Pub Date : 2024-11-20DOI: 10.1016/j.seppur.2024.130621
Peipei Liang, Xuqiang Zhang, Bingjun Yang, Xiaofei Dong, Yun Zhao, Jiangtao Chen, Kai Chen, Lin Ge, Yan Li
Purification of dye-contaminated wastewater has always been a research hotspot, yet also a challenge, due to high concentration and species diversity of pollutants. The present study designs an efficient nitrogen-doped 3D carbon nanosheets (N-3DCNs) adsorbent with 2592.50 m2 g−1 of specific surface area and 2.68 m3/g of average pore volume based on nitrilotriacetic acid trisodium salt by combining calcination and activation techniques. Microstructure and surface potential of N-3DCNs indicate that a large number of N heteroatoms in the lattice of main material can effectively optimize Zeta potential from 1.53 to −31.08 mV with solution pH increases from 3 to 11. So, as-prepared N-3DCNs possesses necessary conditions for efficient and selective adsorption of cationic dyes due to the abundant adsorption sites and strong electrostatic interactions. When 700 mg/L of cationic rhodamine and anionic methyl orange are respectively used as high concentration industrial dye-contaminated wastewater, N-3DCNs shows 97.97 % and 89.13 % of removal efficiency within 60 min. Furthermore, the adsorption capacity of N-3DCNs displays a wider pH tolerance at 1000 mg/L of cationic concentration, with a maximum adsorption capacity of 4888.70 mg/g at pH = 7 and a minimum value of 4203.77 mg/g at pH = 3, only 14 % of attenuation rate. The kinetics mechanism of dye adsorption could be well explained by pseudo-second-order kinetic model, suggesting chemisorption behavior, while fitting better with the linear Langmuir isothermal model. The groundbreaking and exceptional adsorption performances of N-3DCNs can be attributed primarily to the high specific surface area and negatively charged active sites, facilitating synergistic adsorption.
{"title":"N-doped three-dimensional carbon nanosheets: Facile synthesis and high-concentration dye adsorption","authors":"Peipei Liang, Xuqiang Zhang, Bingjun Yang, Xiaofei Dong, Yun Zhao, Jiangtao Chen, Kai Chen, Lin Ge, Yan Li","doi":"10.1016/j.seppur.2024.130621","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130621","url":null,"abstract":"Purification of dye-contaminated wastewater has always been a research hotspot, yet also a challenge, due to high concentration and species diversity of pollutants. The present study designs an efficient nitrogen-doped 3D carbon nanosheets (N-3DCNs) adsorbent with 2592.50 m<sup>2</sup> g<sup>−1</sup> of specific surface area and 2.68 m<sup>3</sup>/g of average pore volume based on nitrilotriacetic acid trisodium salt by combining calcination and activation techniques. Microstructure and surface potential of N-3DCNs indicate that a large number of N heteroatoms in the lattice of main material can effectively optimize Zeta potential from 1.53 to −31.08 mV with solution pH increases from 3 to 11. So, as-prepared N-3DCNs possesses necessary conditions for efficient and selective adsorption of cationic dyes due to the abundant adsorption sites and strong electrostatic interactions. When 700 mg/L of cationic rhodamine and anionic methyl orange are respectively used as high concentration industrial dye-contaminated wastewater, N-3DCNs shows 97.97 % and 89.13 % of removal efficiency within 60 min. Furthermore, the adsorption capacity of N-3DCNs displays a wider pH tolerance at 1000 mg/L of cationic concentration, with a maximum adsorption capacity of 4888.70 mg/g at pH = 7 and a minimum value of 4203.77 mg/g at pH = 3, only 14 % of attenuation rate. The kinetics mechanism of dye adsorption could be well explained by pseudo-second-order kinetic model, suggesting chemisorption behavior, while fitting better with the linear Langmuir isothermal model. The groundbreaking and exceptional adsorption performances of N-3DCNs can be attributed primarily to the high specific surface area and negatively charged active sites, facilitating synergistic adsorption.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"10 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673456","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 : 2024-11-20DOI: 10.1016/j.seppur.2024.130526
Pengwei Fang, Qun Zhang, Menqgi Wu, Can Zhou, Zhengming Yang, Hongwei Yu, Zemin Ji, Yina Yi, Wen Jiang, Xinliang Chen, Yuan Gao, Mengfei Zhou, Meiwen Cao
A novel CO2-responsive hydrogel for intelligent control of gas channeling in CO2– enhanced oil recovery (CO2-EOR) and geological CO2 storage has been developed. A monomeric long-chain tertiary amine surfactant (HXB-2) that has specific amide and carboxyl groups was synthesized. The surfactant can interact with CO2 in aqueous solution to increase the viscosity and induce gelation. The hydrogel is irreversible and does not revert to solution phase after N2 bubbling. It shows excellent structural stability and thermal resistance and the viscosity remains four times higher than that of the initial solution upon heating. For the mechanism, HXB-2 protonates in CO2 environment and self-assembles into worm-like micelles (WLMs) under synergistic forces of hydrophobic interaction, hydrogen bonding, and electrostatic interaction, which further crosslink to form a three-dimensional (3D) network to induce gelation. The hydrogel can be formed in-situ to control gas channeling intelligently and redirect the gas to unswept low-permeability channels. It can enhance the recovery rate by 23.53 % and the maximum seepage resistance reaches 29.45 MPa·min·cm−3 for water-alternatinggas flooding. Moreover, by having spontaneous association and shear-dissociation properties, the hydrogel in the rock pores causes minimal damage to the reservoir. This study provides valuable insights and empirical support for the development of irreversible CO2-responsive hydrogels for CO2 chemical sequestration and gas channeling control to help EOR and geological CO2 storage.
