Pub Date : 2025-02-25DOI: 10.1016/j.memsci.2025.123912
Tianliang Xiao , Wang Yu , Xuejiang Li , Zhaoyue Liu , Bingxin Lu , Wenwei Lei , Jin Zhai
The application of biomimetic nanofluidic nanochannels for the harvest of osmotic energy has attracted considerable interest in recent years. However, there exists a lack in the comprehensive understanding of how geometric parameters similar to the complex configurations of biological counterparts affect the conversion of osmotic energy. In this paper, theoretical models are developed based upon Poisson-Nernst-Planck equations to simulate the performance of nanochannel membranes in generating osmotic power. The results reveal that employing asymmetric nanochannels results in enhanced cation selectively with the transference number increasing from 0.71 to 0.82. Furthermore, shortening the length of nanochannels can improve power generation performance. Various nanochannel configurations are designed to investigate the influence on output characteristics, in which the maximum power increases from 0.84 to 1.41 fW. The model predictions are further verified by experimental data based on nanofluidic devices. These findings provide valuable insights for the development of efficient osmotic energy harvesting devices.
{"title":"Multilevel geometric optimization in nanochannel membranes for osmotic energy conversion","authors":"Tianliang Xiao , Wang Yu , Xuejiang Li , Zhaoyue Liu , Bingxin Lu , Wenwei Lei , Jin Zhai","doi":"10.1016/j.memsci.2025.123912","DOIUrl":"10.1016/j.memsci.2025.123912","url":null,"abstract":"<div><div>The application of biomimetic nanofluidic nanochannels for the harvest of osmotic energy has attracted considerable interest in recent years. However, there exists a lack in the comprehensive understanding of how geometric parameters similar to the complex configurations of biological counterparts affect the conversion of osmotic energy. In this paper, theoretical models are developed based upon Poisson-Nernst-Planck equations to simulate the performance of nanochannel membranes in generating osmotic power. The results reveal that employing asymmetric nanochannels results in enhanced cation selectively with the transference number increasing from 0.71 to 0.82. Furthermore, shortening the length of nanochannels can improve power generation performance. Various nanochannel configurations are designed to investigate the influence on output characteristics, in which the maximum power increases from 0.84 to 1.41 fW. The model predictions are further verified by experimental data based on nanofluidic devices. These findings provide valuable insights for the development of efficient osmotic energy harvesting devices.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123912"},"PeriodicalIF":8.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143519375","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.memsci.2025.123901
Zhen Lu , Xingming Wu , Baixue Liu , Zhenyu Yang , Yatao Zhang , Wenheng Jing , Shi-Peng Sun , Junyong Zhu
Highly permeable nanofiltration membranes comprising selective polyamide nanofilms hold significant promise for energy-efficient molecule/ion separations. However, current polyamide-based nanofiltration membranes, made through polymerization between highly reactive piperazine and triacyl chloride, exhibiting high retention of divalent salts, limiting their applicability for molecule/ion separations such as dye or antibiotics desalination. Herein, we report the fabrication of a loosely nanostructured poly(bipiperidine-amide) membrane via dorsal coating interfacial polymerization (DC-IP) using Kevlar hydrogel as porous support. The hydrogen-bonding and electrostatic interaction between bipiperidine and Kevlar hydrogel play a role in the formation of winkled ring-shaped nanostructures, which effectively enhance water transport area. By employing 4,4′-bipiperidine, a nonplanar monomer with a longer reaction size distance, the resulting membranes exhibited higher free volume and stronger pore connectivity compared to poly(piperazine-amide) counterparts, as evidenced by both experimental and simulation analyses. The impact of monomer concentration and solution pH on the DC-IP parameters influencing membrane separation performance was thoroughly investigated. Importantly, the optimized polyamide membranes demonstrated an exceptional water permeance of 70.1 L m−2 h−1 bar−1, high dye removal efficiency (Congo red, 99.4 %), and low divalent salt rejection (Na2SO4, 38.6 %). Furthermore, the membranes exhibited high antifouling capability and long-term operational stability, rendering them highly promising for rapid and durable dye/salt separations. This study underscores the potential of utilizing moderately reactive bipiperidine to fabricate high-porosity polyamide membranes for fast molecule/ion separation.
