo2S4/TaTp-COF heterojunction driven by the interface confinement effect 界面约束效应驱动下MnCo2S4/ tap - cof异质结产氢机理研究
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136817
Jiayao Du , Xian Yan , Lijun Zhang , Zhiliang Jin
Covalent organic frameworks (COFs) have emerged as versatile platforms for photocatalysis. However, inefficient charge separation at hybrid interfaces remains a critical bottleneck. Herein, we conceptually construct a Schiff base-type COF (TaTp-COF)/MnCo2S4 heterojunction photocatalyst via an in situ growth strategy. Interfacial inhomogeneity and asymmetry at the TaTp-COF/ MnCo2S4 heterointerface give rise to an interface confinement effect, which induces directional electron transfer and localized charge accumulation, thereby effectively suppressing charge recombination. Density functional theory calculations, together with experimental evidence, reveal an interfacial charge redistribution that governs the charge separation behavior and photocatalytic performance. Consequently, the optimized TaTp-COF/ MnCo2S4 composite containing 3 wt% MnCo2S4 exhibits a total hydrogen evolution of 22,651 μmol·h−1·g−1, significantly outperforming the individual components. This work elucidates the hydrogen production mechanism driven by the interface confinement effect and establishes interfacial charge confinement as a decisive design principle for COF-based heterojunction photocatalysts.
共价有机框架(COFs)已成为光催化的通用平台。然而,在混合界面上低效率的电荷分离仍然是一个关键的瓶颈。在此,我们通过原位生长策略在概念上构建了希夫碱型COF (tap -COF)/MnCo2S4异质结光催化剂。ttap - cof / MnCo2S4异质界面的界面不均匀性和不对称性导致界面约束效应,导致定向电子转移和局域电荷积累,从而有效抑制电荷复合。密度泛函理论计算,结合实验证据,揭示了控制电荷分离行为和光催化性能的界面电荷重新分配。结果表明,含3 wt% MnCo2S4的ttap - cof / MnCo2S4复合材料的总析氢量为22,651 μmol·h−1·g−1,明显优于单个组分。本研究阐明了界面约束效应驱动的产氢机理,确立了界面电荷约束作为cof基异质结光催化剂设计的决定性原则。
{"title":"Study on the hydrogen production mechanism of the MnCo2S4/TaTp-COF heterojunction driven by the interface confinement effect","authors":"Jiayao Du ,&nbsp;Xian Yan ,&nbsp;Lijun Zhang ,&nbsp;Zhiliang Jin","doi":"10.1016/j.seppur.2026.136817","DOIUrl":"10.1016/j.seppur.2026.136817","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs) have emerged as versatile platforms for photocatalysis. However, inefficient charge separation at hybrid interfaces remains a critical bottleneck. Herein, we conceptually construct a Schiff base-type COF (TaTp-COF)/MnCo2S4 heterojunction photocatalyst via an in situ growth strategy. Interfacial inhomogeneity and asymmetry at the TaTp-COF/ MnCo<sub>2</sub>S<sub>4</sub> heterointerface give rise to an interface confinement effect, which induces directional electron transfer and localized charge accumulation, thereby effectively suppressing charge recombination. Density functional theory calculations, together with experimental evidence, reveal an interfacial charge redistribution that governs the charge separation behavior and photocatalytic performance. Consequently, the optimized TaTp-COF/ MnCo<sub>2</sub>S<sub>4</sub> composite containing 3 wt% MnCo<sub>2</sub>S<sub>4</sub> exhibits a total hydrogen evolution of 22,651 μmol·h−1·g−1, significantly outperforming the individual components. This work elucidates the hydrogen production mechanism driven by the interface confinement effect and establishes interfacial charge confinement as a decisive design principle for COF-based heterojunction photocatalysts.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"388 ","pages":"Article 136817"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974318","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
Robust phosphate removal by La₂O₂CO₃ in karst waters: Unraveling the promoting role of carbonate through in-situ analysis and theoretical calculation La₂O₂CO₃在岩溶水中的强力除磷作用:通过原位分析和理论计算揭示碳酸盐的促进作用
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136839
Chenge Liang , Yang Wu , Shihao Miao , Yi Shen , Yungui Li , Qingqing Li , Qile Fang
The efficacy of lanthanum (La)-based materials for phosphorus pollution control in karst regions is significantly challenged by the ubiquitous presence of high-concentration carbonates. Herein, the influence and interaction mechanisms of carbonate on phosphate adsorption were systematically investigated across four La-based materials (La₂O₃, La(OH)₃, La₂(CO₃)₃, and La₂O₂CO₃). Contrary to the pronounced inhibition observed on the other three adsorbents, La₂O₂CO₃ exhibited robust phosphate adsorption capacity even with carbonate coexistence. In-situ quartz crystal microbalance with dissipation (QCM-D) monitoring revealed a preferential adsorption of carbonate onto La₂O₂CO₃ during the initial stage, which subsequently facilitated phosphate uptake under alkaline conditions. Combined characterization and density functional theory (DFT) calculations elucidated that the pre-adsorbed carbonate primarily adopted a monodentate mononuclear configuration on La₂O₂CO₃. This configuration induced electron transfer from active La sites to carbonates, thereby significantly enhancing the adsorption energy for phosphate from −164.8 kJ/mol to −311.1 kJ/mol. Consequently, La₂O₂CO₃ demonstrated excellent, consecutive phosphate removal performance in a simulated high‑carbonate karst waterbody. This work unveils a unique carbonate-assisted phosphate adsorption mechanism and highlights the substantial potential of La₂O₂CO₃ for efficient phosphorus remediation in carbonate-rich environments.