{"title":"An intelligent CO2-responsive hydrogel for applications in enhanced oil recovery and CO2 geological storage","authors":"Pengwei Fang, Qun Zhang, Menqgi Wu, Can Zhou, Zhengming Yang, Hongwei Yu, Zemin Ji, Yina Yi, Wen Jiang, Xinliang Chen, Yuan Gao, Mengfei Zhou, Meiwen Cao","doi":"10.1016/j.seppur.2024.130526","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130526","url":null,"abstract":"A novel CO<sub>2</sub>-responsive hydrogel for intelligent control of gas channeling in CO<sub>2</sub>– enhanced oil recovery (CO<sub>2</sub>-EOR) and geological CO<sub>2</sub> storage has been developed. A monomeric long-chain tertiary amine surfactant (HXB-2) that has specific amide and carboxyl groups was synthesized. The surfactant can interact with CO<sub>2</sub> in aqueous solution to increase the viscosity and induce gelation. The hydrogel is irreversible and does not revert to solution phase after N<sub>2</sub> bubbling. It shows excellent structural stability and thermal resistance and the viscosity remains four times higher than that of the initial solution upon heating. For the mechanism, HXB-2 protonates in CO<sub>2</sub> environment and self-assembles into worm-like micelles (WLMs) under synergistic forces of hydrophobic interaction, hydrogen bonding, and electrostatic interaction, which further crosslink to form a three-dimensional (3D) network to induce gelation. The hydrogel can be formed in-situ to control gas channeling intelligently and redirect the gas to unswept low-permeability channels. It can enhance the recovery rate by 23.53 % and the maximum seepage resistance reaches 29.45 MPa·min·cm<sup>−3</sup> for water-alternatinggas flooding. Moreover, by having spontaneous association and shear-dissociation properties, the hydrogel in the rock pores causes minimal damage to the reservoir. This study provides valuable insights and empirical support for the development of irreversible CO<sub>2</sub>-responsive hydrogels for CO<sub>2</sub> chemical sequestration and gas channeling control to help EOR and geological CO<sub>2</sub> storage.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"57 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678598","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}
Significant attention has been focused on the depolymerization of lignin into monophenolics, as lignin is the most abundant biomass feedstock, and its valorization is considered crucial for a complete biomass refinery. In this study, we investigate catalytic oxidative depolymerization using novel bimetallic transition metal (Ni and Co) doped ionic liquid-polyoxometalate (ILPOM) composites under aerobic conditions. We systematically evaluate various catalysts, including [MIMPS]H2PW12O40, Ni[MIMPS]PW12O40, Co[MIMPS]PW12O40, [MIMPS]H2PMo12O40, Ni[MIMPS]PMo12O40, and Co[MIMPS]PMo12O40, assessing their impact on monomer yield and selectivity. Notably, Co[MIMPS]PMo12O40 emerges as a superior catalyst, producing high yields of key aromatic monomers, primarily vanillin and methyl vanillate, under optimized conditions. Additionally, the Co[MIMPS]PMo12O40 catalyst demonstrates effective cleavage of the C-O and/or Cα-Cβ bonds within a β-O-4 dimer model compound, indicating potential catalytic cracking capabilities. This investigation elucidates the intricate interplay among transition metals, ionic liquids (ILs), and lignin, providing a novel pathway for lignin transformation.