{"title":"Loosely nanostructured polyamide membranes with rapid water transport for efficient molecule/ion separation","authors":"Zhen Lu , Xingming Wu , Baixue Liu , Zhenyu Yang , Yatao Zhang , Wenheng Jing , Shi-Peng Sun , Junyong Zhu","doi":"10.1016/j.memsci.2025.123901","DOIUrl":"10.1016/j.memsci.2025.123901","url":null,"abstract":"<div><div>Highly permeable nanofiltration membranes comprising selective polyamide nanofilms hold significant promise for energy-efficient molecule/ion separations. However, current polyamide-based nanofiltration membranes, made through polymerization between highly reactive piperazine and triacyl chloride, exhibiting high retention of divalent salts, limiting their applicability for molecule/ion separations such as dye or antibiotics desalination. Herein, we report the fabrication of a loosely nanostructured poly(bipiperidine-amide) membrane via dorsal coating interfacial polymerization (DC-IP) using Kevlar hydrogel as porous support. The hydrogen-bonding and electrostatic interaction between bipiperidine and Kevlar hydrogel play a role in the formation of winkled ring-shaped nanostructures, which effectively enhance water transport area. By employing 4,4′-bipiperidine, a nonplanar monomer with a longer reaction size distance, the resulting membranes exhibited higher free volume and stronger pore connectivity compared to poly(piperazine-amide) counterparts, as evidenced by both experimental and simulation analyses. The impact of monomer concentration and solution pH on the DC-IP parameters influencing membrane separation performance was thoroughly investigated. Importantly, the optimized polyamide membranes demonstrated an exceptional water permeance of 70.1 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>, high dye removal efficiency (Congo red, 99.4 %), and low divalent salt rejection (Na<sub>2</sub>SO<sub>4</sub>, 38.6 %). Furthermore, the membranes exhibited high antifouling capability and long-term operational stability, rendering them highly promising for rapid and durable dye/salt separations. This study underscores the potential of utilizing moderately reactive bipiperidine to fabricate high-porosity polyamide membranes for fast molecule/ion separation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123901"},"PeriodicalIF":8.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478728","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.memsci.2025.123899
Junjie Zhu , Wei Xu , Yuwei Yang , Xiaomei Su , Xiao Xiao , Feng Dong , Hailu Fu , Chongjun Chen , Jianrong Chen , Faqian Sun
Membrane bioreactor (MBR) has been widely applied in landfill leachate treatment, with significant efforts focusing on sustainable and non-toxic strategies for biofouling mitigation. This study investigated the potential of the quorum quenching (QQ) bacterium Brucella sp. ZJ1 to control biofouling in a MBR system treating landfill leachate. Results demonstrate that QQ-MBR extended the time to reach a transmembrane pressure of 35 kPa by 3∼10-fold compared with the control. After being operated in MBR for 40 days, QQ beads retained about 40 % of their quorum sensing (QS) signals degradation activity. Biofouling reduction was driven by surface scouring, alongside a notable QQ effect, evidenced by 27–41 % lower extracellular polymeric substance (EPS) concentrations and 60 % lower QS signal levels. Metagenomic analysis revealed that QQ beads significantly reduced QS-related and EPS production genes while increasing QQ-related genes in the membrane biocake, effectively mitigating biofouling. This study highlighted the role of QQ in reshaping the microbial community to sustainably reduce biofouling in landfill leachate MBR treatment.