由于岩溶地区普遍存在高浓度碳酸盐,镧基材料控制磷污染的效果受到极大挑战。本文系统地研究了四种La基材料(La₂O₃、La(OH)₃、La₂(CO)₃和La₂O₂CO₃)对磷酸盐吸附的影响及其相互作用机理。与在其他三种吸附剂上观察到的明显的抑制作用相反,即使在碳酸盐共存的情况下,La₂O₂CO₃也表现出强大的磷酸盐吸附能力。原位石英晶体耗散微平衡(QCM-D)监测显示,在初始阶段,碳酸盐优先吸附在La₂O₂CO₃上,随后在碱性条件下促进了磷酸盐的吸收。结合表征和密度泛函理论(DFT)计算表明,预吸附的碳酸盐在La₂O₂CO₃上主要采用单齿单核构型。这种结构诱导电子从活性La位转移到碳酸盐,从而显著提高了对磷酸盐的吸附能,从- 164.8 kJ/mol增加到- 311.1 kJ/mol。因此,La₂O₂CO₃在模拟高碳酸盐岩溶水体中表现出优异的连续除磷性能。这项工作揭示了一种独特的碳酸盐辅助磷酸盐吸附机制,并强调了La₂O₂CO₃在富含碳酸盐的环境中有效修复磷的巨大潜力。
{"title":"Robust phosphate removal by La₂O₂CO₃ in karst waters: Unraveling the promoting role of carbonate through in-situ analysis and theoretical calculation","authors":"Chenge Liang ,&nbsp;Yang Wu ,&nbsp;Shihao Miao ,&nbsp;Yi Shen ,&nbsp;Yungui Li ,&nbsp;Qingqing Li ,&nbsp;Qile Fang","doi":"10.1016/j.seppur.2026.136839","DOIUrl":"10.1016/j.seppur.2026.136839","url":null,"abstract":"<div><div>The efficacy of lanthanum (La)-based materials for phosphorus pollution control in karst regions is significantly challenged by the ubiquitous presence of high-concentration carbonates. Herein, the influence and interaction mechanisms of carbonate on phosphate adsorption were systematically investigated across four La-based materials (La₂O₃, La(OH)₃, La₂(CO₃)₃, and La₂O₂CO₃). Contrary to the pronounced inhibition observed on the other three adsorbents, La₂O₂CO₃ exhibited robust phosphate adsorption capacity even with carbonate coexistence. In-situ quartz crystal microbalance with dissipation (QCM-D) monitoring revealed a preferential adsorption of carbonate onto La₂O₂CO₃ during the initial stage, which subsequently facilitated phosphate uptake under alkaline conditions. Combined characterization and density functional theory (DFT) calculations elucidated that the pre-adsorbed carbonate primarily adopted a monodentate mononuclear configuration on La₂O₂CO₃. This configuration induced electron transfer from active La sites to carbonates, thereby significantly enhancing the adsorption energy for phosphate from −164.8 kJ/mol to −311.1 kJ/mol. Consequently, La₂O₂CO₃ demonstrated excellent, consecutive phosphate removal performance in a simulated high‑carbonate karst waterbody. This work unveils a unique carbonate-assisted phosphate adsorption mechanism and highlights the substantial potential of La₂O₂CO₃ for efficient phosphorus remediation in carbonate-rich environments.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"388 ","pages":"Article 136839"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974329","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
Engineering a nanofiltration membrane with high mono-/divalent anion selectivity and antifouling properties via L-histidine incorporation 通过l -组氨酸掺入,设计一种具有高单/二价阴离子选择性和防污性能的纳滤膜
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136851
Ruohan Liang , Dongsheng Zhao , Fangming Jin , Jun Xu , Guicai Liu
The limited mono−/divalent anion selectivity and inadequate antifouling properties of polyamide (PA) nanofiltration (NF) membranes restrict their use in water treatment. Herein, L-histidine (L-His)-modified NF membranes were prepared through interfacial polymerization on a polyethersulfone porous substrate. The aqueous-phase comonomers were piperazine and L-His, which contain both amino and carboxyl groups, while the organic-phase monomer was trimesoyl chloride. Compared with the NF0 membrane without addition of L-His, all of the L-His-modified membrane was characterized by a higher surface roughness, a thinner PA layer, greater hydrophilicity, a more negative