{"title":"Catalytic oxidative depolymerization of lignin to aromatic compounds using transition metal doped ionic Liquid-based polyoxometalate catalysts","authors":"Yu Zhang, Haoyu Deng, Mingfei Li, Luyao Zhao, Wenbiao Xu, Junyou Shi","doi":"10.1016/j.seppur.2024.130639","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130639","url":null,"abstract":"Significant attention has been focused on the depolymerization of lignin into monophenolics, as lignin is the most abundant biomass feedstock, and its valorization is considered crucial for a complete biomass refinery. In this study, we investigate catalytic oxidative depolymerization using novel bimetallic transition metal (Ni and Co) doped ionic liquid-polyoxometalate (ILPOM) composites under aerobic conditions. We systematically evaluate various catalysts, including [MIMPS]H<sub>2</sub>PW<sub>12</sub>O<sub>40</sub>, Ni[MIMPS]PW<sub>12</sub>O<sub>40</sub>, Co[MIMPS]PW<sub>12</sub>O<sub>40</sub>, [MIMPS]H<sub>2</sub>PMo<sub>12</sub>O<sub>40</sub>, Ni[MIMPS]PMo<sub>12</sub>O<sub>40</sub>, and Co[MIMPS]PMo<sub>12</sub>O<sub>40</sub>, assessing their impact on monomer yield and selectivity. Notably, Co[MIMPS]PMo<sub>12</sub>O<sub>40</sub> emerges as a superior catalyst, producing high yields of key aromatic monomers, primarily vanillin and methyl vanillate, under optimized conditions. Additionally, the Co[MIMPS]PMo<sub>12</sub>O<sub>40</sub> catalyst demonstrates effective cleavage of the C-O and/or C<sub>α</sub>-C<sub>β</sub> bonds within a β-O-4 dimer model compound, indicating potential catalytic cracking capabilities. This investigation elucidates the intricate interplay among transition metals, ionic liquids (ILs), and lignin, providing a novel pathway for lignin transformation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"8 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678639","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 : 2024-11-20DOI: 10.1016/j.seppur.2024.130610
Hongyu Li, Hao Liu, Yang Zong, Zhenyu Zhao, Zhengwei Zhou, Guojie Ye, Deli Wu
The rapid depletion of peroxydisulfate (PDS) and the competitive inactivation of reactive species by excessive Fe restrict the oxidation duration and performance of iron (Fe)-based catalysts activated PDS for in situ chemical oxidation (ISCO). Here, natural chlorite, one of the Fe-rich clay minerals, is used as activator to enhance the performance and efficiency of PDS-based ISCO. It was found that acidification of contaminated groundwater drives the slowly release of aqueous Fe(II) from chlorite and serving as the source of multiple reactive species including hydroxyl radical (•OH), sulfate radical (SO4•−), and Fe(IV). Benefitting from the controlled release of Fe(II), the scavenging of oxidative species by Fe(II) is notably alleviated, leading to the oxidant utilization efficiency of chlorite/PDS improved by 24–95 % compared to the Fe(II)/PDS and ZVI/PDS, and the costs of oxidants reduced by over 50 %. Long-term experiments indicate that PDS is relatively persistent and slowly consumed by chlorite, hence the oxidative ability for pollution control remains for over one month. This work not only proposes an effective, low-cost and promising alternative process for groundwater remediation, but also demonstrates the significance of slowly released Fe(II) in breaking the trade-off between peroxide activation rate and peroxide utilization efficiency in ISCO.
