Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131722
Qiang Li, Man Deng, Jun Gao, Aoxiang Liu, Xiujuan Tang, Erpeng Wang, Zhiheng Li, Huayue Zhu, Qi Wang
The charge separation of photogenerated carriers in the photo-self-Fenton system still limits its ability to remove organic contaminants. To overcome this limitation, a novel MOF/COF direct Z-scheme-based photo-self-Fenton system (MIL-100(Fe)/TpPa-1 COF, MT2) was designed and synthesized for removing tetracycline hydrochloride (TC) from water. As a result, 91 % of TC (20 mg L−1, 100 mL) was removed by MT2 (0.08 g L−1) within 120 min, driven by improved charge separation and the synergistic effects of h+, OH, and O2–. Theoretical calculations confirmed the improved charge dynamics within the heterojunction, supporting efficient photocatalytic degradation. LC-MS analysis and DFT calculations revealed the potential degradation intermediates and pathways of TC. TC was found to significantly inhibit wheat seedling growth and chlorophyll production, while its intermediates exhibited negligible inhibitory effects. Additionally, the ecotoxicity of TC was significantly reduced, as evidenced by the decreased inhibition zones for Escherichia coli and Staphylococcus aureus. Thus, the in-situ photo-Fenton composite shows great potential for practical applications in antibiotics removal.
{"title":"Rational design of a novel MIL-100(Fe)/TpPa-1 COF direct Z-scheme heterojunction for photo-self-Fenton removal of antibiotics: Performance and ecotoxicity assessment","authors":"Qiang Li, Man Deng, Jun Gao, Aoxiang Liu, Xiujuan Tang, Erpeng Wang, Zhiheng Li, Huayue Zhu, Qi Wang","doi":"10.1016/j.seppur.2025.131722","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131722","url":null,"abstract":"The charge separation of photogenerated carriers in the photo-self-Fenton system still limits its ability to remove organic contaminants. To overcome this limitation, a novel MOF/COF direct Z-scheme-based photo-self-Fenton system (MIL-100(Fe)/TpPa-1 COF, MT2) was designed and synthesized for removing tetracycline hydrochloride (TC) from water. As a result, 91 % of TC (20 mg L<sup>−1</sup>, 100 mL) was removed by MT2 (0.08 g L<sup>−1</sup>) within 120 min, driven by improved charge separation and the synergistic effects of h<sup>+</sup>, <sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup>OH, and <sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup>O<sub>2</sub><sup>–</sup>. Theoretical calculations confirmed the improved charge dynamics within the heterojunction, supporting efficient photocatalytic degradation. LC-MS analysis and DFT calculations revealed the potential degradation intermediates and pathways of TC. TC was found to significantly inhibit wheat seedling growth and chlorophyll production, while its intermediates exhibited negligible inhibitory effects. Additionally, the ecotoxicity of TC was significantly reduced, as evidenced by the decreased inhibition zones for <em>Escherichia coli</em> and <em>Staphylococcus aureus</em>. Thus, the in-situ photo-Fenton composite shows great potential for practical applications in antibiotics removal.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"31 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989967","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131714
Jie Yang, Hui Zhou, Yu Luo, Yangliu Cheng, Shan Wang, Lu Yao, Yidong Wan, Junjiang Zhu
The addition of Ce to V − Ti based catalysts is a promising way to improve the middle and low temperature activity for selective catalytic reduction of NO with NH3 (NH3 − SCR). In this study, a series of V − Ce loaded TiO2 catalysts were prepared by impregnation method and studied by in situ spectroscopy experiments and ex situ characterizations. Results show that the SCR reaction on the surface of V − Ce/TiO2 catalysts obeys the Eley − Rideal mechanism. The presence of Ce in V − Ce/TiO2 catalysts strengthens the NH3 adsorption energy of V and promotes its rupture of N − H bond, thus facilitating the reactions, with 100 % NO conversion and 100 % N2 selectivity obtained at 250 °C over 2 V-10Ce/Ti. During the reaction, the Ce4+ ions are reduced by NH3 + NO to yield N2 and Ce3+ ions (the reduction half cycle), which will then be re-oxidized to Ce4+ ions by O2 (the oxidation half cycle), thereby ensuring the proceeding of the overall reaction.