surface charge and a larger mean pore size. Among them, the optimal NF0.5 membrane with the addition of 0.5% (w/v) L-His demonstrated a pure water permeability of 17.9 L/(m2·h·bar) and a 2.7-fold higher NaCl/Na2SO4 selectivity (up to 102.0). In particular, the NaCl/Na2SO4 selectivity improved with higher operating pressure, but decreased with increasing single-salt concentration or NaCl/Na2SO4 mass ratio in the feed solution. In addition, the NF0.5 membrane demonstrated superior resistance to protein fouling and outstanding long-term operational stability throughout a continuous 7-day filtration process. This study could provide valuable insights into the development of NF membranes with high mono−/divalent anion selectivity and excellent antifouling properties.
聚酰胺(PA)纳滤(NF)膜有限的单/二价阴离子选择性和不充分的防污性能限制了其在水处理中的应用。在聚醚砜多孔基质上,采用界面聚合法制备了l -组氨酸修饰的NF膜。水相单体为哌嗪和L-His,它们同时含有氨基和羧基,而有机相单体为三甲基氯。与未添加L-His的NF0膜相比,L-His修饰的膜表面粗糙度更高,PA层更薄,亲水性更强,表面负电荷更多,平均孔径更大。其中,添加0.5% (w/v) L- his的NF0.5膜的纯水渗透率为17.9 L/(m2·h·bar), NaCl/Na2SO4选择性提高2.7倍(达102.0)。NaCl/Na2SO4的选择性随操作压力的增加而提高,但随进料溶液中单盐浓度或NaCl/Na2SO4质量比的增加而降低。此外,NF0.5膜在连续7天的过滤过程中表现出优异的抗蛋白质污染能力和出色的长期运行稳定性。该研究为开发具有高单/二价阴离子选择性和优异防污性能的纳滤膜提供了有价值的见解。
{"title":"Engineering a nanofiltration membrane with high mono-/divalent anion selectivity and antifouling properties via L-histidine incorporation","authors":"Ruohan Liang ,&nbsp;Dongsheng Zhao ,&nbsp;Fangming Jin ,&nbsp;Jun Xu ,&nbsp;Guicai Liu","doi":"10.1016/j.seppur.2026.136851","DOIUrl":"10.1016/j.seppur.2026.136851","url":null,"abstract":"<div><div>The limited mono−/divalent anion selectivity and inadequate antifouling properties of polyamide (PA) nanofiltration (NF) membranes restrict their use in water treatment. Herein, L-histidine (L-His)-modified NF membranes were prepared through interfacial polymerization on a polyethersulfone porous substrate. The aqueous-phase comonomers were piperazine and L-His, which contain both amino and carboxyl groups, while the organic-phase monomer was trimesoyl chloride. Compared with the NF0 membrane without addition of L-His, all of the L-His-modified membrane was characterized by a higher surface roughness, a thinner PA layer, greater hydrophilicity, a more negative surface charge and a larger mean pore size. Among them, the optimal NF0.5 membrane with the addition of 0.5% (<em>w</em>/<em>v</em>) L-His demonstrated a pure water permeability of 17.9 L/(m<sup>2</sup>·h·bar) and a 2.7-fold higher NaCl/Na<sub>2</sub>SO<sub>4</sub> selectivity (up to 102.0). In particular, the NaCl/Na<sub>2</sub>SO<sub>4</sub> selectivity improved with higher operating pressure, but decreased with increasing single-salt concentration or NaCl/Na<sub>2</sub>SO<sub>4</sub> mass ratio in the feed solution. In addition, the NF0.5 membrane demonstrated superior resistance to protein fouling and outstanding long-term operational stability throughout a continuous 7-day filtration process. This study could provide valuable insights into the development of NF membranes with high mono−/divalent anion selectivity and excellent antifouling properties.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"389 ","pages":"Article 136851"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145950105","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
Flue gas desulfurization gypsum enhanced Cd and Pb immobilization by sulfate-reducing bacterium 烟气脱硫石膏增强硫酸盐还原菌对镉、铅的固定化作用
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136831
Zheng Wu, Liang Xiao