{"title":"Long-lasting and efficient peroxydisulfate-based groundwater remediation driven by the slowly released Fe(II) from natural chlorite","authors":"Hongyu Li, Hao Liu, Yang Zong, Zhenyu Zhao, Zhengwei Zhou, Guojie Ye, Deli Wu","doi":"10.1016/j.seppur.2024.130610","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130610","url":null,"abstract":"The rapid depletion of peroxydisulfate (PDS) and the competitive inactivation of reactive species by excessive Fe restrict the oxidation duration and performance of iron (Fe)-based catalysts activated PDS for in situ chemical oxidation (ISCO). Here, natural chlorite, one of the Fe-rich clay minerals, is used as activator to enhance the performance and efficiency of PDS-based ISCO. It was found that acidification of contaminated groundwater drives the slowly release of aqueous Fe(II) from chlorite and serving as the source of multiple reactive species including hydroxyl radical (<sup>•</sup>OH), sulfate radical (SO<sub>4</sub><sup>•−</sup>), and Fe(IV). Benefitting from the controlled release of Fe(II), the scavenging of oxidative species by Fe(II) is notably alleviated, leading to the oxidant utilization efficiency of chlorite/PDS improved by 24–95 % compared to the Fe(II)/PDS and ZVI/PDS, and the costs of oxidants reduced by over 50 %. Long-term experiments indicate that PDS is relatively persistent and slowly consumed by chlorite, hence the oxidative ability for pollution control remains for over one month. This work not only proposes an effective, low-cost and promising alternative process for groundwater remediation, but also demonstrates the significance of slowly released Fe(II) in breaking the trade-off between peroxide activation rate and peroxide utilization efficiency in ISCO.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"14 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673943","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 separation of ternary azeotropic mixtures is a common challenge in the chemical industry due to the unique properties of azeotropes. This phenomenon complicates the separation processes, as traditional distillation methods may not effectively separate the components. The present work introduces a novel pressure-swing distillation (NPSD) process integrated with natural decanting for the effective separation of an n-propanol/benzene/water mixture. By exploiting the liquid–liquid envelope characteristics of the mixture, phase separation prior to distillation significantly enhances the separation efficiency. The NPSD process was optimised using the NSGA-II, addressing economic, environmental, and energetic objectives. Key findings reveal that the implementation of decanting allows the NPSD process to operate without substantial pressure adjustments, thereby facilitating fine separation more efficiently than conventional pressure-swing distillation designs. The proposed NPSD process can achieve up to 25.76 % savings in TAC while reducing CO2 emissions and improving energy efficiency. Furthermore, the integration of mechanical vapour recompression heat pump and Organic Rankine Cycle systems enhances energy saving, resulting in a TAC reduction of up to 31 % and a decrease in CO2 emissions of up to 38 % compared to existing energy-efficient designs. These findings highlight the potential of the NPSD-MVR-ORC system for sustainable chemical separation processes.
{"title":"Novel sustainable design of pressure-swing distillation coupled with natural decanting and Organic Rankine Cycle for separating n-propanol/benzene/water mixture","authors":"Jian Zhai, Qingbo Sun, Zekong Peng, Jinwen Li, Jinzhou Li, Jinqiang Zhang","doi":"10.1016/j.seppur.2024.130622","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130622","url":null,"abstract":"The separation of ternary azeotropic mixtures is a common challenge in the chemical industry due to the unique properties of azeotropes. This phenomenon complicates the separation processes, as traditional distillation methods may not effectively separate the components. The present work introduces a novel pressure-swing distillation (NPSD) process integrated with natural decanting for the effective separation of an <em>n</em>-propanol/benzene/water mixture. By exploiting the liquid–liquid envelope characteristics of the mixture, phase separation prior to distillation significantly enhances the separation efficiency. The NPSD process was optimised using the NSGA-II, addressing economic, environmental, and energetic objectives. Key findings reveal that the implementation of decanting allows the NPSD process to operate without substantial pressure adjustments, thereby facilitating fine separation more efficiently than conventional pressure-swing distillation designs. The proposed NPSD process can achieve up to 25.76 % savings in TAC while reducing CO<sub>2</sub> emissions and improving energy efficiency. Furthermore, the integration of mechanical vapour recompression heat pump and Organic Rankine Cycle systems enhances energy saving, resulting in a TAC reduction of up to 31 % and a decrease in CO<sub>2</sub> emissions of up to 38 % compared to existing energy-efficient designs. These findings highlight the potential of the NPSD-MVR-ORC system for sustainable chemical separation processes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"99 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673455","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 construction of a novel ofloxacin degradation catalyst coupled with photocatalysis and PMS activation is of great significance for the regeneration of water resources. A ternary metal (Co, Zn and Mo) sulfide heterojunction with biomimetic flower structure was synthesized using the solvent heat method. And then PVDF@CoZnMoSx membranes were synthetised by researched solvent-assisted nanoparticle embedding (SANE) method, which yielded efficient ofloxacian (OFX) degradation (97.1 %) by PMS activation. The effects of actual environment (such as co-exist ions, organic matter, and actual water matrices) on OFX degradation were observed, and PVDF@CoZnMoSx-3 (Zn:Co = 3:1, PCZM3) exhibited good tolerance for these factors and application value in practice. The pathways of OFX degradation were clarified by LC-MS analysis, and T.E.S.T software simulated the toxicity of the intermediates (P1-P20) gained from LC-MS, which substantiated the efficacy and safety of the PCZM3/PMS system in OFX degradation. The reusability and stability analysis displayed that the OFX degradation of PCZM3/PMS system was maintained in 5 consecutive cycles without additional treatment, and a small number of ions (Co, Zn and Mo) were leached during the OFX degradation. Totally, a new strategy was raised to construct multivariate metal sulfide membranes and couple the photocatalysis and PMS activation, which provided new insights for catalyst membranes to optimize performance.
