Pub Date : 2024-10-24DOI: 10.1016/j.memsci.2024.123449
Yan Huang , Guangyong Zhang , Zijie Xu , Xiantong Zhao , Wenqi Xie , Luyao Wang , Zhe Zhai , Jie Liu , Shuaifei Zhao , Yuchao Zhao
Poly (tetrafluoroethylene) (PTFE) can be used for robust separation membranes owing to its exceptional chemical and thermal stabilities. Simultaneously achieving construction of hierarchical pore structures and re-entrant surface microstructures during the fabrication of PTFE membrane holds significant importance in addressing the issues of low flux and membrane wetting in membrane distillation (MD). Herein, we proposed a flexible method for manufacturing hierarchically structured PTFE membrane by combining electrospinning/spraying with sintering/welding. The present approach facilitated the controlled fabrication of a superhydrophobic PTFE membrane with slippery surface (exhibiting a water contact angle of 153.5°, and an ultralow sliding angle of 7.5°) without using fluoride-based solvents or external nanoparticles. Moreover, the anti-wetting mechanism and performance stability of the PTFE membranes in MD were thoroughly investigated. In liquid desiccant regeneration experiments, the 20 wt% LiCl solution was successfully concentrated to 28.64 wt%. Furthermore, the PTFE membrane demonstrated a stable flux (>30 kg m−2 h−1) and relatively low permeate conductivity (<15 μs cm−1) during treating simulated seawater for 30 h. The present work offers a new approach to fabricate multi-hierarchical structured superhydrophobic membranes for desalination and regeneration of liquid desiccants.
{"title":"Multi-hierarchical structured PTFE membrane for liquid desiccant dewatering via membrane distillation","authors":"Yan Huang , Guangyong Zhang , Zijie Xu , Xiantong Zhao , Wenqi Xie , Luyao Wang , Zhe Zhai , Jie Liu , Shuaifei Zhao , Yuchao Zhao","doi":"10.1016/j.memsci.2024.123449","DOIUrl":"10.1016/j.memsci.2024.123449","url":null,"abstract":"<div><div>Poly (tetrafluoroethylene) (PTFE) can be used for robust separation membranes owing to its exceptional chemical and thermal stabilities. Simultaneously achieving construction of hierarchical pore structures and re-entrant surface microstructures during the fabrication of PTFE membrane holds significant importance in addressing the issues of low flux and membrane wetting in membrane distillation (MD). Herein, we proposed a flexible method for manufacturing hierarchically structured PTFE membrane by combining electrospinning/spraying with sintering/welding. The present approach facilitated the controlled fabrication of a superhydrophobic PTFE membrane with slippery surface (exhibiting a water contact angle of 153.5°, and an ultralow sliding angle of 7.5°) without using fluoride-based solvents or external nanoparticles. Moreover, the anti-wetting mechanism and performance stability of the PTFE membranes in MD were thoroughly investigated. In liquid desiccant regeneration experiments, the 20 wt% LiCl solution was successfully concentrated to 28.64 wt%. Furthermore, the PTFE membrane demonstrated a stable flux (>30 kg m<sup>−2</sup> h<sup>−1</sup>) and relatively low permeate conductivity (<15 μs cm<sup>−1</sup>) during treating simulated seawater for 30 h. The present work offers a new approach to fabricate multi-hierarchical structured superhydrophobic membranes for desalination and regeneration of liquid desiccants.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123449"},"PeriodicalIF":8.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535108","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}
Pervaporation (PV) shows significant potential for the highly selective isopropanol (IPA). The pursuit of developing PV membranes with outstanding separation effect and enduring high purity permeation is an indispensable goal. Based on polyamide (PA) separation layers, a polydopamine (PDA) mixed g-C3N4 quantum dots (gCNQDs) coating as the interlayer was deposited onto a porous ceramic hollow fiber substrate to fabricate thin-film nanocomposite membranes with an interlayer (TFNi). The nanocomposite interlayer enabled the formation of a smoother and highly separated selective polyamide layer. The separation factor exhibited a 31-fold enhancement with the augmentation of the blending fraction of gCNQDs during the PDA coating process. The resulting TFNi membrane attained an exceedingly high separation factor of 10270 ± 90 with a permeate water concentration of 99.9 % and demonstrated a satisfactory flux of 1.40 ± 0.08 kg m−2 h−1 during the PV process of 90 wt% IPA dehydration at 60 °C. This study presents a fresh perspective on the implementation of nanocomposite interlayers, which is expected to expand the application of high-performance TFNi membranes in PV dehydration processes.
