Pub Date : 2025-02-25DOI: 10.1016/j.seppur.2025.132283
Liang Zhu, Zhiqiang Chen, Qinxue Wen, Xia Huang
Unstable nitrite supply and low ammonia concentration limited the application of mainstream Anammox. In this study, sulfur-based autotrophic denitrification coupled Anammox system (SADA) was established with pyrite and sulfur as electron donors, respectively, to simultaneously remove NH4+-N and NO3–-N. More than 85 % of the total inorganic nitrogen removal efficiency was achieved with S0 as the electron donor. The synergistic nitrogen removal of autotrophic denitrification and Anammox reduced SO42− production. The average NH4+-N removal efficiency reached 94.73 % when pyrite was used as the electron donor, but the NO3–-N concentration in the effluent was higher than that in the influent. Microorganisms associated with nitrogen cycle were significantly enriched at the bottom of both reactors, where major biochemical processes occurred. Batch tests showed the coexistence of multiple N metabolic pathways in SADA, including Anammox, autotrophic denitrification, Sulfammox and Feammox. The genus Thiobacillus, Ferritrophicum, Candidatus_Brocadia, Ignavibacterium and Thermoanaerobaculum played major roles in nitrogen removal.
{"title":"Simultaneous removal of NH4+ and NO3– by coupling sulfur-based autotrophic denitrification and ANAMMOX with different electron donors","authors":"Liang Zhu, Zhiqiang Chen, Qinxue Wen, Xia Huang","doi":"10.1016/j.seppur.2025.132283","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132283","url":null,"abstract":"Unstable nitrite supply and low ammonia concentration limited the application of mainstream Anammox. In this study, sulfur-based autotrophic denitrification coupled Anammox system (SADA) was established with pyrite and sulfur as electron donors, respectively, to simultaneously remove NH<sub>4</sub><sup>+</sup>-N and NO<sub>3</sub><sup>–</sup>-N. More than 85 % of the total inorganic nitrogen removal efficiency was achieved with S<sup>0</sup> as the electron donor. The synergistic nitrogen removal of autotrophic denitrification and Anammox reduced SO<sub>4</sub><sup>2−</sup> production. The average NH<sub>4</sub><sup>+</sup>-N removal efficiency reached 94.73 % when pyrite was used as the electron donor, but the NO<sub>3</sub><sup>–</sup>-N concentration in the effluent was higher than that in the influent. Microorganisms associated with nitrogen cycle were significantly enriched at the bottom of both reactors, where major biochemical processes occurred. Batch tests showed the coexistence of multiple N metabolic pathways in SADA, including Anammox, autotrophic denitrification, Sulfammox and Feammox. The genus <em>Thiobacillus</em>, <em>Ferritrophicum</em>, <em>Candidatus_Brocadia</em>, <em>Ignavibacterium</em> and <em>Thermoanaerobaculum</em> played major roles in nitrogen removal.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"98 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485807","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132234
Haoyuan Deng, Ben Wang, Junqing Xu, Guoying Yang, Zhiang Shi, Haochen Zhu, Wenzhi He, Guangming Li
Some studies have reviewed the different waste lithium-ion batteries (LIBs) recycling methodologies by hydrometallurgy, but whole process was not discussed comprehensively, especially few compared analysis of some typical technologies which are commonly used in commercial production. This paper presents a review on the typical approaches for recycling critical materials from waste LIBs by hydrometallurgy. The whole recovery process is divided into pretreatment, leaching, purification and regeneration. For pretreatment, discharge and materials separation are mainly discussed, which is important for granting the safety and efficiency of subsequent steps. Concerning leaching, inorganic acid leaching, organic acid leaching and alkali leaching are showed, in which the most widely used is inorganic acid leaching, it can extract metallic elements efficiently with reductants cooperation or electrochemical and acid gas assisted leaching. As to purification, it is performed by solvent extraction, chemical precipitation and ion exchange, these three methods are broadly used and quite mature in practical industrial production. As for regeneration, it is related to the quality of reborn products, the sol–gel and co-precipitation have representational significance during battery materials reproduced. The analysis of arguments including technical effect, economical cost and environmental impact are revealed by comparing different technologies. The challenges and perspectives are also proposed to further perfect the available hydrometallurgical technologies. The purpose of this review is to demonstrate the latest research advances of hydrometallurgical process and provide scientific references for techniques-choosing in commercial production, which is helpful to select green, efficient and economic recycling processes during industrial production of waste LIBs recycling.