{"title":"Recyclable biomimetic flower membranes for ofloxacin degradation by peroxymonosulfate activation under visible-light","authors":"Liusha Cen, Fan Yu, Yunying Luo, Chengcai Li, Guojin Liu, Wangyong Jin, Hailin Zhu, Yuhai Guo","doi":"10.1016/j.seppur.2024.130620","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130620","url":null,"abstract":"The construction of a novel ofloxacin degradation catalyst coupled with photocatalysis and PMS activation is of great significance for the regeneration of water resources. A ternary metal (Co, Zn and Mo) sulfide heterojunction with biomimetic flower structure was synthesized using the solvent heat method. And then PVDF@CoZnMoSx membranes were synthetised by researched solvent-assisted nanoparticle embedding (SANE) method, which yielded efficient ofloxacian (OFX) degradation (97.1 %) by PMS activation. The effects of actual environment (such as co-exist ions, organic matter, and actual water matrices) on OFX degradation were observed, and PVDF@CoZnMoSx-3 (Zn:Co = 3:1, PCZM3) exhibited good tolerance for these factors and application value in practice. The pathways of OFX degradation were clarified by LC-MS analysis, and T.E.S.T software simulated the toxicity of the intermediates (P1-P20) gained from LC-MS, which substantiated the efficacy and safety of the PCZM3/PMS system in OFX degradation. The reusability and stability analysis displayed that the OFX degradation of PCZM3/PMS system was maintained in 5 consecutive cycles without additional treatment, and a small number of ions (Co, Zn and Mo) were leached during the OFX degradation. Totally, a new strategy was raised to construct multivariate metal sulfide membranes and couple the photocatalysis and PMS activation, which provided new insights for catalyst membranes to optimize performance.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678595","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}
A loose nanofiltration (LNF) membrane with high permeance and excellent dye/salt selectivity is highly desirable for dye/salts recovery from textile wastewater. Herein, commercial and green ribitol (RT) was employed to fabricate the LNF membrane for dye desalination. The hydroxyl in the RT reacted with acyl chloride under the catalysis of sodium hydroxide, forming a polyester film structured with microspheres, negative charge, and hydrophilic networks. The resultant RT-M membrane possessed a smooth and thin active layer with numerous polar groups. The dye desalination performance of the RT-M membrane was tailored by controlling various IP fabrication conditions. The optimized membrane (RT-M1.0) had superior water permeance (100.3 L m−2h−1 bar−1) and satisfactory CR/Na2SO4 selectivity (281.3). Additionally, the RT-M membrane had favorable stability and antifouling properties, demonstrating excellent potential for application in dye desalination. Therefore, a novel approach for fabricating membranes with outstanding dye desalination properties by using RT was proposed to achieve resource recycling.