{"title":"A novel TFNi pervaporation membrane with g-C3N4 quantum dots for high-efficiency IPA dehydration","authors":"Jia-Rui Yang, Yu-Fei Lin, Zhen-Liang Xu, Rui Jia, Yin-Xin Fang","doi":"10.1016/j.memsci.2024.123451","DOIUrl":"10.1016/j.memsci.2024.123451","url":null,"abstract":"<div><div>Pervaporation (PV) shows significant potential for the highly selective isopropanol (IPA). The pursuit of developing PV membranes with outstanding separation effect and enduring high purity permeation is an indispensable goal. Based on polyamide (PA) separation layers, a polydopamine (PDA) mixed g-C<sub>3</sub>N<sub>4</sub> quantum dots (gCNQDs) coating as the interlayer was deposited onto a porous ceramic hollow fiber substrate to fabricate thin-film nanocomposite membranes with an interlayer (TFNi). The nanocomposite interlayer enabled the formation of a smoother and highly separated selective polyamide layer. The separation factor exhibited a 31-fold enhancement with the augmentation of the blending fraction of gCNQDs during the PDA coating process. The resulting TFNi membrane attained an exceedingly high separation factor of 10270 ± 90 with a permeate water concentration of 99.9 % and demonstrated a satisfactory flux of 1.40 ± 0.08 kg m<sup>−2</sup> h<sup>−1</sup> during the PV process of 90 wt% IPA dehydration at 60 °C. This study presents a fresh perspective on the implementation of nanocomposite interlayers, which is expected to expand the application of high-performance TFNi membranes in PV dehydration processes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123451"},"PeriodicalIF":8.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535104","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 : 2024-10-23DOI: 10.1016/j.memsci.2024.123426
Xiao-Yang Liu , Yubo Chen , Ying Bai , Longyi Lv , Wenfang Gao , Li Sun , Jinsong Liang , Zhijun Ren , Houyun Yang , Guangming Zhang
Biofouling significantly hampers the performance and longevity of ultrafiltration (UF) membranes employed in saline wastewater treatment. This research addresses a crucial knowledge gap by meticulously investigating the influence of salinity variations (0–10 g/L NaCl) on biofouling characteristics, utilizing advanced spectroscopic and microscopic techniques. Combined blocking models elucidated the evolution of fouling mechanisms under varying salinity conditions. Higher salinity levels promoted cake layer formation, potentially circumventing initial fouling stages observed under lower salinity conditions. Quantification of confocal laser scanning microscopy images revealed a denser, thinner, and less heterogeneous cake layer at high salinity, composed of proteins, nucleic acids, and α-polysaccharides. The relatively high abundance of polysaccharides may contribute to maintaining osmotic pressure and bacterial cell viability. Moreover, the integration of the confocal Raman mapping technique and non-negative matrix factorization analysis was innovatively applied to characterize the biofouling layer, identifying the important role of carotenoids within the layer. Carotenoids were found to be more abundant in the upper regions of the biofouling layer formed at high salinity, potentially scavenging the reactive oxygen species within bacterial cells. In conclusion, this investigation offers a comprehensive understanding of the salinity-dependent alterations in the chemical composition and spatial structure of the membrane fouling layer. The findings may facilitate the development of targeted mitigation strategies to combat membrane biofouling in saline wastewater treatment applications.