{"title":"Insight into the promotion effects of Ce on the performances of V − Ti based catalyst for low-temperature NH3 − SCR: In-situ spectroscopy studies","authors":"Jie Yang, Hui Zhou, Yu Luo, Yangliu Cheng, Shan Wang, Lu Yao, Yidong Wan, Junjiang Zhu","doi":"10.1016/j.seppur.2025.131714","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131714","url":null,"abstract":"The addition of Ce to V − Ti based catalysts is a promising way to improve the middle and low temperature activity for selective catalytic reduction of NO with NH<sub>3</sub> (NH<sub>3</sub> − SCR). In this study, a series of V − Ce loaded TiO<sub>2</sub> catalysts were prepared by impregnation method and studied by <em>in situ</em> spectroscopy experiments and <em>ex situ</em> characterizations. Results show that the SCR reaction on the surface of V − Ce/TiO<sub>2</sub> catalysts obeys the Eley − Rideal mechanism. The presence of Ce in V − Ce/TiO<sub>2</sub> catalysts strengthens the NH<sub>3</sub> adsorption energy of V and promotes its rupture of N − H bond, thus facilitating the reactions, with 100 % NO conversion and 100 % N<sub>2</sub> selectivity obtained at 250 °C over 2 V-10Ce/Ti. During the reaction, the Ce<sup>4+</sup> ions are reduced by NH<sub>3</sub> + NO to yield N<sub>2</sub> and Ce<sup>3+</sup> ions (the reduction half cycle), which will then be re-oxidized to Ce<sup>4+</sup> ions by O<sub>2</sub> (the oxidation half cycle), thereby ensuring the proceeding of the overall reaction.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989964","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131716
Yong Yan, Yongli Lv, Yuhai Sun, Min Chen, Dan Zhou, Lei Sun, Hai-bin Cheng, Wei-jia Li, Zhi Chen, Cong-Ming Tang, Li Chang, Jun-Qiang Xu
In the recycling of spent lithium batteries, priority lithium extraction is receiving extensive attention because of its prospects and development difficulties. This paper presents a simple, green, and efficient scheme for lithium extraction. In this process, oxidation is the main driving force, and pressure action and ion exchange assist in effectively achieving selective lithium recovery. The experimental results showed that a reasonable configuration of multiple driving forces caused a partial phase transition (cracks appearing) in the layered structure, which ultimately achieved 95.98 % lithium recovery and 94.69 % selectivity. Notably, the lithium-rich leach solution was nearly neutral, and the residue composition was nearly the same as that obtained after cathode charging. Combined with the corresponding characterization results, a mechanism of multiple driving forces for selective lithium extraction is proposed, which will provide a reference for subsequent metal selective recovery.
{"title":"Green and efficient selective lithium extraction from spent lithium-ion batteries using a self-pressurizing-assisted oxidative fixation system","authors":"Yong Yan, Yongli Lv, Yuhai Sun, Min Chen, Dan Zhou, Lei Sun, Hai-bin Cheng, Wei-jia Li, Zhi Chen, Cong-Ming Tang, Li Chang, Jun-Qiang Xu","doi":"10.1016/j.seppur.2025.131716","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131716","url":null,"abstract":"In the recycling of spent lithium batteries, priority lithium extraction is receiving extensive attention because of its prospects and development difficulties. This paper presents a simple, green, and efficient scheme for lithium extraction. In this process, oxidation is the main driving force, and pressure action and ion exchange assist in effectively achieving selective lithium recovery. The experimental results showed that a reasonable configuration of multiple driving forces caused a partial phase transition (cracks appearing) in the layered structure, which ultimately achieved 95.98 % lithium recovery and 94.69 % selectivity. Notably, the lithium-rich leach solution was nearly neutral, and the residue composition was nearly the same as that obtained after cathode charging. Combined with the corresponding characterization results, a mechanism of multiple driving forces for selective lithium extraction is proposed, which will provide a reference for subsequent metal selective recovery.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"107 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991046","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}
The extraction of rare earth elements (REEs) via chemical leaching from ion-adsorption type rare earth ores has led to serious ecological and environmental risks. Organic acid leaching agents possessed advantages in environmental friendliness and differential leaching capabilities. This study investigated the leaching behaviors of REEs from ion-adsorption type rare earth ores using organic acids and focused on the differential leaching properties of light rare earth elements and heavy rare earth elements. The leaching conditions using acetic acid, malic acid, and citric acid were optimized, and the influences of organic acid on mineral properties and soil ecological functions were elaborated. The experimental results indicated that acetic acid, malic acid, and citric acid had unique REEs differential leaching properties, without significantly altering the mineral structure. The leaching efficiency of full-phase, and colloidal sediment phase REEs reached 49.75%, and 28.03% for acetic acid, 52.07%, and 26.65% for malic acid, 51.79%, and 33.07% for citric acid, respectively. Furthermore, the patterns of the soil enzyme activity also confirmed the perspective that the soil ecology had not been affected obviously by the organic acids leaching process and rapidly recovered after leaching. Subsequently, Visual Minteq simulation and Density Functional Theory calculations indicated the differential leaching mechanism of light and heavy rare earths depended on the differences in complexation effects of organic acid, and the leaching of colloidal sediment phase REEs was the result of combined effects of acid leaching and complexation competition. The work provided molecular-level insights into the colloidal sediment phase REEs leaching and differential leaching mechanisms of light and heavy rare earths by organic acids, contributing to the understanding of REEs extraction processes.