{"title":"Quorum quenching driven microbial community to biofouling control in membrane bioreactor for landfill leachate treatment","authors":"Junjie Zhu , Wei Xu , Yuwei Yang , Xiaomei Su , Xiao Xiao , Feng Dong , Hailu Fu , Chongjun Chen , Jianrong Chen , Faqian Sun","doi":"10.1016/j.memsci.2025.123899","DOIUrl":"10.1016/j.memsci.2025.123899","url":null,"abstract":"<div><div>Membrane bioreactor (MBR) has been widely applied in landfill leachate treatment, with significant efforts focusing on sustainable and non-toxic strategies for biofouling mitigation. This study investigated the potential of the quorum quenching (QQ) bacterium <em>Brucella</em> sp. ZJ1 to control biofouling in a MBR system treating landfill leachate. Results demonstrate that QQ-MBR extended the time to reach a transmembrane pressure of 35 kPa by 3∼10-fold compared with the control. After being operated in MBR for 40 days, QQ beads retained about 40 % of their quorum sensing (QS) signals degradation activity. Biofouling reduction was driven by surface scouring, alongside a notable QQ effect, evidenced by 27–41 % lower extracellular polymeric substance (EPS) concentrations and 60 % lower QS signal levels. Metagenomic analysis revealed that QQ beads significantly reduced QS-related and EPS production genes while increasing QQ-related genes in the membrane biocake, effectively mitigating biofouling. This study highlighted the role of QQ in reshaping the microbial community to sustainably reduce biofouling in landfill leachate MBR treatment.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123899"},"PeriodicalIF":8.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509824","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.memsci.2025.123900
Nathalie Lenaerts , Rhea Verbeke , Douglas M. Davenport , Scout Caspers , Samuel Eyley , Karim-Alexandros Kantre , Alexander Volodine , Ricardo Helm , Maik Butterling , Maciej Oskar Liedke , Andreas Wagner , Wim Thielemans , Johan Meersschaut , Marcel Dickmann , Ivo F.J. Vankelecom
The drive to expand the implementation of membrane separation technology towards harsher environments prompted the development of chemically robust epoxide-based TFC membranes. This work seeks to better understand the influence of the support on epoxide-based TFC membrane performance and properties. More specifically, it investigates the impact of porous PAN support layers of different porosities and pore sizes on the formation of poly(epoxyether) (PEE) thin films via interfacial initiation of polymerization (IIP), and their more cross-linked and more charged PEE counterparts (XL-PEE) arising from a subsequent post-treatment step. A systematic study was conducted using a series of supports with pore sizes varying from 20 nm to 90 nm and porosities in the range of 4% to 10%, while maintaining identical synthesis conditions for the selective layer. The physicochemical properties of the selective layer were characterized in-depth with X-ray photoelectron spectroscopy (XPS), elastic recoil detection (ERD), transmission electron microscopy (TEM), positron annihilation lifetime spectroscopy (PALS), and atomic force microscopy (AFM) to elucidate the synthesis-structure-performance relationship. PEE TFC membranes comprising these supports had a broad range in water permeances of 5 – 30 L m−2 h−1 bar−1 with consistent methyl orange (327.33 g mol−1) rejections of ca. 90%. The densified XL-PEE TFC membranes all achieved ca. 65% NaCl rejections, again independent of the support properties. In contrast, more porous supports resulted in more permeable TFC membranes, which can be attributed to the so-called funnel effect. Additionally, the solvent used to prepare the support layers through non-solvent induced phase separation also impacted the selective layer by affecting the interfacial properties during IIP. This work thus demonstrates that the support can serve as an easy tool to fine-tune the performance of the next-generation of high-performance epoxide-based TFC membranes.