{"title":"Unraveling the impact of salinity on biofouling on ultrafiltration membranes: A spectroscopic and microscopic view","authors":"Xiao-Yang Liu , Yubo Chen , Ying Bai , Longyi Lv , Wenfang Gao , Li Sun , Jinsong Liang , Zhijun Ren , Houyun Yang , Guangming Zhang","doi":"10.1016/j.memsci.2024.123426","DOIUrl":"10.1016/j.memsci.2024.123426","url":null,"abstract":"<div><div>Biofouling significantly hampers the performance and longevity of ultrafiltration (UF) membranes employed in saline wastewater treatment. This research addresses a crucial knowledge gap by meticulously investigating the influence of salinity variations (0–10 g/L NaCl) on biofouling characteristics, utilizing advanced spectroscopic and microscopic techniques. Combined blocking models elucidated the evolution of fouling mechanisms under varying salinity conditions. Higher salinity levels promoted cake layer formation, potentially circumventing initial fouling stages observed under lower salinity conditions. Quantification of confocal laser scanning microscopy images revealed a denser, thinner, and less heterogeneous cake layer at high salinity, composed of proteins, nucleic acids, and α-polysaccharides. The relatively high abundance of polysaccharides may contribute to maintaining osmotic pressure and bacterial cell viability. Moreover, the integration of the confocal Raman mapping technique and non-negative matrix factorization analysis was innovatively applied to characterize the biofouling layer, identifying the important role of carotenoids within the layer. Carotenoids were found to be more abundant in the upper regions of the biofouling layer formed at high salinity, potentially scavenging the reactive oxygen species within bacterial cells. In conclusion, this investigation offers a comprehensive understanding of the salinity-dependent alterations in the chemical composition and spatial structure of the membrane fouling layer. The findings may facilitate the development of targeted mitigation strategies to combat membrane biofouling in saline wastewater treatment applications.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123426"},"PeriodicalIF":8.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660215","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 : 2024-10-23DOI: 10.1016/j.memsci.2024.123445
Zhaohuan Mai , Yongxuan Shi , Bowen Li , Sheng Han , Yingxin Sun , Haochen Zhu , Ping Xu , Mengyang Hu , Tomohisa Yoshioka , Hideto Matsuyama
The rare earth elements (REEs) industrial wastewater is characterized by high ammonium nitrogen and low-strength organic compounds. Reverse osmosis (RO) process is effective for the REEs wastewater treatment. However, membrane fouling deteriorated the RO process. In this work, the fouling mechanism during RO process of REEs wastewater was elucidated via multiscale methods. A series of bench-scale fouling tests with simulated REEs wastewater containing high NH4+–N and different concentrations of 2-ethylhexyl phosphonic acid mono-(2-ethylhexyl) ester (P507) were performed with a commercial RO membrane to evaluate the fouling extent of the RO process. A critical P507 concentration (0.25 mg L−1) was observed where the fouling pattern changed qualitatively. When the P507 concentration was lower than 0.25 mg L−1, the relative flux increased and the membrane surface became more hydrophilic. When P507 reached this critical point, severe fouling occurred accompanied with a more hydrophobic membrane surface. Multiscale simulations [i.e., molecular dynamics (MD) and dissipative particle dynamics (DPD)] revealed that the fouling layer network varied with P507 concentration. This work provides in-depth insights into membrane fouling mechanism in the REEs wastewater, and has enlightening significance for fouling control strategies and the innovation of anti-fouling membrane materials.
{"title":"Multiscale insights into polyamide membrane fouling during reverse osmosis of rare earth wastewater","authors":"Zhaohuan Mai , Yongxuan Shi , Bowen Li , Sheng Han , Yingxin Sun , Haochen Zhu , Ping Xu , Mengyang Hu , Tomohisa Yoshioka , Hideto Matsuyama","doi":"10.1016/j.memsci.2024.123445","DOIUrl":"10.1016/j.memsci.2024.123445","url":null,"abstract":"<div><div>The rare earth elements (REEs) industrial wastewater is characterized by high ammonium nitrogen and low-strength organic compounds. Reverse osmosis (RO) process is effective for the REEs wastewater treatment. However, membrane fouling deteriorated the RO process. In this work, the fouling mechanism during RO process of REEs wastewater was elucidated via multiscale methods. A series of bench-scale fouling tests with simulated REEs wastewater containing high NH4<sup>+</sup>–N and different concentrations of 2-ethylhexyl phosphonic acid mono-(2-ethylhexyl) ester (P507) were performed with a commercial RO membrane to evaluate the fouling extent of the RO process. A critical P507 concentration (0.25 mg L<sup>−1</sup>) was observed where the fouling pattern changed qualitatively. When the P507 concentration was lower than 0.25 mg L<sup>−1</sup>, the relative flux increased and the membrane surface became more hydrophilic. When P507 reached this critical point, severe fouling occurred accompanied with a more hydrophobic membrane surface. Multiscale simulations [<em>i.e.</em>, molecular dynamics (MD) and dissipative particle dynamics (DPD)] revealed that the fouling layer network varied with P507 concentration. This work provides in-depth insights into membrane fouling mechanism in the REEs wastewater, and has enlightening significance for fouling control strategies and the innovation of anti-fouling membrane materials.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123445"},"PeriodicalIF":8.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535065","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 trade-off effect of the oxygen permeability and stability of oxygen transport membranes (OTMs) still exists in working atmospheres containing CO2. Herein, we reported a new series of 60 wt%Ce0.9Ln0.1O2-δ-40 wt%Ln0.6Sr0.4Fe0.9Ti0.1O3-δ (CLnO-LnSFTO, Ln = La, Pr, Nd, Sm, Gd, Tb) dual-phase OTMs by selecting different Ln elements based on the reported highly stable Ti-doped CPrO-PrSFTO. The effects of different Ln elements on the structure and oxygen permeability of Ti-doped dual-phase OTMs were systematically studied. Basically, as the atomic number of Ln elements increases, the unit cell parameters of both the fluorite phase and the perovskite phase become smaller. The unit cell volume and spatial symmetry of the perovskite phase are reduced, resulting in a reduction in oxygen permeability. The optimal CLaO-LaSFTO showed of 0.60 and 0.54 mL min−1 cm−2 with He and CO2 sweeping at 1000 °C, respectively. In addition, all CLnO-LnSFTO OTMs could work for more than 100 h with no significant performance degradation in a CO2 atmosphere, maintaining excellent stability. This work explores candidate OTM materials for CO2 capture and oxygen separation, as well as provides some ideas for addressing the trade-off effect.