{"title":"Differential leaching mechanisms and ecological impact of organic acids on ion-adsorption type rare earth ores","authors":"Mengfei Zhao, Hualin Zhang, Hexing Han, Xiaoliang Jiang, Youming Yang, Tinggang Li","doi":"10.1016/j.seppur.2025.131701","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131701","url":null,"abstract":"The extraction of rare earth elements (REEs) via chemical leaching from ion-adsorption type rare earth ores has led to serious ecological and environmental risks. Organic acid leaching agents possessed advantages in environmental friendliness and differential leaching capabilities. This study investigated the leaching behaviors of REEs from ion-adsorption type rare earth ores using organic acids and focused on the differential leaching properties of light rare earth elements and heavy rare earth elements. The leaching conditions using acetic acid, malic acid, and citric acid were optimized, and the influences of organic acid on mineral properties and soil ecological functions were elaborated. The experimental results indicated that acetic acid, malic acid, and citric acid had unique REEs differential leaching properties, without significantly altering the mineral structure. The leaching efficiency of full-phase, and colloidal sediment phase REEs reached 49.75%, and 28.03% for acetic acid, 52.07%, and 26.65% for malic acid, 51.79%, and 33.07% for citric acid, respectively. Furthermore, the patterns of the soil enzyme activity also confirmed the perspective that the soil ecology had not been affected obviously by the organic acids leaching process and rapidly recovered after leaching. Subsequently, Visual Minteq simulation and Density Functional Theory calculations indicated the differential leaching mechanism of light and heavy rare earths depended on the differences in complexation effects of organic acid, and the leaching of colloidal sediment phase REEs was the result of combined effects of acid leaching and complexation competition. The work provided molecular-level insights into the colloidal sediment phase REEs leaching and differential leaching mechanisms of light and heavy rare earths by organic acids, contributing to the understanding of REEs extraction processes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"24 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991047","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131618
Dongsheng Zhao, Jiyu Song, Ruohan Liang, Junxia Liu, Jun Xu, Guicai Liu, Xiaohang Ma, Zonghua Wang, Kang Xie
The low permeability and high fouling susceptibility of nanofiltration (NF) membranes limit their widespread application in water treatment. In this study, a polyethylenimine (PEI)-based NF membrane was synthesized via interfacial polymerization with a mixture of PEI and the polyethylene glycol derivative Jeffamine (JA) as the aqueous phase comonomer and trimesoyl chloride as the organic phase monomer. A 1/1 mass ratio of PEI to JA with a total aqueous phase monomer concentration of 1.00 % (weight/volume) yielded NF membranes with optimal water permeance and satisfactory salt exclusion. Compared with the pristine membrane, the JA-doped PEI-based (JA/PEI) membrane exhibited enhanced surface hydrophilicity, a more positively charged surface, an enlarged effective pore size, a thinner polyamide layer, and greater surface roughness. Furthermore, the optimal JA/PEI membrane was more resistant to protein fouling because of the lower adhesion energy between it and protein molecules. Additionally, the optimal JA/PEI membrane exhibited excellent permeation flux and comparable retention performance in the treatment of actual drinking water. This JA-doping strategy provides a facile avenue to fabricate NF membranes with higher permeability and better antifouling ability for water treatment applications.