{"title":"Influence of support pore size and porosity on epoxide-based TFC membranes","authors":"Nathalie Lenaerts , Rhea Verbeke , Douglas M. Davenport , Scout Caspers , Samuel Eyley , Karim-Alexandros Kantre , Alexander Volodine , Ricardo Helm , Maik Butterling , Maciej Oskar Liedke , Andreas Wagner , Wim Thielemans , Johan Meersschaut , Marcel Dickmann , Ivo F.J. Vankelecom","doi":"10.1016/j.memsci.2025.123900","DOIUrl":"10.1016/j.memsci.2025.123900","url":null,"abstract":"<div><div>The drive to expand the implementation of membrane separation technology towards harsher environments prompted the development of chemically robust epoxide-based TFC membranes. This work seeks to better understand the influence of the support on epoxide-based TFC membrane performance and properties. More specifically, it investigates the impact of porous PAN support layers of different porosities and pore sizes on the formation of poly(epoxyether) (PEE) thin films via interfacial initiation of polymerization (IIP), and their more cross-linked and more charged PEE counterparts (XL-PEE) arising from a subsequent post-treatment step. A systematic study was conducted using a series of supports with pore sizes varying from 20 nm to 90 nm and porosities in the range of 4% to 10%, while maintaining identical synthesis conditions for the selective layer. The physicochemical properties of the selective layer were characterized in-depth with X-ray photoelectron spectroscopy (XPS), elastic recoil detection (ERD), transmission electron microscopy (TEM), positron annihilation lifetime spectroscopy (PALS), and atomic force microscopy (AFM) to elucidate the synthesis-structure-performance relationship. PEE TFC membranes comprising these supports had a broad range in water permeances of 5 – 30 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> with consistent methyl orange (327.33 g mol<sup>−1</sup>) rejections of ca. 90%. The densified XL-PEE TFC membranes all achieved ca. 65% NaCl rejections, again independent of the support properties. In contrast, more porous supports resulted in more permeable TFC membranes, which can be attributed to the so-called funnel effect. Additionally, the solvent used to prepare the support layers through non-solvent induced phase separation also impacted the selective layer by affecting the interfacial properties during IIP. This work thus demonstrates that the support can serve as an easy tool to fine-tune the performance of the next-generation of high-performance epoxide-based TFC membranes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123900"},"PeriodicalIF":8.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143552084","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 : 2025-02-21DOI: 10.1016/j.memsci.2025.123897
Shiwei Tian , Yaqi Zhang , Qiankun Sha , Yixuan Wang , Xingxiang Zhang , Xuhuan Yan , Na Han
Polyphenylene sulfide (PPS) membrane materials have attracted significant attention for separating oily wastewater due to their remarkable separation precision and permeation capability. Nevertheless, the inherent hydrophobic characteristics result in a single wetting property, which restricts their broad applicability in treating diverse types of oily wastewater. In this study, the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes exhibit outstanding under-liquid dual superlyophobicity, which were formed via constructing a composite coating containing polyphenol-polycation and calcium alginate (CaAlg) hydrogel, and assembling ZIF-8 nanocrystals with suitable surface chemistry. Through the solvent pre-wetting approach, the surface wettability of the PPS composite membranes can be flexibly transitioned between under-water superoleophobicity and under-oil superhydrophobicity, thus realizing on-demand separation of oily wastewater. It is noteworthy that the treatment efficiency of the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes for the various oil-water mixtures (surfactant-free) and emulsions (stabilized by surfactants) attained greater than 98.1 %. Meanwhile, the rapid transport capability of diverse types of oil-water emulsions can also be exhibited, with a permeance of 1652.4 L m−2 h−1 bar−1 for water-in-oil (W/O) emulsions and 2087.5 L m−2 h−1 bar−1 for oil-in-water (O/W) emulsions. In addition, the PPS composite membranes demonstrated outstanding anti-fouling capacity, recyclability, and switchable separation capacity. This work extended the utilization of the PPS membrane material in the controllable treatment of oily wastewater.