{"title":"Effects of lanthanides on the structure and oxygen permeability of Ti-doped dual-phase membranes","authors":"Chao Zhang, Zaichen Xiang, Lingyong Zeng, Peifeng Yu, Kuan Li, Kangwang Wang, Longfu Li, Rui Chen, Huixia Luo","doi":"10.1016/j.memsci.2024.123446","DOIUrl":"10.1016/j.memsci.2024.123446","url":null,"abstract":"<div><div>The trade-off effect of the oxygen permeability and stability of oxygen transport membranes (OTMs) still exists in working atmospheres containing CO<sub>2</sub>. Herein, we reported a new series of 60 wt%Ce<sub>0.9</sub>Ln<sub>0.1</sub>O<sub>2-δ</sub>-40 wt%Ln<sub>0.6</sub>Sr<sub>0.4</sub>Fe<sub>0.9</sub>Ti<sub>0.1</sub>O<sub>3-δ</sub> (CLnO-LnSFTO, Ln = La, Pr, Nd, Sm, Gd, Tb) dual-phase OTMs by selecting different Ln elements based on the reported highly stable Ti-doped CPrO-PrSFTO. The effects of different Ln elements on the structure and oxygen permeability of Ti-doped dual-phase OTMs were systematically studied. Basically, as the atomic number of Ln elements increases, the unit cell parameters of both the fluorite phase and the perovskite phase become smaller. The unit cell volume and spatial symmetry of the perovskite phase are reduced, resulting in a reduction in oxygen permeability. The optimal CLaO-LaSFTO showed <span><math><mrow><msub><mi>J</mi><msub><mi>O</mi><mn>2</mn></msub></msub></mrow></math></span> of 0.60 and 0.54 mL min<sup>−1</sup> cm<sup>−2</sup> with He and CO<sub>2</sub> sweeping at 1000 °C, respectively. In addition, all CLnO-LnSFTO OTMs could work for more than 100 h with no significant performance degradation in a CO<sub>2</sub> atmosphere, maintaining excellent stability. This work explores candidate OTM materials for CO<sub>2</sub> capture and oxygen separation, as well as provides some ideas for addressing the trade-off effect.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123446"},"PeriodicalIF":8.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535063","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 investigated the effectiveness of the nanoconfined catalytic membrane (NCCM), fabricated by nitrogen-doped carbon nanotubes (NCNT) incorporated with graphene oxide membrane (NCNT@GO-M), in mitigating fouling caused by effluent organic matter (EfOM). Compared to conventional catalytic membranes (NRCM) that lack precise spatial design and prepared with only NCNT, NCCM exhibits a unique advantage by preferentially retaining and adsorbing protein-like substances in EfOM during the fouling formation process, forming a cake layer that effectively mitigates pore blockage from irreversible foulants. Furthermore, the ordered nanoconfined structure of NCCM facilitates an intelligent “pore-centric” hierarchical degradation strategy based on the molecular size of EfOM, preferentially removing irreversible foulants caused by fulvic acid-like and low molecular weight protein-like substances. The results demonstrated effective preservation of catalytic sites by the NCCM’s advanced nanoconfined configuration and a 1.6-fold increase in the mass transfer rate of peroxymonosulfate (PMS) compared to NRCM, synergistically promoting hydroxyl radical (•OH) enrichment, resulting in rapid EfOM degradation kinetics. Additionally, chemical cleaning almost completely eliminated irreversible fouling, restoring the NCCM to near its original flux. Overall, this study sheds light on the fouling mitigation mechanisms of NCCM, aiding their tailored design and application in targeted wastewater treatment.