{"title":"A comprehensive review of whole process typical hydrometallurgical technologies for recycling waste lithium-ion batteries","authors":"Haoyuan Deng, Ben Wang, Junqing Xu, Guoying Yang, Zhiang Shi, Haochen Zhu, Wenzhi He, Guangming Li","doi":"10.1016/j.seppur.2025.132234","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132234","url":null,"abstract":"Some studies have reviewed the different waste lithium-ion batteries (LIBs) recycling methodologies by hydrometallurgy, but whole process was not discussed comprehensively, especially few compared analysis of some typical technologies which are commonly used in commercial production. This paper presents a review on the typical approaches for recycling critical materials from waste LIBs by hydrometallurgy. The whole recovery process is divided into pretreatment, leaching, purification and regeneration. For pretreatment, discharge and materials separation are mainly discussed, which is important for granting the safety and efficiency of subsequent steps. Concerning leaching, inorganic acid leaching, organic acid leaching and alkali leaching are showed, in which the most widely used is inorganic acid leaching, it can extract metallic elements efficiently with reductants cooperation or electrochemical and acid gas assisted leaching. As to purification, it is performed by solvent extraction, chemical precipitation and ion exchange, these three methods are broadly used and quite mature in practical industrial production. As for regeneration, it is related to the quality of reborn products, the sol–gel and co-precipitation have representational significance during battery materials reproduced. The analysis of arguments including technical effect, economical cost and environmental impact are revealed by comparing different technologies. The challenges and perspectives are also proposed to further perfect the available hydrometallurgical technologies. The purpose of this review is to demonstrate the latest research advances of hydrometallurgical process and provide scientific references for techniques-choosing in commercial production, which is helpful to select green, efficient and economic recycling processes during industrial production of waste LIBs recycling.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"18 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485808","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 : 2025-02-24DOI: 10.1016/j.seppur.2025.132268
Lu Xiao, Jiahao Mo, Yang Yang, Xianhui Li
Membrane distillation (MD) provides an effective solution for hypersaline wastewater treatment. However, its widespread industrial application is hindered by surfactant-induced wetting that leads to a decline in membrane performance. Removing surfactants through water flushing has emerged as a practicable strategy for wetting restoration. Nevertheless, the uneven distribution of temperature along the membrane axis can affect the uniformity of wetting, which may in turn influence the overall recovery of membrane wetting. To address this issue, this work studied the impact of non-uniform wetting on wetting restoration realized by water flushing. The ultrasonic time-domain reflectometry was employed to enable real-time observation of the wetting interface migration at various membrane locations during flushing. The results showed an enhanced wetting restoration along the membrane’s axial direction, ascribed to reduced wetting depths from inlet to outlet positions. Decreasing the flow rate and the water temperature accelerates the cleaning efficacy of water flushing because it dramatically enlarges the cleaning depth. These findings were further supported by optical coherence tomography, computational fluid dynamic simulations and force balance theoretical calculations. Our results provide a comprehensive evaluation of local wetting restoration along membrane and shed light on effective maintenance strategies for hydrophobicity recovery of MD systems.