{"title":"Enhancing the filtration performance and antifouling ability of polyethylenimine-based nanofiltration membranes by doping with polyethylene glycol derivatives","authors":"Dongsheng Zhao, Jiyu Song, Ruohan Liang, Junxia Liu, Jun Xu, Guicai Liu, Xiaohang Ma, Zonghua Wang, Kang Xie","doi":"10.1016/j.seppur.2025.131618","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131618","url":null,"abstract":"The low permeability and high fouling susceptibility of nanofiltration (NF) membranes limit their widespread application in water treatment. In this study, a polyethylenimine (PEI)-based NF membrane was synthesized via interfacial polymerization with a mixture of PEI and the polyethylene glycol derivative Jeffamine (JA) as the aqueous phase comonomer and trimesoyl chloride as the organic phase monomer. A 1/1 mass ratio of PEI to JA with a total aqueous phase monomer concentration of 1.00 % (weight/volume) yielded NF membranes with optimal water permeance and satisfactory salt exclusion. Compared with the pristine membrane, the JA-doped PEI-based (JA/PEI) membrane exhibited enhanced surface hydrophilicity, a more positively charged surface, an enlarged effective pore size, a thinner polyamide layer, and greater surface roughness. Furthermore, the optimal JA/PEI membrane was more resistant to protein fouling because of the lower adhesion energy between it and protein molecules. Additionally, the optimal JA/PEI membrane exhibited excellent permeation flux and comparable retention performance in the treatment of actual drinking water. This JA-doping strategy provides a facile avenue to fabricate NF membranes with higher permeability and better antifouling ability for water treatment applications.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"7 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989909","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}
As an important group of endocrine disrupting compounds, most steroid estrogens (SEs) found in environmental water have adverse health effects on aquatic organisms and humans. Sensitive detection of these SEs is crucial for protecting human health and ecosystem safety. Herein, a novel heterogeneous MOF-on-MOF membrane (ESM@His-ZIF-90@ZIF-8) was rationally designed by sequentially growing histidine-modified ZIF-90 and ZIF-8 on natural eggshell membrane (ESM), and employed as an efficient adsorbent for dispersive membrane extraction (DME) of three SEs from environmental water. Due to the multiple adsorption sites provided by His-ZIF-90@ZIF-8 and the rapid separation of ESM from solution, the ESM@His-ZIF-90@ZIF-8 exhibited extraordinary extraction efficiency towards three SEs. The adsorption behavior of the three SEs on ESM@His-ZIF-90@ZIF-8 followed Langmuir isotherm and pseudo-second-order kinetic models. Notably, the ESM@His-ZIF-90@ZIF-8 showed fast adsorption kinetics with adsorption equilibrium of only 10 min. FT-IR, XPS and DFT calculation revealed that the rapid adsorption was attributed to the synergy of π-π stacking, hydrophobic and hydrogen bonding interactions. Additionally, the ESM@His-ZIF-90@ZIF-8 showed excellent reusability and the extraction efficiency remained above 90 % after 20 cycles of reuse. Under optimal conditions, ESM@His-ZIF-90@ZIF-8 based DME coupled with HPLC-UV offered good linearity (R2 ≥ 0.9941) and low limits of detection of 0.30–0.45 μg L-1. The method recoveries ranged from 85.0-102 % with RSDs lower than 7.2 %. This study highlighted the promising application of heterogeneous MOF-on-MOF composites in the field of sample pretreatment.