{"title":"Nanoconfined catalytic membranes for EfOM fouling mitigation: An intelligent “pore-centric” cleaning strategy","authors":"Wenjun Wu, Jin Guo, Wenhui Wang, Xiaomeng Yu, Yufei Wang, Tong Zhou, Guangshuo Yin","doi":"10.1016/j.memsci.2024.123444","DOIUrl":"10.1016/j.memsci.2024.123444","url":null,"abstract":"<div><div>This study investigated the effectiveness of the nanoconfined catalytic membrane (NCCM), fabricated by nitrogen-doped carbon nanotubes (NCNT) incorporated with graphene oxide membrane (NCNT@GO-M), in mitigating fouling caused by effluent organic matter (EfOM). Compared to conventional catalytic membranes (NRCM) that lack precise spatial design and prepared with only NCNT, NCCM exhibits a unique advantage by preferentially retaining and adsorbing protein-like substances in EfOM during the fouling formation process, forming a cake layer that effectively mitigates pore blockage from irreversible foulants. Furthermore, the ordered nanoconfined structure of NCCM facilitates an intelligent “pore-centric” hierarchical degradation strategy based on the molecular size of EfOM, preferentially removing irreversible foulants caused by fulvic acid-like and low molecular weight protein-like substances. The results demonstrated effective preservation of catalytic sites by the NCCM’s advanced nanoconfined configuration and a 1.6-fold increase in the mass transfer rate of peroxymonosulfate (PMS) compared to NRCM, synergistically promoting hydroxyl radical (•OH) enrichment, resulting in rapid EfOM degradation kinetics. Additionally, chemical cleaning almost completely eliminated irreversible fouling, restoring the NCCM to near its original flux. Overall, this study sheds light on the fouling mitigation mechanisms of NCCM, aiding their tailored design and application in targeted wastewater treatment.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123444"},"PeriodicalIF":8.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142592963","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 : 2024-10-22DOI: 10.1016/j.memsci.2024.123442
Jieun Kang , Seung Hwan Kim , Young Kyu Hwang , Bao Tran Duy Nguyen , Jihoon Kim , Jeong F. Kim
The transition towards a carbon-neutral society necessitates radical approaches in the bio-refinery pipeline, particularly in the production of organic acids. The current downstream process from a dilute fermentation broth is limited by the extensive use of acids and bases, along with heavy reliance on energy-intensive distillation. In this work, we propose an entirely membrane-based process to purify organic acids (e.g., gluconic acid) from a crude solution of catalytic dehydrogenation of glucose. To facilitate downstream purification, we introduce an innovative membrane-assisted ion exchange (MEM-IE) strategy, which is a scalable process that can protonate ionic compounds entirely in the solution phase. Instead of a solid ion exchange resin, a bulky yet soluble acidification agent is used to protonate the target compound, which can be easily separated via a size exclusion membrane. We selected non-toxic poly (4-styrene sulfonic acid) (H-PSS, 75 kDa) as the acidification agent to selectively protonate gluconate ions and to enable facile fractionation. The proposed MEM-IE strategy can overcome the scale-up limitation of traditional solid ion exchange resins and can be applied to many types of ionic compounds. The versatility of the proposed process was also demonstrated on formate and lactate compounds. A techno-economic evaluation using the Verberne cost model showed that the proposed process achieves an 80 % reduction in energy consumption compared to the fermentation-based process, and the return on investment (ROI) of a 330 ton-per-day plant was less than a year. The proposed membrane-based process for the purification of organic acids, particularly the MEM-IE strategy, offers a sustainable and energy-efficient downstream separation platform.