{"title":"Unraveling the impact of uneven wetting induced by temperature distribution on wetting restoration by water flushing","authors":"Lu Xiao, Jiahao Mo, Yang Yang, Xianhui Li","doi":"10.1016/j.seppur.2025.132268","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132268","url":null,"abstract":"Membrane distillation (MD) provides an effective solution for hypersaline wastewater treatment. However, its widespread industrial application is hindered by surfactant-induced wetting that leads to a decline in membrane performance. Removing surfactants through water flushing has emerged as a practicable strategy for wetting restoration. Nevertheless, the uneven distribution of temperature along the membrane axis can affect the uniformity of wetting, which may in turn influence the overall recovery of membrane wetting. To address this issue, this work studied the impact of non-uniform wetting on wetting restoration realized by water flushing. The ultrasonic time-domain reflectometry was employed to enable real-time observation of the wetting interface migration at various membrane locations during flushing. The results showed an enhanced wetting restoration along the membrane’s axial direction, ascribed to reduced wetting depths from inlet to outlet positions. Decreasing the flow rate and the water temperature accelerates the cleaning efficacy of water flushing because it dramatically enlarges the cleaning depth. These findings were further supported by optical coherence tomography, computational fluid dynamic simulations and force balance theoretical calculations. Our results provide a comprehensive evaluation of local wetting restoration along membrane and shed light on effective maintenance strategies for hydrophobicity recovery of MD systems.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"19 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477374","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 : 2025-02-24DOI: 10.1016/j.seppur.2025.132265
Yunlong Wang, Rongshan Bi, Jijun Ge, Pan Xu
Volatile organic compounds (VOC) are one of the primary pollutants in the atmosphere, mainly from industrial emissions, vehicle exhaust, incomplete fuel combustion, and other processes. The emission of VOCs not only causes harm to air quality and the ecological environment but also seriously threatens human health. Thus, it is highly important to develop environmentally friendly and effective technologies for VOC capture. In recent years, ionic liquids (ILs), a new type of green solvent, have attracted unprecedented attention due to their non-volatility, high thermal stability, and structural tunability, showing great potential in VOC capture. The designability of ILs enables them to optimize their capture performance for specific VOCs by selecting appropriate cations and anions. This review systematically summarizes the research progress of ILs in capturing different types of VOCs, including the capture mechanisms and application examples of volatile hydrocarbons, oxygen-containing VOCs, chlorine-containing VOCs, sulfur-containing VOCs, and fluorine-containing VOCs. In addition, IL regeneration methods have also been introduced to achieve efficient recycling. Finally, current research challenges and future development directions are summarized and prospected. This review provides a scientific basis for applying ILs in VOC capture and a reference for future research
{"title":"VOCs absorption using ionic liquids","authors":"Yunlong Wang, Rongshan Bi, Jijun Ge, Pan Xu","doi":"10.1016/j.seppur.2025.132265","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132265","url":null,"abstract":"Volatile organic compounds (VOC) are one of the primary pollutants in the atmosphere, mainly from industrial emissions, vehicle exhaust, incomplete fuel combustion, and other processes. The emission of VOCs not only causes harm to air quality and the ecological environment but also seriously threatens human health. Thus, it is highly important to develop environmentally friendly and effective technologies for VOC capture. In recent years, ionic liquids (ILs), a new type of green solvent, have attracted unprecedented attention due to their non-volatility, high thermal stability, and structural tunability, showing great potential in VOC capture. The designability of ILs enables them to optimize their capture performance for specific VOCs by selecting appropriate cations and anions. This review systematically summarizes the research progress of ILs in capturing different types of VOCs, including the capture mechanisms and application examples of volatile hydrocarbons, oxygen-containing VOCs, chlorine-containing VOCs, sulfur-containing VOCs, and fluorine-containing VOCs. In addition, IL regeneration methods have also been introduced to achieve efficient recycling. Finally, current research challenges and future development directions are summarized and prospected. This review provides a scientific basis for applying ILs in VOC capture and a reference for future research","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"128 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485856","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}
This study evaluated the separation performance of an ammonium ion concentration process in aqueous solutions using osmotically assisted reverse osmosis (OARO) membrane separation. The investigation focused on the advanced separation of an aqueous ammonium chloride solution (flow rate: 1000 kg/day, concentration: 0.4 wt%) by analyzing discharge pressure, membrane area, and reflux ratio as the main parameters for both OARO and RO systems. The results indicated that OARO achieved higher separation performance and energy efficiency compared to RO under conditions where discharge pressure exceeded 4.0 MPa, the reflux ratio was above 7.2, and the membrane area was at least 45 m2. It was found that as the discharge pressure, membrane area and reflux ratio increased in OARO, the concentration ratio increased up to 50 times. Notably, it was suggested that reducing the membrane area towards the downstream side in OARO improves the concentration performance regardless of the total membrane area, identifying this as a key parameter in process design.