This study aimed to investigate the effectiveness and mechanisms of immobilizing Cd and Pb in water and soil using industrial by-product flue gas desulfurization gypsum (FGD gypsum) as a slow-release sulfur source, combined with the sulfate-reducing bacterium (SRB) Clostridium sulfidigenes HY-1. Batch experiments were conducted to evaluate the sulfate reduction efficiency of strain HY-1 utilizing different types of gypsum (FGD gypsum, phospho gypsum, titan gypsum) as sulfur sources. The effects of key parameters, including FGD gypsum dosage, temperature, pH, salinity, inoculum size, and initial heavy metal concentration, on the immobilization of Cd2+ and Pb2+ were systematically examined. The immobilization products were characterized using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The remediation potential was further validated through soil incubation experiments. FGD gypsum was identified as the most effective sulfur source for strain HY-1, achieving a sulfate reduction rate of up to 60% under optimal conditions (pH 7.0–8.0, 35 °C, salinity 2.0 g/L NaCl, inoculum size 4 × 106 cells/mL). With an FGD gypsum dosage of 10 g/L, the immobilization rates for 5 mg/L Cd2+ and 30 mg/L Pb2+ reached 79% and 89.3%, respectively. Characterization analyses confirmed that the primary immobilization products were stable CdS and PbS crystals. Soil remediation experiments demonstrated that the “SRB + FGD gypsum” treatment effectively decreased the acid-extractable fraction and increased the residual fraction of Cd and Pb in the soil. Clostridium sulfidigenes HY-1 can efficiently utilize sulfate from FGD gypsum to biogenically induce the precipitation of metal sulfides, leading to the effective immobilization of Cd2+ and Pb2+. This technology adopts a “waste-treats-waste” approach, offering a promising novel strategy for heavy metal pollution control and the resource utilization of industrial solid waste.
本研究旨在探讨以工业副产烟气脱硫石膏(FGD石膏)为缓释硫源,结合硫酸盐还原菌(Clostridium sulfidigenes HY-1)对水和土壤中Cd和Pb的固定化效果及机制。采用不同类型的石膏(脱硫石膏、磷石膏、泰坦石膏)作为硫源,对菌株HY-1的硫酸盐还原效果进行了批量试验。系统考察了脱硫石膏投加量、温度、pH、盐度、接种量、初始重金属浓度等关键参数对固定化Cd2+和Pb2+的影响。采用扫描电镜(SEM)、傅里叶变换红外光谱(FTIR)、x射线衍射(XRD)和x射线光电子能谱(XPS)对固定化产物进行了表征。通过土壤培养实验进一步验证了其修复潜力。FGD石膏被确定为菌株HY-1最有效的硫源,在最佳条件下(pH 7.0-8.0,35 °C,盐度2.0 g/L NaCl,接种量4 × 106个细胞/mL),硫酸盐还原率高达60%。当脱硫石膏投加量为10 g/L时,对5 mg/L Cd2+和30 mg/L Pb2+的固定化率分别达到79%和89.3%。表征分析证实了初级固定产物是稳定的CdS和PbS晶体。土壤修复实验表明,“SRB + FGD石膏”处理有效降低了土壤中酸萃取组分,增加了土壤中Cd和Pb的残留组分。硫代梭菌HY-1可以有效地利用脱硫石膏中的硫酸盐生物诱导金属硫化物的沉淀,从而有效地固定Cd2+和Pb2+。该技术采用“废物-处理-废物”的方法,为重金属污染控制和工业固体废物资源化利用提供了一种有前景的新策略。
{"title":"Flue gas desulfurization gypsum enhanced Cd and Pb immobilization by sulfate-reducing bacterium","authors":"Zheng Wu, Liang Xiao","doi":"10.1016/j.seppur.2026.136831","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.136831","url":null,"abstract":"This study aimed to investigate the effectiveness and mechanisms of immobilizing Cd and Pb in water and soil using industrial by-product flue gas desulfurization gypsum (FGD gypsum) as a slow-release sulfur source, combined with the sulfate-reducing bacterium (SRB) <em>Clostridium sulfidigenes</em> HY-1. Batch experiments were conducted to evaluate the sulfate reduction efficiency of strain HY-1 utilizing different types of gypsum (FGD gypsum, phospho gypsum, titan gypsum) as sulfur sources. The effects of key parameters, including FGD gypsum dosage, temperature, pH, salinity, inoculum size, and initial heavy metal concentration, on the immobilization of Cd<sup>2+</sup> and