对于从纺织废水中回收染料/盐来说，具有高渗透性和优异染料/盐选择性的松散纳滤膜（LNF）是非常理想的。在此，我们采用商用绿色核糖醇（RT）来制造用于染料脱盐的 LNF 膜。在氢氧化钠的催化作用下，RT 中的羟基与酰基氯发生反应，形成具有微球、负电荷和亲水网络结构的聚酯薄膜。由此形成的 RT-M 膜具有光滑而薄的活性层，其中含有大量极性基团。RT-M 膜的染料脱盐性能是通过控制各种 IP 制备条件来实现的。优化后的膜（RT-M1.0）具有优异的透水性（100.3 L m-2h-1 bar-1）和令人满意的 CR/Na2SO4 选择性（281.3）。此外，RT-M 膜还具有良好的稳定性和防污性能，在染料脱盐中具有出色的应用潜力。因此，我们提出了一种利用 RT 制造具有出色染料脱盐性能的膜的新方法，以实现资源循环利用。
{"title":"High-performance polyester composite nanofiltration membrane fabricated by interfacial polymerization of ribitol and trimesoyl chloride: Dye desalination performance and mechanisms","authors":"Zhongyue Sun, Hui Qiu, Xinwei Kang, Weiwei Zhou, Wenxin Yan, Feiyong Chen, Jingtao Xu, Daoji Wu, Daliang Xu, Xuewu Zhu","doi":"10.1016/j.seppur.2024.130520","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130520","url":null,"abstract":"A loose nanofiltration (LNF) membrane with high permeance and excellent dye/salt selectivity is highly desirable for dye/salts recovery from textile wastewater. Herein, commercial and green ribitol (RT) was employed to fabricate the LNF membrane for dye desalination. The hydroxyl in the RT reacted with acyl chloride under the catalysis of sodium hydroxide, forming a polyester film structured with microspheres, negative charge, and hydrophilic networks. The resultant RT-M membrane possessed a smooth and thin active layer with numerous polar groups. The dye desalination performance of the RT-M membrane was tailored by controlling various IP fabrication conditions. The optimized membrane (RT-M1.0) had superior water permeance (100.3 L m<sup>−2</sup>h<sup>−1</sup> bar<sup>−1</sup>) and satisfactory CR/Na<sub>2</sub>SO<sub>4</sub> selectivity (281.3). Additionally, the RT-M membrane had favorable stability and antifouling properties, demonstrating excellent potential for application in dye desalination. Therefore, a novel approach for fabricating membranes with outstanding dye desalination properties by using RT was proposed to achieve resource recycling.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"23 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678596","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 : 2024-11-20DOI: 10.1016/j.seppur.2024.130618
Xiaojun Lv, Xuan Tan, Zexun Han, Yongcong Wu
Numerous fluorine-containing hazardous solid wastes from the electrolytic aluminum process pose a serious threat to the ecosystem and human health. Currently, in the study of leaching on these wastes, Al and F are usually recovered by adjusting the pH of the leaching solution to precipitate aluminium hydroxyfluoride hydrate, which can be used to produce aluminum fluoride by roasting. However, aluminium hydroxyfluoride hydrate is often mingled with cryolite and other impurities when precipitating, which ultimately affects the purity of obtained aluminum fluoride by calcination. Interestingly, herein, the aluminium hydroxyfluoride hydrate residue was digested by fluorosilicic acid to effectively remove impurities and obtain a pure aluminum fluoride solution, from which the β-AlF3 product was produced by crystallization at a high-temperature. The results show that under the conditions of a temperature of 60 °C, time of 35 min, initial fluorine-aluminum molar ratio of 3:1 and initial concentration of fluorosilicic acid of 18 %, the gross yield of fluorine is 86.2 %, and the recovery of silicon in the form of SiO2 is 95.2 %. During crystallization, the product changes from AlF3·3H2O to β-AlF3 with the increase of temperature. Under the conditions of a crystallization temperature of 150 °C, an initial concentration of aluminum fluoride of 191.10 g/L and a stirring speed of 200 rpm, β-AlF3 of an average particle size of 43.22 μm was obtained by adding 5 % seed. The contents of Al and F in β-AlF3 products are 32.57 % and 61.49 % respectively, which meet the requirements of GB/T 4292–2017 (AF-0) about National Standards of China. According to DFT calculation, the β-AlF3 tends to adsorb two or three water molecules in its cavity structure, which explains why the crystallized β-AlF3 contains water of 5.10 % at 180 °C.