{"title":"PPS/TA-PEI/CaAlg/ZIF-8 composite membranes with under-liquid dual superlyophobicity for on-demand separation of oil-water emulsions","authors":"Shiwei Tian , Yaqi Zhang , Qiankun Sha , Yixuan Wang , Xingxiang Zhang , Xuhuan Yan , Na Han","doi":"10.1016/j.memsci.2025.123897","DOIUrl":"10.1016/j.memsci.2025.123897","url":null,"abstract":"<div><div>Polyphenylene sulfide (PPS) membrane materials have attracted significant attention for separating oily wastewater due to their remarkable separation precision and permeation capability. Nevertheless, the inherent hydrophobic characteristics result in a single wetting property, which restricts their broad applicability in treating diverse types of oily wastewater. In this study, the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes exhibit outstanding under-liquid dual superlyophobicity, which were formed via constructing a composite coating containing polyphenol-polycation and calcium alginate (CaAlg) hydrogel, and assembling ZIF-8 nanocrystals with suitable surface chemistry. Through the solvent pre-wetting approach, the surface wettability of the PPS composite membranes can be flexibly transitioned between under-water superoleophobicity and under-oil superhydrophobicity, thus realizing on-demand separation of oily wastewater. It is noteworthy that the treatment efficiency of the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes for the various oil-water mixtures (surfactant-free) and emulsions (stabilized by surfactants) attained greater than 98.1 %. Meanwhile, the rapid transport capability of diverse types of oil-water emulsions can also be exhibited, with a permeance of 1652.4 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> for water-in-oil (W/O) emulsions and 2087.5 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> for oil-in-water (O/W) emulsions. In addition, the PPS composite membranes demonstrated outstanding anti-fouling capacity, recyclability, and switchable separation capacity. This work extended the utilization of the PPS membrane material in the controllable treatment of oily wastewater.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123897"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509288","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}
High-performance thin-film composite (TFC) nanofiltration (NF) membranes featuring suitable pore size and appropriate charge density are critical for achieving high ion selectivity. Herein, a secondary interfacial polymerization (SIP) strategy was proposed to prepare TFC NF membrane with dual-polyamide (PA) layer structure using polyethylenimine (PEI) and piperazine (PIP) as aqueous monomers in sequence. The first PEI-PA layer with a smoother surface and uniform pore size distribution serves as an interlayer for the SIP, contributing to the uniform distribution of PIP monomers and producing a controllable regulation of the SIP reaction. The resultant NF membrane featured thinner thickness, smoother surface, denser pore size, and asymmetric charge properties, achieving greater than 99 % rejections of five heavy metals (Cu2+, Mn2+, Zn2+, Ni2+, Co2+) during mixed salts solution filtration test at concentration range of 100–2000 mg L−1. More importantly, the unique dual-PA layer NF membrane achieved an excellent selectivity of Li+ and Mg2+of 79.1 under the combined effects of pore size exclusion and charge repulsion. Interestingly, its pure water permeance (13.5 L m−2 h−1 bar−1) was increased by about 35 % due to the “gutter effect” between the bilayers in comparison with the monolayer PA membrane. Moreover, the transition state theory was introduced to analyze the partition and diffusion energy barriers of salts during filtration. Our work demonstrates that the SIP strategy is promising for realizing ultra-high solute-selective NF membrane.
{"title":"Novel insight into dual-polyamide layer composite nanofiltration membrane toward enhanced ion selective performance","authors":"Cunxian Lai , Wentian Zhang , Lichao Xia , Fangang Meng , Shanshan Zhao","doi":"10.1016/j.memsci.2025.123895","DOIUrl":"10.1016/j.memsci.2025.123895","url":null,"abstract":"<div><div>High-performance thin-film composite (TFC) nanofiltration (NF) membranes featuring suitable pore size and appropriate charge density are critical for achieving high ion selectivity. Herein, a secondary interfacial polymerization (SIP) strategy was proposed to prepare TFC NF membrane with dual-polyamide (PA) layer structure using polyethylenimine (PEI) and piperazine (PIP) as aqueous monomers in sequence. The first PEI-PA layer with a smoother surface and uniform pore size distribution serves as an interlayer for the SIP, contributing to the uniform distribution of PIP monomers and producing a controllable regulation of the SIP reaction. The resultant NF membrane featured thinner thickness, smoother surface, denser pore size, and asymmetric charge properties, achieving greater than 99 % rejections of five heavy metals (Cu<sup>2+</sup>, Mn<sup>2+</sup>, Zn<sup>2+</sup>, Ni<sup>2+</sup>, Co<sup>2+</sup>) during mixed salts solution filtration test at concentration range of 100–2000 mg L<sup>−1</sup>. More importantly, the unique dual-PA layer NF membrane achieved an excellent selectivity of Li<sup>+</sup> and Mg<sup>2+</sup>of 79.1 under the combined effects of pore size exclusion and charge repulsion. Interestingly, its pure water permeance (13.5 L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>) was increased by about 35 % due to the “gutter effect” between the bilayers in comparison with the monolayer PA membrane. Moreover, the transition state theory was introduced to analyze the partition and diffusion energy barriers of salts during filtration. Our work demonstrates that the SIP strategy is promising for realizing ultra-high solute-selective NF membrane.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123895"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509825","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 : 2025-02-21DOI: 10.1016/j.memsci.2025.123885
Zongwu Zhang , Ziqian Xiang , Fengjin Qu , Jun Wang , Hua Yang , Jun Li , Barbara Mecheri , Alessandra D'Epifanio , Tengjiao Ou , Fang Chen , Xiaoyan Ma
Both chemical compositions of ionomers and surface properties of nanofillers significantly impact the performances of composite proton exchange membranes (PEMs) for water electrolysis. Despite progress in optimizing the chemical compositions of ionomers, it remains challenging to rationally modulate the micro/nano interface between nanofillers and ionomers due to the undesirable surface functionalization of nanofillers. In this study, core-shell silica@poly(1-vinylimidazole) (SiO2@PVI) nanoparticles with tunable grafting densities are fabricated via sonochemical technique and incorporated into sulfonated polysulfone (SPSF60) ionomer. The SiO2@PVI nanoparticles strengthen the interfacial hydrogen bond with SPSF60 by elevating the surface tethered imidazole groups, yielding a customizable interfacial network that further boosts the proton conductivity and stability of SPSF60/SiO2@PVI membranes. As a result, integrating the SPSF60/SiO2@PVI-12C membrane into a water electrolyzer achieves an exceptional operating current density of 5.84 A/cm2 at 2.0 V and 80 °C, which is 31.2 % higher than that with pure SPSF60. Moreover, the electrolyzer's durability is doubled due to the enhanced stability of the modified membrane. This study underscores the critical role of ionomer/filler interfacial structure on properties of composite PEMs, presenting an effective strategy to enhance the performance of proton exchange membranes for water electrolysis through interface modulation.
{"title":"Sulfonated polysulfone composite membranes with tailored interfacial hydrogen bond network for efficient proton exchange membrane water electrolysis","authors":"Zongwu Zhang , Ziqian Xiang , Fengjin Qu , Jun Wang , Hua Yang , Jun Li , Barbara Mecheri , Alessandra D'Epifanio , Tengjiao Ou , Fang Chen , Xiaoyan Ma","doi":"10.1016/j.memsci.2025.123885","DOIUrl":"10.1016/j.memsci.2025.123885","url":null,"abstract":"<div><div>Both chemical compositions of ionomers and surface properties of nanofillers significantly impact the performances of composite proton exchange membranes (PEMs) for water electrolysis. Despite progress in optimizing the chemical compositions of ionomers, it remains challenging to rationally modulate the micro/nano interface between nanofillers and ionomers due to the undesirable surface functionalization of nanofillers. In this study, core-shell silica@poly(1-vinylimidazole) (SiO<sub>2</sub>@PVI) nanoparticles with tunable grafting densities are fabricated via sonochemical technique and incorporated into sulfonated polysulfone (SPSF60) ionomer. The SiO<sub>2</sub>@PVI nanoparticles strengthen the interfacial hydrogen bond with SPSF60 by elevating the surface tethered imidazole groups, yielding a customizable interfacial network that further boosts the proton conductivity and stability of SPSF60/SiO<sub>2</sub>@PVI membranes. As a result, integrating the SPSF60/SiO<sub>2</sub>@PVI-12C membrane into a water electrolyzer achieves an exceptional operating current density of 5.84 A/cm<sup>2</sup> at 2.0 V and 80 °C, which is 31.2 % higher than that with pure SPSF60. Moreover, the electrolyzer's durability is doubled due to the enhanced stability of the modified membrane. This study underscores the critical role of ionomer/filler interfacial structure on properties of composite PEMs, presenting an effective strategy to enhance the performance of proton exchange membranes for water electrolysis through interface modulation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123885"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509823","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 : 2025-02-21DOI: 10.1016/j.memsci.2025.123887
Simone Colantoni , Guillaume Pillot , Sofia Cvoro , Sven Kerzenmacher , Óscar Santiago