Pb<sup>2+</sup> were systematically examined. The immobilization products were characterized using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The remediation potential was further validated through soil incubation experiments. FGD gypsum was identified as the most effective sulfur source for strain HY-1, achieving a sulfate reduction rate of up to 60% under optimal conditions (pH 7.0–8.0, 35 °C, salinity 2.0 g/L NaCl, inoculum size 4 × 10<sup>6</sup> cells/mL). With an FGD gypsum dosage of 10 g/L, the immobilization rates for 5 mg/L Cd<sup>2+</sup> and 30 mg/L Pb<sup>2+</sup> reached 79% and 89.3%, respectively. Characterization analyses confirmed that the primary immobilization products were stable CdS and PbS crystals. Soil remediation experiments demonstrated that the “SRB + FGD gypsum” treatment effectively decreased the acid-extractable fraction and increased the residual fraction of Cd and Pb in the soil. <em>Clostridium sulfidigenes</em> HY-1 can efficiently utilize sulfate from FGD gypsum to biogenically induce the precipitation of metal sulfides, leading to the effective immobilization of Cd<sup>2+</sup> and Pb<sup>2+</sup>. This technology adopts a “waste-treats-waste” approach, offering a promising novel strategy for heavy metal pollution control and the resource utilization of industrial solid waste.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"38 1","pages":"136831"},"PeriodicalIF":8.6,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145961869","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 the gas permeance of the fly-ash based ceramic membranes for ultra-fine particles filtration at high temperatures 提高粉煤灰基陶瓷膜高温超细颗粒过滤的透气性
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136848
Ying Yang, Shiying Ni, Dudu Yang, Huandi Yao, Dong Zou, Zhaoxiang Zhong, Weihong Xing
Fly-ash is widely available and its chemical composition is similar to traditional ceramic membrane materials. Thus, using fly ash to produce low-cost ceramic membranes can achieve waste resource utilization and environment protection simultaneously. However, the broad size distribution of fly ash leads to densely packed structures with limited interconnected porosity during sintering. In this work, a fly-ash based ceramic membrane was fabricated through phase inversion and one-step sintering. The process involved introducing rigid Al2O3 particles during the phase inversion step to inhibit the densification of fly ash and refine the pore structure, thereby creating an asymmetric structure characterized by finger-like pores. This strategy greatly enhanced the gas permeance of the membrane. It was indicated that the membrane had an average pore size of ~4.10 μm by optimizing the sintering temperature and solid content of the dope solution, exhibiting an excellent gas permeance of 687.51 m3·m−2·h−1·kPa−1. Moreover, the membrane exhibited outstanding thermal shock resistance after 15 cycles between 25 °C and 800 °C. In the filtration of ultra-fine particles (mean size of ~300 nm) at high temperatures, the membrane achieved a filtration efficiency of 99.99% with a low pressure drop in a 12-h filtration process at 300 °C. Compared with the literature, the fly-ash based ceramic membrane developed by phase inversion displayed superior gas permeance and lower filtration pressure drop. This work proposed an effective and feasible solution for alternative materials in ceramic membranes used for ultra-fine particles filtration at high temperatures.