{"title":"Preparation of β-AlF3 from fluorine-containing wastes: Leaching with fluorosilicic acid and crystallization","authors":"Xiaojun Lv, Xuan Tan, Zexun Han, Yongcong Wu","doi":"10.1016/j.seppur.2024.130618","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130618","url":null,"abstract":"Numerous fluorine-containing hazardous solid wastes from the electrolytic aluminum process pose a serious threat to the ecosystem and human health. Currently, in the study of leaching on these wastes, Al and F are usually recovered by adjusting the pH of the leaching solution to precipitate aluminium hydroxyfluoride hydrate, which can be used to produce aluminum fluoride by roasting. However, aluminium hydroxyfluoride hydrate is often mingled with cryolite and other impurities when precipitating, which ultimately affects the purity of obtained aluminum fluoride by calcination. Interestingly, herein, the aluminium hydroxyfluoride hydrate residue was digested by fluorosilicic acid to effectively remove impurities and obtain a pure aluminum fluoride solution, from which the β-AlF<sub>3</sub> product was produced by crystallization at a high-temperature. The results show that under the conditions of a temperature of 60 °C, time of 35 min, initial fluorine-aluminum molar ratio of 3:1 and initial concentration of fluorosilicic acid of 18 %, the gross yield of fluorine is 86.2 %, and the recovery of silicon in the form of SiO<sub>2</sub> is 95.2 %. During crystallization, the product changes from AlF<sub>3</sub>·3H<sub>2</sub>O to β-AlF<sub>3</sub> with the increase of temperature. Under the conditions of a crystallization temperature of 150 °C, an initial concentration of aluminum fluoride of 191.10 g/L and a stirring speed of 200 rpm, β-AlF<sub>3</sub> of an average particle size of 43.22 μm was obtained by adding 5 % seed. The contents of Al and F in β-AlF<sub>3</sub> products are 32.57 % and 61.49 % respectively, which meet the requirements of GB/T 4292–2017 (AF-0) about National Standards of China. According to DFT calculation, the β-AlF<sub>3</sub> tends to adsorb two or three water molecules in its cavity structure, which explains why the crystallized β-AlF<sub>3</sub> contains water of 5.10 % at 180 °C.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"818 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673457","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 : 2024-11-19DOI: 10.1016/j.seppur.2024.130598
Musie Welldegerima Atsbha, Oded Nir, Treavor H. Boyer
This study explores a novel multi-stage process for recovering valuable nutrients–nitrogen, phosphorus, and potassium–from real hydrolyzed urine as value-added products. The approach utilizes a combination of membrane contactor, zeolite ion exchange, and mineral precipitation techniques. A closed-loop system was established by reusing the acid regeneration solution from ion exchange as the acid-stripping solution in the hollow fiber membrane contactor (HFMC), thereby minimizing chemical usage. Ammonia recovery using the HFMC achieved over 90 % removal across three cycles from hydrolyzed urine. Zeolite columns of chabazite and clinoptilolite demonstrated consistent potassium recovery from HFMC-treated urine, with slightly higher uptake by chabazite compared with clinoptilolite. This suggests zeolite selection can be based on cost and availability. The regeneration of the potassium-saturated zeolite columns using sulfuric acid exhibited rapid and substantial amounts of potassium desorption. Potassium regeneration remained stable over two cycles, with potassium concentrations reaching up to 14 g/L. The release of other ions, such as sodium, was minor compared with potassium, highlighting the minimal impact of sodium interference. The combined ammonia–potassium liquid fertilizer exhibited a favorable N:K mass ratio (3.6 % N and 0.7 % K), with negligible amounts of other ions, making it suitable for facilitating plant growth. Iron phosphate precipitation, a promising alternative resource for fertilizer or lithium iron phosphate batteries, was successfully achieved. Iron doses were more effective in precipitating phosphate at neutral pH than basic pH, reaching over 90 % phosphate removal. This study provides a promising approach for recovering valuable resources from human urine, promoting a more sustainable approach to wastewater management and nutrient recycling.