{"title":"Design of an ammonium chloride aqueous solution concentration process using osmotically assisted reverse osmosis (OARO)","authors":"Yota Fujii, Shuya Yoneyama, Masaru Nakaiwa, Keigo Matsuda","doi":"10.1016/j.seppur.2025.132266","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132266","url":null,"abstract":"This study evaluated the separation performance of an ammonium ion concentration process in aqueous solutions using osmotically assisted reverse osmosis (OARO) membrane separation. The investigation focused on the advanced separation of an aqueous ammonium chloride solution (flow rate: 1000 kg/day, concentration: 0.4 wt%) by analyzing discharge pressure, membrane area, and reflux ratio as the main parameters for both OARO and RO systems. The results indicated that OARO achieved higher separation performance and energy efficiency compared to RO under conditions where discharge pressure exceeded 4.0 MPa, the reflux ratio was above 7.2, and the membrane area was at least 45 m<sup>2</sup>. It was found that as the discharge pressure, membrane area and reflux ratio increased in OARO, the concentration ratio increased up to 50 times. Notably, it was suggested that reducing the membrane area towards the downstream side in OARO improves the concentration performance regardless of the total membrane area, identifying this as a key parameter in process design.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"52 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485812","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 expansion of nuclear energy necessitates advances uranium recovery from radioactive wastewater containing persistent UO22+-organic complexes. We present a solar-driven coupling system (SSCS) integrating the TiO2 nanorod (TNR) photoanodes with the NiCo2O4 nanowire-decorated carbon felt cathode (NiCo2O4-CF), enabling simultaneous uranium removal and organic pollutant degradation. The SSCS enhances photo-generated charge excitation with providing a bias potential, which drives rapid electron transfer from organics to UO22+ adsorption and reduction sites. The NiCo2O4-CF cathode maintains excellent efficiency of 97.8 % and 98.0 % for uranium reduction and Rhodamine B (RhB) degradation, respectively, through 20 cycles in complex wastewater matrices. This study proposes a nanostructure-engineered electrode with excellent electrochemical performance, offering a straightforward, resourceful and sustainable solution for uranium-laden radioactive wastewater remediation that synergizes environmental decontamination with nuclear resource recovery within circular economy frameworks.
{"title":"A NiCo2O4 nanowire arrays decorated carbon felt cathode for synergistic treatment of complex uranium-organic wastewater in a self-driven solar coupling system","authors":"Guolong Tang, Qingyan Zhang, Yuhan Cao, Jiachen Wang, Yaqian Zhang, Qingyi Zeng","doi":"10.1016/j.seppur.2025.132257","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132257","url":null,"abstract":"The expansion of nuclear energy necessitates advances uranium recovery from radioactive wastewater containing persistent UO<sub>2</sub><sup>2+</sup>-organic complexes. We present a solar-driven coupling system (SSCS) integrating the TiO<sub>2</sub> nanorod (TNR) photoanodes with the NiCo<sub>2</sub>O<sub>4</sub> nanowire-decorated carbon felt cathode (NiCo<sub>2</sub>O<sub>4</sub>-CF), enabling simultaneous uranium removal and organic pollutant degradation. The SSCS enhances photo-generated charge excitation with providing a bias potential, which drives rapid electron transfer from organics to UO<sub>2</sub><sup>2+</sup> adsorption and reduction sites. The NiCo<sub>2</sub>O<sub>4</sub>-CF cathode maintains excellent efficiency of 97.8 % and 98.0 % for uranium reduction and Rhodamine B (RhB) degradation, respectively, through 20 cycles in complex wastewater matrices. This study proposes a nanostructure-engineered electrode with excellent electrochemical performance, offering a straightforward, resourceful and sustainable solution for uranium-laden radioactive wastewater remediation that synergizes environmental decontamination with nuclear resource recovery within circular economy frameworks.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"174 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485811","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 : 2025-02-24DOI: 10.1016/j.seppur.2025.132267
Qindong Wang, Yu Yang, Shiqiang Liang, Tongyao Wu, Jinkai Zhang, Yixin Ji, Zhongmin Su, Chi Wang, Zhi Geng, Mingxin Huo
Amid escalating global water scarcity, the efficient treatment of brackish water as a desalination source holds critical importance for ensuring water security and promoting sustainable development. In this study, we developed a novel photothermal hydrogel draw agent, CB-PNIPAM/SA, optimized for forward osmosis (FO) desalination. This hydrogel enables effective brackish water desalination and draw agent regeneration driven solely by solar irradiation. The CB-PNIPAM/SA hydrogel integrates sodium acrylate (SA), N-isopropyl acrylamide (NIPAM), and carbon black (CB), where SA provides high osmotic pressure, NIPAM offers pronounced thermosensitivity, and CB facilitating solar-driven photothermal conversion. This synergistic design supports freshwater recovery through evaporation while ensuring efficient regeneration of the draw agent. Under continuous solar irradiation, the 3 %CB-PNIPAM/SA hydrogel achieved a water flux of 9.46 L m−2 per day and a freshwater recovery rate of 8.16 kg m−2 per day over a five-day cycle, highlighting its potential for sustainable all-weather (continuous operation across diurnal cycles) desalination applications. This study offers a novel strategy for continuous brackish water desalination using solar energy, presenting a promising approach to mitigate global water scarcity and advance sustainable development.