粉煤灰应用广泛,其化学成分与传统陶瓷膜材料相似。因此,利用粉煤灰生产低成本陶瓷膜,可以实现废弃物资源化利用和环境保护的同时实现。然而,粉煤灰的宽尺寸分布导致了烧结过程中致密的结构和有限的互连孔隙率。本文采用相变和一步烧结法制备了粉煤灰基陶瓷膜。该工艺通过在相转变步骤中引入刚体Al2O3颗粒来抑制粉煤灰致密化并细化孔隙结构,从而形成以指状孔隙为特征的不对称结构。这一策略大大提高了膜的透气性。通过对烧结温度和固相含量的优化,发现该膜的平均孔径为~4.10 μm,透气性为687.51 m3·m−2·h−1·kPa−1。此外,在25 °C和800 °C之间进行15次 循环后,膜表现出出色的抗热震性。在高温下过滤超细颗粒(平均粒径~300 nm)时,膜在300 ℃下经过12 h的低压降过滤,过滤效率达到99.99%。与文献相比,相转化制备的粉煤灰基陶瓷膜具有优异的透气性和较低的过滤压降。本工作为陶瓷膜高温超细颗粒过滤的替代材料提供了一种有效可行的解决方案。
{"title":"Boosting the gas permeance of the fly-ash based ceramic membranes for ultra-fine particles filtration at high temperatures","authors":"Ying Yang, Shiying Ni, Dudu Yang, Huandi Yao, Dong Zou, Zhaoxiang Zhong, Weihong Xing","doi":"10.1016/j.seppur.2026.136848","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.136848","url":null,"abstract":"Fly-ash is widely available and its chemical composition is similar to traditional ceramic membrane materials. Thus, using fly ash to produce low-cost ceramic membranes can achieve waste resource utilization and environment protection simultaneously. However, the broad size distribution of fly ash leads to densely packed structures with limited interconnected porosity during sintering. In this work, a fly-ash based ceramic membrane was fabricated through phase inversion and one-step sintering. The process involved introducing rigid Al<sub>2</sub>O<sub>3</sub> particles during the phase inversion step to inhibit the densification of fly ash and refine the pore structure, thereby creating an asymmetric structure characterized by finger-like pores. This strategy greatly enhanced the gas permeance of the membrane. It was indicated that the membrane had an average pore size of ~4.10 μm by optimizing the sintering temperature and solid content of the dope solution, exhibiting an excellent gas permeance of 687.51 m<sup>3</sup>·m<sup>−2</sup>·h<sup>−1</sup>·kPa<sup>−1</sup>. Moreover, the membrane exhibited outstanding thermal shock resistance after 15 cycles between 25 °C and 800 °C. In the filtration of ultra-fine particles (mean size of ~300 nm) at high temperatures, the membrane achieved a filtration efficiency of 99.99% with a low pressure drop in a 12-h filtration process at 300 °C. Compared with the literature, the fly-ash based ceramic membrane developed by phase inversion displayed superior gas permeance and lower filtration pressure drop. This work proposed an effective and feasible solution for alternative materials in ceramic membranes used for ultra-fine particles filtration at high temperatures.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"54 1","pages":"136848"},"PeriodicalIF":8.6,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145961911","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
Piezoelectric catalysis for selective recovery of precious metals (Cu and Au) from waste CPUs 压电催化从废cpu中选择性回收贵金属(Cu和Au)
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136854
Jiangyuan Qiu , Ruxin Liu , Tao Yu , Wenxuan Li , Lingyuan Wu , Weiming Zhong , Ting Wan , Rui Guo , Zaiyin Huang , Xuanwen Liu
This study addresses the technical challenges of traditional processes for precious metal recovery from electronic waste, including high energy consumption, severe pollution, and the use of highly corrosive reagents. We innovatively propose a green recovery strategy based on piezoelectric catalysis. By combining the compositional characteristics of electronic waste (Cu > 80 wt%, Au 0.1–0.5 wt%) with the hard-soft acid-base (HSAB) theory, we developed a BOC-NH₄Cl-CH₃CN-H₂O catalytic system. This system achieves efficient dissolution of copper and gold (1334 mg h−1·g-cat−1 and 2.7 mg h−1·g-cat−1, respectively) through an oxidation-coordination mechanism, with dissolution rates reaching 99.8% and 95.5% in simulated systems and enrichment purity exceeding 99%. Based on the experimental data, it is proposed that under piezocatalysis, acetonitrile is oxidized to acetamide, which then synergistically coordinates with NH₃/Cl to form stable coordination products (with binding energies of E_Cu = −4.034 eV and E_Au = −2.993 eV, respectively). This process may serve as a key mechanism responsible for the significant enhancement of metal dissolution. Due to the lower oxidation potential of Cu ( = 0.34 V) compared to Au ( = 1.5 V), the system exhibits a “high‑copper, low-gold” selective dissolution characteristic that aligns well with waste composition. This technology provides an efficient and environmentally friendly solution for metal recovery from electronic waste.