{"title":"Multi-stage recovery of ammonia–potassium liquid fertilizer and phosphate mineral from real human urine","authors":"Musie Welldegerima Atsbha, Oded Nir, Treavor H. Boyer","doi":"10.1016/j.seppur.2024.130598","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130598","url":null,"abstract":"This study explores a novel multi-stage process for recovering valuable nutrients–nitrogen, phosphorus, and potassium–from real hydrolyzed urine as value-added products. The approach utilizes a combination of membrane contactor, zeolite ion exchange, and mineral precipitation techniques. A closed-loop system was established by reusing the acid regeneration solution from ion exchange as the acid-stripping solution in the hollow fiber membrane contactor (HFMC), thereby minimizing chemical usage. Ammonia recovery using the HFMC achieved over 90 % removal across three cycles from hydrolyzed urine. Zeolite columns of chabazite and clinoptilolite demonstrated consistent potassium recovery from HFMC-treated urine, with slightly higher uptake by chabazite compared with clinoptilolite. This suggests zeolite selection can be based on cost and availability. The regeneration of the potassium-saturated zeolite columns using sulfuric acid exhibited rapid and substantial amounts of potassium desorption. Potassium regeneration remained stable over two cycles, with potassium concentrations reaching up to 14 g/L. The release of other ions, such as sodium, was minor compared with potassium, highlighting the minimal impact of sodium interference. The combined ammonia–potassium liquid fertilizer exhibited a favorable N:K mass ratio (3.6 % N and 0.7 % K), with negligible amounts of other ions, making it suitable for facilitating plant growth. Iron phosphate precipitation, a promising alternative resource for fertilizer or lithium iron phosphate batteries, was successfully achieved. Iron doses were more effective in precipitating phosphate at neutral pH than basic pH, reaching over 90 % phosphate removal. This study provides a promising approach for recovering valuable resources from human urine, promoting a more sustainable approach to wastewater management and nutrient recycling.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670921","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 : 2024-11-19DOI: 10.1016/j.seppur.2024.130593
Biswajit Mishra, Nidhi C. Dubey, Bijay P. Tripathi
Self-assembly of block copolymers (BCPs) offers numerous advantages in forming membranes with ordered porous architectures, showcasing their potential applications in membrane-based separation applications. However, the spontaneous accumulation of various foulants or biofoulants on the membrane surface severely hampers their practical applicability. Establishing stable functionalization of BCPs to create an anti(−bio)fouling surface without compromising the porous morphology of membranes is an ideal choice. In this context, we fabricated an isoporous membrane through the self-assembly of polystyrene-b-poly(4-vinyl pyridine) (PS-b-P4VP) BCP followed by covalent functionalization of pyridine moieties with zwitterionic pyrazolium moieties to obtain dual-charged (containing quaternized pyridinium and zwitterionic pyrazolium moieties) BCP-Py-Z membrane. The functionalization imparted anti(bio)fouling properties to the membranes. After post-functionalization, the quaternized pyridine and sulfobetaine pyrazolium moieties were thoroughly characterized using various techniques. Benefitting from this modification, the BCP-Py-Z membrane exhibited robust bactericidal properties against both E. coli and S. epidermidis bacteria and resulted in reduced fouling with organic compounds. Compared to the pristine BCP membrane, which is severely affected by fouling, the BCP-Py-Z membrane exhibits a much higher BSA rejection (∼95 %) and flux recovery (∼92 %). Most importantly, the BCP-Py-Z membrane consistently maintained its water filtration and flux recovery tendency throughout the continuous dynamic fouling experiment cycle. This work embodies a straightforward and stable surface functionalization method to endow BCP membrane with a strong antifouling surface, which proves advantageous for various membrane-based filtration applications.
{"title":"Zwitterionic pyrazole functionalized PS-b-P4VP block copolymer membranes with enhanced Anti(−bio)fouling properties","authors":"Biswajit Mishra, Nidhi C. Dubey, Bijay P. Tripathi","doi":"10.1016/j.seppur.2024.130593","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130593","url":null,"abstract":"Self-assembly of block copolymers (BCPs) offers numerous advantages in forming membranes with ordered porous architectures, showcasing their potential applications in membrane-based separation applications. However, the spontaneous accumulation of various foulants or biofoulants on the membrane surface severely hampers their practical applicability. Establishing stable functionalization of BCPs to create an anti(−bio)fouling surface without compromising the porous morphology of membranes is an ideal choice. In this context, we fabricated an isoporous membrane through the self-assembly of polystyrene-<em>b</em>-poly(4-vinyl pyridine) (PS-<em>b</em>-P4VP) BCP followed by covalent functionalization of pyridine moieties with zwitterionic pyrazolium moieties to obtain dual-charged (containing quaternized pyridinium and zwitterionic pyrazolium moieties) BCP-Py-Z membrane. The functionalization imparted anti(bio)fouling properties to the membranes. After post-functionalization, the quaternized pyridine and sulfobetaine pyrazolium moieties were thoroughly characterized using various techniques. Benefitting from this modification, the BCP-Py-Z membrane exhibited robust bactericidal properties against both <em>E. coli</em> and <em>S. epidermidis</em> bacteria and resulted in reduced fouling with organic compounds. Compared to the pristine BCP membrane, which is severely affected by fouling, the BCP-Py-Z membrane exhibits a much higher BSA rejection (∼95 %) and flux recovery (∼92 %). Most importantly, the BCP-Py-Z membrane consistently maintained its water filtration and flux recovery tendency throughout the continuous dynamic fouling experiment cycle. This work embodies a straightforward and stable surface functionalization method to endow BCP membrane with a strong antifouling surface, which proves advantageous for various membrane-based filtration applications.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"99 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670924","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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