{"title":"Solar-driven bifunctional hydrogel enables all-weather pure water and draw agent regeneration for forward osmosis","authors":"Qindong Wang, Yu Yang, Shiqiang Liang, Tongyao Wu, Jinkai Zhang, Yixin Ji, Zhongmin Su, Chi Wang, Zhi Geng, Mingxin Huo","doi":"10.1016/j.seppur.2025.132267","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132267","url":null,"abstract":"Amid escalating global water scarcity, the efficient treatment of brackish water as a desalination source holds critical importance for ensuring water security and promoting sustainable development. In this study, we developed a novel photothermal hydrogel draw agent, CB-PNIPAM/SA, optimized for forward osmosis (FO) desalination. This hydrogel enables effective brackish water desalination and draw agent regeneration driven solely by solar irradiation. The CB-PNIPAM/SA hydrogel integrates sodium acrylate (SA), N-isopropyl acrylamide (NIPAM), and carbon black (CB), where SA provides high osmotic pressure, NIPAM offers pronounced thermosensitivity, and CB facilitating solar-driven photothermal conversion. This synergistic design supports freshwater recovery through evaporation while ensuring efficient regeneration of the draw agent. Under continuous solar irradiation, the 3 %CB-PNIPAM/SA hydrogel achieved a water flux of 9.46 L m<sup>−2</sup> per day and a freshwater recovery rate of 8.16 kg m<sup>−2</sup> per day over a five-day cycle, highlighting its potential for sustainable all-weather (continuous operation across diurnal cycles) desalination applications. This study offers a novel strategy for continuous brackish water desalination using solar energy, presenting a promising approach to mitigate global water scarcity and advance sustainable development.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"175 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477371","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 : 2025-02-24DOI: 10.1016/j.seppur.2025.132254
Sergio V. Gutiérrez-Hernández, Fernando Pardo, Andrew B. Foster, Peter M. Budd, Gabriel Zarca, Ane Urtiaga
In this work, we explored for the first time the gas separation performance of a branched PIM-1 polymer ( 11 % substituted) in a hollow fiber-thin film composite membrane (HF–TFCM) configuration. HF-TFCMs were successfully obtained by the dip-coating methodology with a 1–2 µm thin selective layer of the branched PIM-1 (B-PIM-1). The permeability of these membranes to pure carbon dioxide, methane, nitrogen, carbon monoxide and hydrogen was tested in a tubular membrane module. The herein prepared HF-TFCMs offered a remarkable initial CO2 permeance of 650 GPU, along with ideal gas selectivity of 20.8 and 14.8 for CO2/N2 and CO2/CO separations, respectively. In addition, the aging of the B-PIM-1 HF-TFCM was weekly monitored over 307 days, showing a 54 % permeance drop for CO2 with a 24 % drop in CO2/N2 selectivity, highlighting a moderate aging resistance of the B-PIM-1 structure. The membrane performance for mixed gas separation was further explored with CO2/N2 mixtures in the range 10–70 CO2 vol%, and, for the first time, with a CO2/CO mixture (50/50 vol%), showing similar performance to that observed with pure gases for CO2/N2 separation and only a slightly lower CO2 permeance in CO2/CO separation. These results emphasize the potential of B-PIM-1 hollow fibers for the recovery of CO2 from CO2/N2 and CO2/CO mixtures. In addition, gas sorption isotherms of all gases at 30 °C were obtained and modelled. The solubility results showed that the branched structure did not affect gas solubility compared to the conventional predominantly di-substituted PIM-1.