本研究解决了从电子废物中回收贵金属的传统工艺所面临的技术挑战,包括高能耗、严重污染和使用高腐蚀性试剂。我们创新性地提出了一种基于压电催化的绿色回收策略。结合电子废弃物的组成特点(Cu > 80 wt%, Au 0.1 ~ 0.5 wt%)和硬-软酸碱(HSAB)理论,建立了BOC-NH₄Cl-CH₃CN-H₂O催化体系。该体系通过氧化配位机制实现了铜和金的高效溶出(分别为1334 mg h−1·g-cat−1和2.7 mg h−1·g-cat−1),在模拟体系中溶出率分别达到99.8%和95.5%,富集纯度超过99%。根据实验数据,提出在压催化作用下乙腈氧化生成乙酰胺,乙酰胺与nh3 /Cl -协同配位形成稳定的配位产物(结合能分别为E_Cu = - 4.034 eV和E_Au = - 2.993 eV)。这一过程可能是显著增强金属溶解的关键机制。由于Cu (E°= 0.34 V)的氧化电位比Au (E°= 1.5 V)低,该体系表现出“高铜、低金”的选择性溶解特性,这与废物成分很好地吻合。这项技术为从电子废物中回收金属提供了一种高效环保的解决方案。
{"title":"Piezoelectric catalysis for selective recovery of precious metals (Cu and Au) from waste CPUs","authors":"Jiangyuan Qiu ,&nbsp;Ruxin Liu ,&nbsp;Tao Yu ,&nbsp;Wenxuan Li ,&nbsp;Lingyuan Wu ,&nbsp;Weiming Zhong ,&nbsp;Ting Wan ,&nbsp;Rui Guo ,&nbsp;Zaiyin Huang ,&nbsp;Xuanwen Liu","doi":"10.1016/j.seppur.2026.136854","DOIUrl":"10.1016/j.seppur.2026.136854","url":null,"abstract":"<div><div>This study addresses the technical challenges of traditional processes for precious metal recovery from electronic waste, including high energy consumption, severe pollution, and the use of highly corrosive reagents. We innovatively propose a green recovery strategy based on piezoelectric catalysis. By combining the compositional characteristics of electronic waste (Cu &gt; 80 wt%, Au 0.1–0.5 wt%) with the hard-soft acid-base (HSAB) theory, we developed a BOC-NH₄Cl-CH₃CN-H₂O catalytic system. This system achieves efficient dissolution of copper and gold (1334 mg h<sup>−1</sup>·g-cat<sup>−1</sup> and 2.7 mg h<sup>−1</sup>·g-cat<sup>−1</sup>, respectively) through an oxidation-coordination mechanism, with dissolution rates reaching 99.8% and 95.5% in simulated systems and enrichment purity exceeding 99%. Based on the experimental data, it is proposed that under piezocatalysis, acetonitrile is oxidized to acetamide, which then synergistically coordinates with NH₃/Cl<sup>−</sup> to form stable coordination products (with binding energies of E_Cu = −4.034 eV and E_Au = −2.993 eV, respectively). This process may serve as a key mechanism responsible for the significant enhancement of metal dissolution. Due to the lower oxidation potential of Cu (<em>E°</em> = 0.34 V) compared to Au (<em>E°</em> = 1.5 V), the system exhibits a “high‑copper, low-gold” selective dissolution characteristic that aligns well with waste composition. This technology provides an efficient and environmentally friendly solution for metal recovery from electronic waste.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"389 ","pages":"Article 136854"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975400","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
Recovery of lead and fluorine from non-ferrous smelting acid sludge by synergistic leaching and stepwise precipitation 协同浸出-分步沉淀法回收有色冶炼酸泥中的铅和氟
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-09 DOI: 10.1016/j.seppur.2026.136793
Ziyuan Liu , Xiaoguang Zhang , Zhe Tan , De'an Pan , Guosai Jiang
Acid sludge, a hazardous waste from lead (Pb) and zinc (Zn) smelting process, commonly contains low-boiling-point elements such as Pb and fluorine (F). However, the complex phase composition of acid sludge typically results in low recovery efficiencies of Pb and F. Herein, we proposed an efficient recovery method for Pb and F through synergistic leaching using a solution containing aluminum ions (Al3+) and chloride ions (Cl) followed by stepwise precipitation involving PbCl2 cooling crystallization and cryolite formation. The single-factor experiment results showed the leaching efficiencies of 98.37% and 92.35% for Pb and F, respectively, which is superior to that of the separate leaching of Pb or F process, due to the intermingle structure of Pb and F phases in acid sludge. The precipitation efficiencies reached 94.44% for Pb and 97.88% for F, and the obtained PbCl2 and cryolite products meet national standards. Density functional theory (DFT) calculations revealed the chemical states of Al3+, calcium ion (Ca2+), and F in leaching solution and their coexistence mechanism, and thermodynamic analysis clarified the preferential precipitation of cryolite with high quality. Further, the Life Cycle Assessment (LCA) and economic evaluation were conducted for the entire recovery process, indicating the significantly economic and environmental benefits with a cost of only ¥1.61 for treating 100 g of acid sludge. This study provides an efficient and sustainable method for recovering Pb and F from acid sludge, which not only mitigates environmental hazards but also enhances resource valorization, thereby supporting the development of a circular economy in the non-ferrous metal industry.