{"title":"Rational design and synthesis of heterogeneous MOF-on-MOF on natural eggshell membrane for highly efficient extraction of trace steroid estrogens in environmental water","authors":"Wei Zhou, Liangtao Xu, Ruxue Chen, Xin Wang, Youping Liu, Xin Di","doi":"10.1016/j.seppur.2025.131705","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131705","url":null,"abstract":"As an important group of endocrine disrupting compounds, most steroid estrogens (SEs) found in environmental water have adverse health effects on aquatic organisms and humans. Sensitive detection of these SEs is crucial for protecting human health and ecosystem safety. Herein, a novel heterogeneous MOF-on-MOF membrane (ESM@His-ZIF-90@ZIF-8) was rationally designed by sequentially growing histidine-modified ZIF-90 and ZIF-8 on natural eggshell membrane (ESM), and employed as an efficient adsorbent for dispersive membrane extraction (DME) of three SEs from environmental water. Due to the multiple adsorption sites provided by His-ZIF-90@ZIF-8 and the rapid separation of ESM from solution, the ESM@His-ZIF-90@ZIF-8 exhibited extraordinary extraction efficiency towards three SEs. The adsorption behavior of the three SEs on ESM@His-ZIF-90@ZIF-8 followed Langmuir isotherm and pseudo-second-order kinetic models. Notably, the ESM@His-ZIF-90@ZIF-8 showed fast adsorption kinetics with adsorption equilibrium of only 10 min. FT-IR, XPS and DFT calculation revealed that the rapid adsorption was attributed to the synergy of π-π stacking, hydrophobic and hydrogen bonding interactions. Additionally, the ESM@His-ZIF-90@ZIF-8 showed excellent reusability and the extraction efficiency remained above 90 % after 20 cycles of reuse. Under optimal conditions, ESM@His-ZIF-90@ZIF-8 based DME coupled with HPLC-UV offered good linearity (R<sup>2</sup> ≥ 0.9941) and low limits of detection of 0.30–0.45 μg L<sup>-1</sup>. The method recoveries ranged from 85.0-102 % with RSDs lower than 7.2 %. This study highlighted the promising application of heterogeneous MOF-on-MOF composites in the field of sample pretreatment.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989958","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131709
Ying Tian, Changqing He, Lin He, Hong Sui, Xingang Li
The low recovery rate of petroleum and the inevitable formation of large quantities of oil–water emulsions limit the efficiency of petroleum production, transportation, and storage. To enhance demulsification efficiency, four nonionic interfacial regulators (PA-1, PA-2, PAMA-1, and PAMA-2) were developed by incorporating oxygen atoms into a polyether substrate via esterification and polymerization reactions. Additionally, PAMA-1 and PAMA-2 were further modified with sulfonyl groups. Experimental results demonstrated that all regulators exhibited high-efficiency cleaning and demulsification performance at 25 °C. These regulators achieved 100 % oil removal from mineral and metal surfaces without causing damage. Furthermore, they could effectively break various water-in-oil (W/O) emulsions. It is also found that over 95.33 % demulsification could be achieved at 20 °C in 15 mins when PAMA-1 (600 mg/L) is added into asphaltene-stabilized emulsion and complete dehydration (100 %) within 40 mins. These interfacial regulators possess high interfacial activity and are rich in polar groups (–COOR, –OH, O = S = O, –C–O–C–). Mechanistic studies revealed that the heteroatomic groups introduced into the regulators serve as active sites for noncovalent interactions, forming hydrogen bonds with natural interfacially active substances (e.g., asphaltenes) and water molecules. This promotes oil dispersion on solid surfaces and disrupts the oil–water interfacial film, improving cleaning and demulsification efficiency. Importantly, pre-treatment with these interfacial regulators effectively prevents emulsion formation. These regulators hold significant potential for applications in oil–water and oil–solid separation processes during petroleum exploitation.