This study presents the successful preparation of a novel chemically modified Cellophane separator with polydimethylsiloxane (PDMS) for potential use in microbial electrolysis cells (MECs) with real anaerobic digester effluent (ADE). The modified separator was assessed against commercial materials, including anion exchange membrane (AEM), cation exchange membrane (CEM), and unmodified Cellophane. They were evaluated in a conventional two-chamber electrolysis cell, serving as a surrogate for a MEC, and in a bioreactor to assess biofouling. The modified Cellophane demonstrated potential for reducing costs and enhancing separator performance. Cellophane, Cellophane + PDMS and AEM effectively prevented pH imbalances, maintaining stable anode pH levels above 7 without cathode alkalinization. However, the CEM was unsuitable due to excessive pH splitting (Δ6 pH) and elevated resistance. The study highlighted the pronounced impact of using real ADE on overpotentials and resistances of all separators. Organic acid crossover occurred across all materials, with Cellophane exhibiting higher rates (0.16–0.2 mg m−2 s−1) than CEM and AEM (0.04–0.1 mg m−2 s−1). An extensive investigation into biofouling and degradation under anaerobic digestion conditions revealed that unmodified Cellophane degraded completely within a month, whereas PDMS modification extended its durability to two months before complete disintegration occurred.
{"title":"Evaluation of separators for potential use in microbial electrolysis cells under anaerobic digester conditions","authors":"Simone Colantoni , Guillaume Pillot , Sofia Cvoro , Sven Kerzenmacher , Óscar Santiago","doi":"10.1016/j.memsci.2025.123887","DOIUrl":"10.1016/j.memsci.2025.123887","url":null,"abstract":"<div><div>This study presents the successful preparation of a novel chemically modified Cellophane separator with polydimethylsiloxane (PDMS) for potential use in microbial electrolysis cells (MECs) with real anaerobic digester effluent (ADE). The modified separator was assessed against commercial materials, including anion exchange membrane (AEM), cation exchange membrane (CEM), and unmodified Cellophane. They were evaluated in a conventional two-chamber electrolysis cell, serving as a surrogate for a MEC, and in a bioreactor to assess biofouling. The modified Cellophane demonstrated potential for reducing costs and enhancing separator performance. Cellophane, Cellophane + PDMS and AEM effectively prevented pH imbalances, maintaining stable anode pH levels above 7 without cathode alkalinization. However, the CEM was unsuitable due to excessive pH splitting (Δ6 pH) and elevated resistance. The study highlighted the pronounced impact of using real ADE on overpotentials and resistances of all separators. Organic acid crossover occurred across all materials, with Cellophane exhibiting higher rates (0.16–0.2 mg m<sup>−2</sup> s<sup>−1</sup>) than CEM and AEM (0.04–0.1 mg m<sup>−2</sup> s<sup>−1</sup>). An extensive investigation into biofouling and degradation under anaerobic digestion conditions revealed that unmodified Cellophane degraded completely within a month, whereas PDMS modification extended its durability to two months before complete disintegration occurred.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123887"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143519376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-21DOI: 10.1016/j.memsci.2025.123881
Qian Yang , Lin Cao , Ling Tan , Jing Li , Shanshan Zhao , Miao Tian
Interfacial polymerization (IP) has been extensively utilized for fabrication of polyamide (PA) membranes. The PA selective layer synthesized via IP typically exhibits a ridge and valley loose upper layer and dense lower layer, leading to issues such as membrane fouling and flux decline due to contaminant adhesion and passage. Previous studies have been devoted to addressing the perm-selectivity trade-off in PA, with little attention paid to tuning the PA structure in gradient to control membrane permeance and selectivity and investigate its impact on fouling resistance. In this study, the crosslinking structure of the PA selective layer in gradient was regulated by modulating the internal structure of sodium alginate (SA) by pre-crosslinking with Ca2+, producing a pyramid membrane (Ca/SA-0.04) with a dense upper layer and a looser lower layer. The dense upper PA layer effectively retains salt, achieving a NaCl rejection of 99.10 %. The loose lower layer, formed by the interwoven crosslinking of PA and SA, provided high salt water flux (1.08 Lm−2h−1bar−1) due to the ease of the Ca/SA chains de-crosslinking in NaCl solution, outperforming conventional prepared membranes by 46.57 %. Additionally, in fouling tests, the Ca/SA-0.04 membrane demonstrated excellent anti-fouling performance against Humic acid and Bovine Serum Albumin, with a flux decline rate below 17 % and a flux recovery rate exceeding 93 %. Our study proposes an innovative strategy for designing PA RO membranes with superior perm-selectivity and anti-fouling efficiency.