{"title":"Scalable membrane-assisted ion exchange (MEM-IE) strategy for organic acid purification in biorefinery process","authors":"Jieun Kang , Seung Hwan Kim , Young Kyu Hwang , Bao Tran Duy Nguyen , Jihoon Kim , Jeong F. Kim","doi":"10.1016/j.memsci.2024.123442","DOIUrl":"10.1016/j.memsci.2024.123442","url":null,"abstract":"<div><div>The transition towards a carbon-neutral society necessitates radical approaches in the bio-refinery pipeline, particularly in the production of organic acids. The current downstream process from a dilute fermentation broth is limited by the extensive use of acids and bases, along with heavy reliance on energy-intensive distillation. In this work, we propose an entirely membrane-based process to purify organic acids (e.g., gluconic acid) from a crude solution of catalytic dehydrogenation of glucose. To facilitate downstream purification, we introduce an innovative membrane-assisted ion exchange (MEM-IE) strategy, which is a scalable process that can protonate ionic compounds entirely in the solution phase. Instead of a solid ion exchange resin, a bulky yet soluble acidification agent is used to protonate the target compound, which can be easily separated via a size exclusion membrane. We selected non-toxic poly (4-styrene sulfonic acid) (H-PSS, 75 kDa) as the acidification agent to selectively protonate gluconate ions and to enable facile fractionation. The proposed MEM-IE strategy can overcome the scale-up limitation of traditional solid ion exchange resins and can be applied to many types of ionic compounds. The versatility of the proposed process was also demonstrated on formate and lactate compounds. A techno-economic evaluation using the Verberne cost model showed that the proposed process achieves an 80 % reduction in energy consumption compared to the fermentation-based process, and the return on investment (ROI) of a 330 ton-per-day plant was less than a year. The proposed membrane-based process for the purification of organic acids, particularly the MEM-IE strategy, offers a sustainable and energy-efficient downstream separation platform.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123442"},"PeriodicalIF":8.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535105","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 : 2024-10-22DOI: 10.1016/j.memsci.2024.123434
Yiman He , Zenghao Yue , Wangxi Fang , Zilin Zhao , Yuzhang Zhu , Jian Jin
Polyamide (PA) membranes play a crucial role in nanofiltration and reverse osmosis separations, while their pore size is primary to determine the separation performance. Current methods for pore size analysis, such as atomic force microscopy (AFM), positron annihilation spectroscopy (PAS), and the filtration experiment of neutral molecules are time-consuming and lack real-time capabilities. This limitation hinders in-situ monitoring of pore size dynamics under various operating conditions. Therefore, a rapid and real-time method is highly desirable for pore size analysis. This work presents a novel approach for real-time detection of pore size variations in PA membranes under different solvent conditions. It utilizes aggregation-induced emission (AIE) with tetraphenylethylene (TPE) groups covalently linked to the PA polymer chain during interfacial polymerization using 1-(4-Aminophenyl)-1,2,2-triphenylethene as a co-monomer. Fluorescence intensity of the PA membrane serves as an indicator of the confined state of the TPE molecules within the polymer network, thereby reflecting pore size changes under various conditions. The accuracy of the AIE-based approach is validated through complementary analyses such as small-angle X-ray scattering (SAXS) and rejection of dye molecules. The observed consistency between fluorescence variations in the PA membrane and pore size changes under different solvent conditions confirms the effectiveness of this method. This work provides a valuable visual tool for in-situ monitoring of pore size dynamics in polyamide membranes.
聚酰胺（PA）膜在纳滤和反渗透分离中起着至关重要的作用，而其孔径则是决定分离性能的主要因素。目前的孔径分析方法，如原子力显微镜（AFM）、正电子湮灭光谱（PAS）和中性分子过滤实验，都非常耗时且缺乏实时性。这种限制阻碍了在各种操作条件下对孔径动态的原位监测。因此，一种快速、实时的方法非常适合孔径分析。本研究提出了一种在不同溶剂条件下实时检测 PA 膜孔径变化的新方法。它以 1-(4-氨基苯基)-1,2,2-三苯基乙烯为共聚单体，利用聚合诱导发射（AIE）将四苯基乙烯（TPE）基团在界面聚合过程中共价连接到 PA 聚合物链上。PA 膜的荧光强度可作为聚合物网络中 TPE 分子封闭状态的指标，从而反映出不同条件下孔径的变化。通过小角 X 射线散射（SAXS）和染料分子剔除等补充分析，验证了基于 AIE 方法的准确性。在不同溶剂条件下观察到的 PA 膜荧光变化与孔径变化之间的一致性证实了这种方法的有效性。这项工作为现场监测聚酰胺膜的孔径动态提供了宝贵的可视化工具。
{"title":"Unveiling the pore size change in polyamide membrane using aggregation induced emission","authors":"Yiman He , Zenghao Yue , Wangxi Fang , Zilin Zhao , Yuzhang Zhu , Jian Jin","doi":"10.1016/j.memsci.2024.123434","DOIUrl":"10.1016/j.memsci.2024.123434","url":null,"abstract":"<div><div>Polyamide (PA) membranes play a crucial role in nanofiltration and reverse osmosis separations, while their pore size is primary to determine the separation performance. Current methods for pore size analysis, such as atomic force microscopy (AFM), positron annihilation spectroscopy (PAS), and the filtration experiment of neutral molecules are time-consuming and lack real-time capabilities. This limitation hinders in-situ monitoring of pore size dynamics under various operating conditions. Therefore, a rapid and real-time method is highly desirable for pore size analysis. This work presents a novel approach