{"title":"Gas separation performance of branched PIM-1 thin-film composite hollow fiber membranes","authors":"Sergio V. Gutiérrez-Hernández, Fernando Pardo, Andrew B. Foster, Peter M. Budd, Gabriel Zarca, Ane Urtiaga","doi":"10.1016/j.seppur.2025.132254","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132254","url":null,"abstract":"In this work, we explored for the first time the gas separation performance of a branched PIM-1 polymer (<span><span style=\"\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mspace width=\"3.33333pt\" is=\"true\" /></math>' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"0.24ex\" role=\"img\" style=\"vertical-align: -0.12ex;\" viewbox=\"0 -51.7 333.3 103.4\" width=\"0.774ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mspace is=\"true\" width=\"3.33333pt\"></mspace></math></span></span><script type=\"math/mml\"><math><mspace width=\"3.33333pt\" is=\"true\"></mspace></math></script></span> 11 % substituted) in a hollow fiber-thin film composite membrane (HF–TFCM) configuration. HF-TFCMs were successfully obtained by the dip-coating methodology with a 1–2 µm thin selective layer of the branched PIM-1 (B-PIM-1). The permeability of these membranes to pure carbon dioxide, methane, nitrogen, carbon monoxide and hydrogen was tested in a tubular membrane module. The herein prepared HF-TFCMs offered a remarkable initial CO<sub>2</sub> permeance of 650 GPU, along with ideal gas selectivity of 20.8 and 14.8 for CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CO separations, respectively. In addition, the aging of the B-PIM-1 HF-TFCM was weekly monitored over 307 days, showing a 54 % permeance drop for CO<sub>2</sub> with a 24 % drop in CO<sub>2</sub>/N<sub>2</sub> selectivity, highlighting a moderate aging resistance of the B-PIM-1 structure. The membrane performance for mixed gas separation was further explored with CO<sub>2</sub>/N<sub>2</sub> mixtures in the range 10–70 CO<sub>2</sub> vol%, and, for the first time, with a CO<sub>2</sub>/CO mixture (50/50 vol%), showing similar performance to that observed with pure gases for CO<sub>2</sub>/N<sub>2</sub> separation and only a slightly lower CO<sub>2</sub> permeance in CO<sub>2</sub>/CO separation. These results emphasize the potential of B-PIM-1 hollow fibers for the recovery of CO<sub>2</sub> from CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CO mixtures. In addition, gas sorption isotherms of all gases at 30 °C were obtained and modelled. The solubility results showed that the branched structure did not affect gas solubility compared to the conventional predominantly di-substituted PIM-1.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"24 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477376","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 : 2025-02-24DOI: 10.1016/j.seppur.2025.132262
Yi Hu, Tao Shi, Ao Yang, Tao Xu, Zhigang Lei, Xiangping Zhang, Weifeng Shen
The limited selectivity of single organic solvents and the high viscosity of single ionic liquids present considerable challenges to the efficient separation of azeotropic mixtures within the extractive distillation system. To address the constraints of single solvents application, a mixed solvent comprising ionic liquid and organic entrainer was investigated for azeotropes separation based on the improved extractive distillation scheme, which including the determination of effective entrainers, molecular mechanism analysis, process-scale stochastic optimization, and the heat pump-based improvement. Quantum chemical calculations were utilized to preliminarily select dimethyl sulfoxide (DMSO) and 1-butyl-3-methylimidazolium acetate ([BMIM][AC]) as a mixed solvent for the separation of a binary azeotropic mixture of ethanol and isopropyl acetate. A strong hydrogen bonding interaction between [AC]− and ethanol was observed via the interaction mechanism-based analysis. The pure [BMIM][AC], pure DMSO, and mixed solvent were integrated into the extractive distillation process design. Three conventional schemes and two heat pump-based processes were proposed and optimized using the multi-objective particle swarm optimization (MOPSO) algorithm. The results indicated that the introduction of organic solvents not only effectively mitigates the high viscosity drawback of ionic liquids but also significantly enhances economic performance. Compared to the design using pure DMSO solvent, the intensified extractive distillation with mixed solvents (HP-MEED) reduces the total annual cost by 41.21 %, lowers CO2 emissions by 58.89 %, and decreases energy consumption by 53.64 %. These results suggest that the ionic liquid-based mixed solvent exhibits significant potential for azeotropic mixture separation, and more combinations of ionic liquid-based mixtures can be expected in future studies.