石油采收率低，不可避免地形成大量油水乳状体，限制了石油生产、运输和储存的效率。为了提高破乳效率，通过酯化和聚合反应将氧原子掺入聚醚底物中，制备了4种非离子界面调节剂（PA-1、PA-2、PAMA-1和PAMA-2）。此外，PAMA-1和PAMA-2进一步用磺酰基修饰。实验结果表明，在25 °C下，所有调节剂都具有高效的清洗和破乳性能。这些调节剂在不造成损害的情况下，从矿物和金属表面去除100% %的油。此外，它们还能有效地破坏各种油包水（W/O）乳液。在沥青质稳定乳状液中加入600 mg/L的PAMA-1，在20 ℃条件下，15 min破乳率可达95.33 %以上，40 min内完全脱水（100 %）。这些界面调节剂具有高的界面活性，并且富含极性基团（- coor, - oh, O = S = O, - c - O - c -）。机理研究表明，引入调控剂的杂原子基团作为非共价相互作用的活性位点，与天然界面活性物质（如沥青质）和水分子形成氢键。这促进了油在固体表面的分散，破坏了油水界面膜，提高了清洁和破乳效率。重要的是，用这些界面调节剂进行预处理可以有效地防止乳液的形成。这些调节剂在石油开采过程中的油水和油固分离过程中具有重要的应用潜力。
{"title":"Enhancing interfacial regulation by S/O co-doping for effective oil–solid and oil–water separation at room temperature","authors":"Ying Tian, Changqing He, Lin He, Hong Sui, Xingang Li","doi":"10.1016/j.seppur.2025.131709","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131709","url":null,"abstract":"The low recovery rate of petroleum and the inevitable formation of large quantities of oil–water emulsions limit the efficiency of petroleum production, transportation, and storage. To enhance demulsification efficiency, four nonionic interfacial regulators (PA-1, PA-2, PAMA-1, and PAMA-2) were developed by incorporating oxygen atoms into a polyether substrate via esterification and polymerization reactions. Additionally, PAMA-1 and PAMA-2 were further modified with sulfonyl groups. Experimental results demonstrated that all regulators exhibited high-efficiency cleaning and demulsification performance at 25 °C. These regulators achieved 100 % oil removal from mineral and metal surfaces without causing damage. Furthermore, they could effectively break various water-in-oil (W/O) emulsions. It is also found that over 95.33 % demulsification could be achieved at 20 °C in 15 mins when PAMA-1 (600 mg/L) is added into asphaltene-stabilized emulsion and complete dehydration (100 %) within 40 mins. These interfacial regulators possess high interfacial activity and are rich in polar groups (–COOR, –OH, O = S = O, –C–O–C–). Mechanistic studies revealed that the heteroatomic groups introduced into the regulators serve as active sites for noncovalent interactions, forming hydrogen bonds with natural interfacially active substances (e.g., asphaltenes) and water molecules. This promotes oil dispersion on solid surfaces and disrupts the oil–water interfacial film, improving cleaning and demulsification efficiency. Importantly, pre-treatment with these interfacial regulators effectively prevents emulsion formation. These regulators hold significant potential for applications in oil–water and oil–solid separation processes during petroleum exploitation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"6 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989961","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131700
Ruixue Deng, Zhaonian Ren, Tingting Tang, Xinsheng Wang, Pu Liu
The extraction technology of total triterpenoid saponins from ornamental and medicinal plant Lysimachia christinae was optimized by ultrasonic-assisted extraction (UAE) method. The triterpenoid saponins compounds in the extraction were isolated and separated by repeated column chromatography, the structure of the isolated compounds was elucidated on the base of spectroscopic analysis (NMR, HR-ESI-MS, IR) and chemical methods, and the cytotoxicity of the isolated compounds against cancer cells were also evaluated. The results revealed that the optimal extraction conditions for triterpenoid saponins from L. christinae were optimized as liquid-to-solid ratio of 32 mL/g, extraction time of 40 min, extraction temperature of 50 °C, and ethanol concentration of 66 %, with the extraction yield of 17.32 %. Four undescribed oleanane-type triterpenoid saponins (1–4), named Lysichriside C-F, along with four known oleanane-type triterpenoid saponins (5–8) were isolated from the extraction of L. christinae. Compounds 1–3 and 6–7 had the structure type of 13β, 28-epoxy (type I), and compounds 4 and 8 had the structure type of Δ12 −17-CH2OH (type II). All the isolated compounds had high toxicity against cancer cell lines in vitro, compounds 3, 5 and 6 revealed significant inhibition against the cancer cell lines tested than other compounds, and with the IC50 values of 2.9–12.3, 1.9–15.7 and 1.8–12.6 μM, respectively. The studies revealed that oleanane-derived sapogenols with the structure of 13β, 28-epoxy and Δ 12 –17-CH2OH were the main two structural types of L. christinae, and the triterpenoid saponins in L. christinae had important research and development value.