for real-time detection of pore size variations in PA membranes under different solvent conditions. It utilizes aggregation-induced emission (AIE) with tetraphenylethylene (TPE) groups covalently linked to the PA polymer chain during interfacial polymerization using 1-(4-Aminophenyl)-1,2,2-triphenylethene as a co-monomer. Fluorescence intensity of the PA membrane serves as an indicator of the confined state of the TPE molecules within the polymer network, thereby reflecting pore size changes under various conditions. The accuracy of the AIE-based approach is validated through complementary analyses such as small-angle X-ray scattering (SAXS) and rejection of dye molecules. The observed consistency between fluorescence variations in the PA membrane and pore size changes under different solvent conditions confirms the effectiveness of this method. This work provides a valuable visual tool for in-situ monitoring of pore size dynamics in polyamide membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"714 ","pages":"Article 123434"},"PeriodicalIF":8.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142534645","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 : 2024-10-22DOI: 10.1016/j.memsci.2024.123437
Fariba Oulad , Ali Akbar Zinatizadeh , Sirus Zinadini , Amir Razmjou
Reverse osmosis (RO) membranes are crucial for water purification and desalination, facing challenges like balancing permeate flux and rejection, dealing with membrane fouling, and chlorine resistance. This study focuses on developing new membranes using cellulose acetate (CA) polymers and magnetic nanoparticles of magnesium ferrite (MgFe2O4) and hydroxyl-functionalized magnesium ferrite (OH–MgFe2O4) through a phase inversion method, with and without the presence of a magnetic field, to address the limitations of RO membranes. This study conducted a unique experiment where magnetic nanoparticles migrated to the membrane surface and underwent phase exchange in the coagulation bath under the influence of a 2.0 T magnetic field. As a result, the magnetic nanoparticles were arranged in a specific pattern and evenly spread across the membrane surface, enhancing the membrane's surface characteristics and hydrophilic properties. Furthermore, the flux of the synthesized membranes experienced an increase when exposed to the magnetic field, while maintaining a consistently high rejection rate. An evaluation was conducted on the membranes' resistance to organic fouling from bovine serum albumin (BSA), inorganic fouling from scaling, and the combined effects of BSA and scaling. Based on the findings, the membranes showed a notable enhancement in their anti-fouling properties, particularly when exposed to a magnetic field. An assessment was conducted on the resistance to chlorine for both the standard and improved membranes. Comparing the flux and rejection of the membranes before and after chlorine exposure revealed a minor variation, suggesting the membrane's ability to resist surface damage from chlorine. Hence, through the creation of innovative MgFe2O4/CA and OH–MgFe2O4/CA membranes, the identified constraints of RO membranes were effectively addressed. One of the synthesized RO membranes, OH–MgFe2O4/CA, demonstrated superior performance in permeate flux, rejection, anti-fouling, and chlorine resistance when compared to MgFe2O4/CA membranes. Furthermore, the stability of the synthesized membranes was assessed through tensile strength testing, which confirmed the preservation of the membrane structure.
{"title":"An efficient approach in water desalination using high flux induced magnetic-field hydroxyl-functionalized MgFe2O4 /CA RO membranes with organic/inorganic fouling control capability","authors":"Fariba Oulad , Ali Akbar Zinatizadeh , Sirus Zinadini , Amir Razmjou","doi":"10.1016/j.memsci.2024.123437","DOIUrl":"10.1016/j.memsci.2024.123437","url":null,"abstract":"<div><div>Reverse osmosis (RO) membranes are crucial for water purification and desalination, facing challenges like balancing permeate flux and rejection, dealing with membrane fouling, and chlorine resistance. This study focuses on developing new membranes using cellulose acetate (CA) polymers and magnetic nanoparticles of magnesium ferrite (MgFe<sub>2</sub>O<sub>4</sub>) and hydroxyl-functionalized magnesium ferrite (OH–MgFe<sub>2</sub>O<sub>4</sub>) through a phase inversion method, with and without the presence of a magnetic field, to address the limitations of RO membranes. This study conducted a unique experiment where magnetic nanoparticles migrated to the membrane surface and underwent phase exchange in the coagulation bath under the influence of a 2.0 T magnetic field. As a result, the magnetic nanoparticles were arranged in a specific pattern and evenly spread across the membrane surface, enhancing the membrane's surface characteristics and hydrophilic properties. Furthermore, the flux of the synthesized membranes experienced an increase when exposed to the magnetic field, while maintaining a consistently high rejection rate. An evaluation was conducted on the membranes' resistance to organic fouling from bovine serum albumin (BSA), inorganic fouling from scaling, and the combined effects of BSA and scaling. Based on the findings, the membranes showed a notable enhancement in their anti-fouling properties, particularly