{"title":"Investigation on the molecular interaction mechanisms of ionic liquid-organic mixed entrainers for azeotrope separation in extractive distillation","authors":"Yi Hu, Tao Shi, Ao Yang, Tao Xu, Zhigang Lei, Xiangping Zhang, Weifeng Shen","doi":"10.1016/j.seppur.2025.132262","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132262","url":null,"abstract":"The limited selectivity of single organic solvents and the high viscosity of single ionic liquids present considerable challenges to the efficient separation of azeotropic mixtures within the extractive distillation system. To address the constraints of single solvents application, a mixed solvent comprising ionic liquid and organic entrainer was investigated for azeotropes separation based on the improved extractive distillation scheme, which including the determination of effective entrainers, molecular mechanism analysis, process-scale stochastic optimization, and the heat pump-based improvement. Quantum chemical calculations were utilized to preliminarily select dimethyl sulfoxide (DMSO) and 1-butyl-3-methylimidazolium acetate ([BMIM][AC]) as a mixed solvent for the separation of a binary azeotropic mixture of ethanol and isopropyl acetate. A strong hydrogen bonding interaction between [AC]<sup>−</sup> and ethanol was observed via the interaction mechanism-based analysis. The pure [BMIM][AC], pure DMSO, and mixed solvent were integrated into the extractive distillation process design. Three conventional schemes and two heat pump-based processes were proposed and optimized using the multi-objective particle swarm optimization (MOPSO) algorithm. The results indicated that the introduction of organic solvents not only effectively mitigates the high viscosity drawback of ionic liquids but also significantly enhances economic performance. Compared to the design using pure DMSO solvent, the intensified extractive distillation with mixed solvents (HP-MEED) reduces the total annual cost by 41.21 %, lowers CO<sub>2</sub> emissions by 58.89 %, and decreases energy consumption by 53.64 %. These results suggest that the ionic liquid-based mixed solvent exhibits significant potential for azeotropic mixture separation, and more combinations of ionic liquid-based mixtures can be expected in future studies.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"4 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477417","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 : 2025-02-23DOI: 10.1016/j.seppur.2025.132201
Gengyi Zhang, Shiwen Dong, Chintan Jayesh Shah, Narjes Esmaeili, Kai Chen, Farhang Pazanialenjareghi, Haiqing Lin
Poly(ethylene glycol) (PEG)-based polymers have emerged as leading membrane materials for CO2/N2 separation, and higher CO2 permeability is desirable to reduce carbon capture costs. Herein, we design two series of microphase-separated bottlebrush copolymers containing PEG and highly permeable polydimethylsiloxane (PDMS) and systematically optimize the PDMS content to enhance CO2/N2 separation properties. The PDMS forms a separate phase and is partially miscible in the PEG phase, increasing CO2 permeability. The flexible brush end groups can also increase gas permeability. One of the copolymers having the best combination of CO2 permeability of 1300 Barrer and CO2/N2 selectivity of 31 was fabricated into thin-film composite membranes with the selective layer of 110 nm, which exhibits stable CO2 permeance of 2600 GPU and CO2/N2 selectivity of 25, meeting the performance target and comparable with state-of-the-art membranes for CO2/N2 separation. This study demonstrates that incorporating a highly permeable phase in a highly selective phase can maximize both permeability and selectivity for various molecular separations while retaining the large-scale manufacturability of the membranes.
{"title":"Designing microphase-separated bottlebrush copolymers of polydimethylsiloxane and poly(ethylene glycol) for carbon capture","authors":"Gengyi Zhang, Shiwen Dong, Chintan Jayesh Shah, Narjes Esmaeili, Kai Chen, Farhang Pazanialenjareghi, Haiqing Lin","doi":"10.1016/j.seppur.2025.132201","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132201","url":null,"abstract":"Poly(ethylene glycol) (PEG)-based polymers have emerged as leading membrane materials for CO<sub>2</sub>/N<sub>2</sub> separation, and higher CO<sub>2</sub> permeability is desirable to reduce carbon capture costs. Herein, we design two series of microphase-separated bottlebrush copolymers containing PEG and highly permeable polydimethylsiloxane (PDMS) and systematically optimize the PDMS content to enhance CO<sub>2</sub>/N<sub>2</sub> separation properties. The PDMS forms a separate phase and is partially miscible in the PEG phase, increasing CO<sub>2</sub> permeability. The flexible brush end groups can also increase gas permeability. One of the copolymers having the best combination of CO<sub>2</sub> permeability of 1300 Barrer and CO<sub>2</sub>/N<sub>2</sub> selectivity of 31 was fabricated into thin-film composite membranes with the selective layer of 110 nm, which exhibits stable CO<sub>2</sub> permeance of 2600 GPU and CO<sub>2</sub>/N<sub>2</sub> selectivity of 25, meeting the performance target and comparable with state-of-the-art membranes for CO<sub>2</sub>/N<sub>2</sub> separation. This study demonstrates that incorporating a highly permeable phase in a highly selective phase can maximize both permeability and selectivity for various molecular separations while retaining the large-scale manufacturability of the membranes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"30 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477378","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}