{"title":"Extraction, isolation and cytotoxic activities of triterpene saponins from ornamental and medicinal plant Lysimachia christinae","authors":"Ruixue Deng, Zhaonian Ren, Tingting Tang, Xinsheng Wang, Pu Liu","doi":"10.1016/j.seppur.2025.131700","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131700","url":null,"abstract":"The extraction technology of total triterpenoid saponins from ornamental and medicinal plant <em>Lysimachia christinae</em> was optimized by ultrasonic-assisted extraction (UAE) method. The triterpenoid saponins compounds in the extraction were isolated and separated by repeated column chromatography, the structure of the isolated compounds was elucidated on the base of spectroscopic analysis (NMR, HR-ESI-MS, IR) and chemical methods, and the cytotoxicity of the isolated compounds against cancer cells were also evaluated. The results revealed that the optimal extraction conditions for triterpenoid saponins from <em>L. christinae</em> were optimized as liquid-to-solid ratio of 32 mL/g, extraction time of 40 min, extraction temperature of 50 °C, and ethanol concentration of 66 %, with the extraction yield of 17.32 %. Four undescribed oleanane-type triterpenoid saponins (<strong>1</strong>–<strong>4</strong>), named Lysichriside C-F, along with four known oleanane-type triterpenoid saponins (<strong>5</strong>–<strong>8</strong>) were isolated from the extraction of <em>L. christinae</em>. Compounds <strong>1</strong>–<strong>3</strong> and <strong>6</strong>–<strong>7</strong> had the structure type of 13β, 28-epoxy (type <strong>I</strong>), and compounds <strong>4</strong> and <strong>8</strong> had the structure type of Δ<sup>12</sup> −17-CH<sub>2</sub>OH (type <strong>II</strong>). All the isolated compounds had high toxicity against cancer cell lines <em>in vitro</em>, compounds <strong>3</strong>, <strong>5</strong> and <strong>6</strong> revealed significant inhibition against the cancer cell lines tested than other compounds, and with the IC<sub>50</sub> values of 2.9–12.3, 1.9–15.7 and 1.8–12.6 μM, respectively. The studies revealed that oleanane-derived sapogenols with the structure of 13β, 28-epoxy and Δ <sup>12</sup> –17-CH<sub>2</sub>OH were the main two structural types of <em>L. christinae</em>, and the triterpenoid saponins in <em>L. christinae</em> had important research and development value.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"70 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989965","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131636
Shuliang Chen, Yuxin Yang, Futing Zi, Xianzhi Hu, Xinrong Li
The high capacity and selective recovery of gold(I) thiosulfate complex are the greatest obstacles hindering the rapid development of thiosulfate gold leaching technology. In this study, a batch of adsorbents for gold ion recovery from thiosulfate solutions were synthesized by functionalizing polystyrene cross-linked microspheres (PCMS) via nucleophilic substitution reactions using organic phosphines(III) with different carbon number as functional monomers. Increasing the pH of the adsorption solution or reducing the carbon number of the functional monomer in the adsorbent were found to enhance the gold ion adsorption performance of the adsorbent. The adsorbent (PCMS-TMP) obtained from the reaction of trimethylphosphine and PCMS exhibited the best gold adsorption performance, achieving a gold loading capacity of 136.42 mg/g. It also demonstrated selective recovery of low-concentration gold ions (6.175 mg/L), with a recovery rate as high as 98 %. The adsorption process of gold ions on PCMS-TMP was accurately described by the Langmuir isotherm and pseudo-second-order kinetic model. The gold adsorption process on PCMS-TMP primarily involved an anion exchange between Cl- and Au(S2O3)23-, which was also theoretically validated through density functional theory calculations. Clearly, PCMS-TMP is an adsorbent with significant capacity and selective recovery capabilities for Au(I) from thiosulfate solutions.
{"title":"Constructing phosphine-containing microspheres for selective recovery of gold(I) thiosulfate complex by adjusting the interaction site","authors":"Shuliang Chen, Yuxin Yang, Futing Zi, Xianzhi Hu, Xinrong Li","doi":"10.1016/j.seppur.2025.131636","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131636","url":null,"abstract":"The high capacity and selective recovery of gold(I) thiosulfate complex are the greatest obstacles hindering the rapid development of thiosulfate gold leaching technology. In this study, a batch of adsorbents for gold ion recovery from thiosulfate solutions were synthesized by functionalizing polystyrene cross-linked microspheres (PCMS) via nucleophilic substitution reactions using organic phosphines(III) with different carbon number as functional monomers. Increasing the pH of the adsorption solution or reducing the carbon number of the functional monomer in the adsorbent were found to enhance the gold ion adsorption performance of the adsorbent. The adsorbent (PCMS-TMP) obtained from the reaction of trimethylphosphine and PCMS exhibited the best gold adsorption performance, achieving a gold loading capacity of 136.42 mg/g. It also demonstrated selective recovery of low-concentration gold ions (6.175 mg/L), with a recovery rate as high as 98 %. The adsorption process of gold ions on PCMS-TMP was accurately described by the Langmuir isotherm and pseudo-second-order kinetic model. The gold adsorption process on PCMS-TMP primarily involved an anion exchange between Cl<sup>-</sup> and Au(S<sub>2</sub>O<sub>3</sub>)<sub>2</sub><sup>3-</sup>, which was also theoretically validated through density functional theory calculations. Clearly, PCMS-TMP is an adsorbent with significant capacity and selective recovery capabilities for Au(I) from thiosulfate solutions.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"31 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991044","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}