酸性污泥是铅(Pb)和锌(Zn)冶炼过程产生的危险废物,通常含有低沸点元素,如Pb和氟(F)。然而,酸性污泥的复杂相组成通常导致Pb和F的回收效率较低。为此,我们提出了一种高效的Pb和F回收方法,即使用含有铝离子(Al3+)和氯离子(Cl−)的溶液进行协同浸出,然后通过PbCl2冷却结晶和冰晶石形成的逐步沉淀。单因素试验结果表明,由于酸性污泥中Pb和F相的混合结构,Pb和F的浸出效率分别为98.37%和92.35%,优于单独浸出Pb或F的工艺。Pb的沉淀效率为94.44%,F的沉淀效率为97.88%,所得的PbCl2和冰晶石产品均达到国家标准。密度泛函理论(DFT)计算揭示了浸出液中Al3+、钙离子(Ca2+)和F−的化学态及其共存机理,热力学分析明确了高质量冰晶石的优先沉淀。对整个回收过程进行了生命周期评价(LCA)和经济评价,表明处理100 g酸污泥的成本仅为1.61元,具有显著的经济效益和环境效益。本研究为从酸性污泥中回收铅和F提供了一种高效、可持续的方法,既减轻了环境危害,又提高了资源价值,从而支持有色金属工业循环经济的发展。
{"title":"Recovery of lead and fluorine from non-ferrous smelting acid sludge by synergistic leaching and stepwise precipitation","authors":"Ziyuan Liu ,&nbsp;Xiaoguang Zhang ,&nbsp;Zhe Tan ,&nbsp;De'an Pan ,&nbsp;Guosai Jiang","doi":"10.1016/j.seppur.2026.136793","DOIUrl":"10.1016/j.seppur.2026.136793","url":null,"abstract":"<div><div>Acid sludge, a hazardous waste from lead (Pb) and zinc (Zn) smelting process, commonly contains low-boiling-point elements such as Pb and fluorine (F). However, the complex phase composition of acid sludge typically results in low recovery efficiencies of Pb and F. Herein, we proposed an efficient recovery method for Pb and F through synergistic leaching using a solution containing aluminum ions (Al<sup>3+</sup>) and chloride ions (Cl<sup>−</sup>) followed by stepwise precipitation involving PbCl<sub>2</sub> cooling crystallization and cryolite formation. The single-factor experiment results showed the leaching efficiencies of 98.37% and 92.35% for Pb and F, respectively, which is superior to that of the separate leaching of Pb or F process, due to the intermingle structure of Pb and F phases in acid sludge. The precipitation efficiencies reached 94.44% for Pb and 97.88% for F, and the obtained PbCl<sub>2</sub> and cryolite products meet national standards. Density functional theory (DFT) calculations revealed the chemical states of Al<sup>3+</sup>, calcium ion (Ca<sup>2+</sup>), and F<sup>−</sup> in leaching solution and their coexistence mechanism, and thermodynamic analysis clarified the preferential precipitation of cryolite with high quality. Further, the Life Cycle Assessment (LCA) and economic evaluation were conducted for the entire recovery process, indicating the significantly economic and environmental benefits with a cost of only ¥1.61 for treating 100 g of acid sludge. This study provides an efficient and sustainable method for recovering Pb and F from acid sludge, which not only mitigates environmental hazards but also enhances resource valorization, thereby supporting the development of a circular economy in the non-ferrous metal industry.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"388 ","pages":"Article 136793"},"PeriodicalIF":9.0,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974323","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
期刊
Separation and Purification Technology
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1