when exposed to a magnetic field. An assessment was conducted on the resistance to chlorine for both the standard and improved membranes. Comparing the flux and rejection of the membranes before and after chlorine exposure revealed a minor variation, suggesting the membrane's ability to resist surface damage from chlorine. Hence, through the creation of innovative MgFe<sub>2</sub>O<sub>4</sub>/CA and OH–MgFe<sub>2</sub>O<sub>4</sub>/CA membranes, the identified constraints of RO membranes were effectively addressed. One of the synthesized RO membranes, OH–MgFe<sub>2</sub>O<sub>4</sub>/CA, demonstrated superior performance in permeate flux, rejection, anti-fouling, and chlorine resistance when compared to MgFe<sub>2</sub>O<sub>4</sub>/CA membranes. Furthermore, the stability of the synthesized membranes was assessed through tensile strength testing, which confirmed the preservation of the membrane structure.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123437"},"PeriodicalIF":8.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535015","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 : 2024-10-22DOI: 10.1016/j.memsci.2024.123441
Xiaoxia Sun , Bin Wang , Qingshan Liu , Congjie Gao , Jia Xu
Application of unrefined crude salt not only leads to a serious equipment scaling and a low product quality, but also increases operational risks and poses health hazards. Therefore, it is essential to refine crude salt prior to its use. However, traditional methods of crude salt refinement are energy-intensive and probably produce additional chemical by-products. In this work, membrane technology was used to accomplish the refinement of crude salt due to its unique characteristics, such as environmentally friendly and lower energy consumption. To improve the separation performance, the membranes were fabricated by simply adjusting the aqueous monomer concentration. For single-salt feed, the membrane (M10) prepared with a high ratio of 10 exhibited excellent salt rejection due to the formation of a thicker and denser PA layer. And it owned a superior MgCl2/NaCl selectivity of ∼22.0, demonstrating that the membrane can achieve outstanding selectivity for mono-/divalent ions. The selectivity of Mg2+/Na+ increased to ∼23.5 for bi-salt feed and further improved to 66.2 for multi-salt feed due to the stronger charge shielding effect. Most importantly, the membrane was also successfully applied in the refinement of crude salt. When using crude salt (NaCl 30 g/L, purity 0.90) as feed, the M10 exhibited both excellent retention of bivalent ions and permeation of univalent ions, resulting in the corresponding Mg2+/Na+ selectivity up to ∼251.6 and the tremendous enhancement in the Na + purity of ∼0.997. This work offers a feasible strategy for crude salt refinement, and could expand to some other potential applications such as resource utilization in the salinization industry and zero-liquid discharge of industrial wastewater.
{"title":"Chloride-salt separation type nanofiltration membranes for efficient crude salt refinement","authors":"Xiaoxia Sun , Bin Wang , Qingshan Liu , Congjie Gao , Jia Xu","doi":"10.1016/j.memsci.2024.123441","DOIUrl":"10.1016/j.memsci.2024.123441","url":null,"abstract":"<div><div>Application of unrefined crude salt not only leads to a serious equipment scaling and a low product quality, but also increases operational risks and poses health hazards. Therefore, it is essential to refine crude salt prior to its use. However, traditional methods of crude salt refinement are energy-intensive and probably produce additional chemical by-products. In this work, membrane technology was used to accomplish the refinement of crude salt due to its unique characteristics, such as environmentally friendly and lower energy consumption. To improve the separation performance, the membranes were fabricated by simply adjusting the aqueous monomer concentration. For single-salt feed, the membrane (M<sub>10</sub>) prepared with a high ratio of 10 exhibited excellent salt rejection due to the formation of a thicker and denser PA layer. And it owned a superior MgCl<sub>2</sub>/NaCl selectivity of ∼22.0, demonstrating that the membrane can achieve outstanding selectivity for mono-/divalent ions. The selectivity of Mg<sup>2+</sup>/Na<sup>+</sup> increased to ∼23.5 for bi-salt feed and further improved to 66.2 for multi-salt feed due to the stronger charge shielding effect. Most importantly, the membrane was also successfully applied in the refinement of crude salt. When using crude salt (NaCl 30 g/L, purity 0.90) as feed, the M<sub>10</sub> exhibited both excellent retention of bivalent ions and permeation of univalent ions, resulting in the corresponding Mg<sup>2+</sup>/Na<sup>+</sup> selectivity up to ∼251.6 and the tremendous enhancement in the Na <sup>+</sup> purity of ∼0.997. This work offers a feasible strategy for crude salt refinement, and could expand to some other potential applications such as resource utilization in the salinization industry and zero-liquid discharge of industrial wastewater.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"715 ","pages":"Article 123441"},"PeriodicalIF":8.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660181","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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