Pub Date : 2025-01-20DOI: 10.1016/j.seppur.2025.131710
Haoyan Li, Sohrab Rohani, Minyu He, Xi Jin, Chunlian Ding, Dong Wang, Weizao Liu
With the rapid development of new energy industry, the quantity of spent lithium-ion batteries (LIBs) is increasing accordingly. From the environmental protection and resource recovery standpoints, it is crucial to recover valuable metals from spent LIBs. In this study, an efficient and integrated process was proposed to extract the valuable metals from spent LIBs with inexpensive Fe2(SO4)3 as a reagent. The effects of various process parameters including the mass ratio of Fe2(SO4)3 to the cathode material (F/C), roasting temperature, and roasting time on the leaching efficiencies were investigated. The leaching efficiency of Li was approximately 100 %, and that of cobalt reached 96 %, while the iron was hardly leached under the optimal conditions. The reaction mechanism of sulfation roasting process was studied through thermodynamic behavior, phase transformation as well as valence state transition. When roasting at a low temperature (＜600 °C), the ion-exchange reaction dominated, which converted lithium into its soluble sulfate prior to cobalt. With increased temperature (600–700 °C), Fe2(SO4)3 decomposed and generated SO2, promoting the sulfation reaction through gas–solid interaction, and thus increasing the leaching efficiency of Li and Co. Once the temperature reached 800 °C, CoSO4 decomposed and the resulting cobalt oxide reacted with Fe2O3 to create a spinel phase CoFe2O4, which is very difficult to dissolve, will reduce the recovery of cobalt. Furthermore, the recovery of Li and Co from the filtrate using H2C2O4 and Na2CO3 was investigated, where the recovery efficiency of Co and Li from the filtrate reached 94 % and 88 %, respectively. The findings demonstrated that it is possible to recover valuable metals from the cathode materials of spent LiCoO2 batteries through the sulfation roasting-water leaching process followed by stepwise precipitation.
{"title":"An integrated process for recycling spent LiCoO2 cathode materials via sulfate roasting and stepwise precipitation","authors":"Haoyan Li, Sohrab Rohani, Minyu He, Xi Jin, Chunlian Ding, Dong Wang, Weizao Liu","doi":"10.1016/j.seppur.2025.131710","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131710","url":null,"abstract":"With the rapid development of new energy industry, the quantity of spent lithium-ion batteries (LIBs) is increasing accordingly. From the environmental protection and resource recovery standpoints, it is crucial to recover valuable metals from spent LIBs. In this study, an efficient and integrated process was proposed to extract the valuable metals from spent LIBs with inexpensive Fe<sub>2</sub>(SO<sub>4</sub>)<sub>3</sub> as a reagent. The effects of various process parameters including the mass ratio of Fe<sub>2</sub>(SO<sub>4</sub>)<sub>3</sub> to the cathode material (F/C), roasting temperature, and roasting time on the leaching efficiencies were investigated. The leaching efficiency of Li was approximately 100 %, and that of cobalt reached 96 %, while the iron was hardly leached under the optimal conditions. The reaction mechanism of sulfation roasting process was studied through thermodynamic behavior, phase transformation as well as valence state transition. When roasting at a low temperature (＜600 °C), the ion-exchange reaction dominated, which converted lithium into its soluble sulfate prior to cobalt. With increased temperature (600–700 °C), Fe<sub>2</sub>(SO<sub>4</sub>)<sub>3</sub> decomposed and generated SO<sub>2</sub>, promoting the sulfation reaction through gas–solid interaction, and thus increasing the leaching efficiency of Li and Co. Once the temperature reached 800 °C, CoSO<sub>4</sub> decomposed and the resulting cobalt oxide reacted with Fe<sub>2</sub>O<sub>3</sub> to create a spinel phase CoFe<sub>2</sub>O<sub>4</sub>, which is very difficult to dissolve, will reduce the recovery of cobalt. Furthermore, the recovery of Li and Co from the filtrate using H<sub>2</sub>C<sub>2</sub>O<sub>4</sub> and Na<sub>2</sub>CO<sub>3</sub> was investigated, where the recovery efficiency of Co and Li from the filtrate reached 94 % and 88 %, respectively. The findings demonstrated that it is possible to recover valuable metals from the cathode materials of spent LiCoO<sub>2</sub> batteries through the sulfation roasting-water leaching process followed by stepwise precipitation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"78 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989963","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}
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