{"title":"Design of gradient polyamide membrane for anti-fouling high-performance reverse osmosis desalination","authors":"Qian Yang , Lin Cao , Ling Tan , Jing Li , Shanshan Zhao , Miao Tian","doi":"10.1016/j.memsci.2025.123881","DOIUrl":"10.1016/j.memsci.2025.123881","url":null,"abstract":"<div><div>Interfacial polymerization (IP) has been extensively utilized for fabrication of polyamide (PA) membranes. The PA selective layer synthesized via IP typically exhibits a ridge and valley loose upper layer and dense lower layer, leading to issues such as membrane fouling and flux decline due to contaminant adhesion and passage. Previous studies have been devoted to addressing the perm-selectivity trade-off in PA, with little attention paid to tuning the PA structure in gradient to control membrane permeance and selectivity and investigate its impact on fouling resistance. In this study, the crosslinking structure of the PA selective layer in gradient was regulated by modulating the internal structure of sodium alginate (SA) by pre-crosslinking with Ca<sup>2+</sup>, producing a pyramid membrane (Ca/SA-0.04) with a dense upper layer and a looser lower layer. The dense upper PA layer effectively retains salt, achieving a NaCl rejection of 99.10 %. The loose lower layer, formed by the interwoven crosslinking of PA and SA, provided high salt water flux (1.08 Lm<sup>−2</sup>h<sup>−1</sup>bar<sup>−1</sup>) due to the ease of the Ca/SA chains de-crosslinking in NaCl solution, outperforming conventional prepared membranes by 46.57 %. Additionally, in fouling tests, the Ca/SA-0.04 membrane demonstrated excellent anti-fouling performance against Humic acid and Bovine Serum Albumin, with a flux decline rate below 17 % and a flux recovery rate exceeding 93 %. Our study proposes an innovative strategy for designing PA RO membranes with superior perm-selectivity and anti-fouling efficiency.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123881"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509826","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 : 2025-02-21DOI: 10.1016/j.memsci.2025.123886
Song Liu , Qianqian Liu , Yun Cai , Xuemei Bao , Wenyao Zhou , Yang Yang
Combining membrane ultrafiltration with adsorption and advanced oxidation processes is considered to be an efficient strategy to improve removal capacity, alleviate membrane fouling and extend membrane lifespan for the treatment of wastewater with complex organic pollutants. The removal efficiency of small-molecule pollutants is closely related to the amount of adsorption sites, which is limited with the loading level of adsorbents. Herein, we proposed a blending-to-entrapping two-step method to load spherical resorcinol-formaldehyde (RF) resins, a metal-free photocatalyst with phenolic hydroxyl groups on surface, utmost possibly in the polyethersulfone (PES) membrane for removing small-molecule cationic pollutants from aqueous solution in an ultrafiltration process. By entrapping adequate RF resin microspheres in the finger-like pores of a PES ultrafiltration (UF) membrane blended with the RF resin microspheres, the obtained membrane possessed ultrafiltration and adsorption simultaneously based on pore size exclusion effect and electrostatic attraction, respectively. Owning to the photocatalytic in situ H2O2 production ability of RF resins, the membrane also showed good reusability through a visible-light-induced self-cleaning process based on Fenton reaction. This work provides a feasible strategy to construct renewable adsorptive composite UF membranes for complex wastewater treatment.
{"title":"Functionalized ultrafiltration membrane with complementary adsorption and self-cleaning performances by blending-to-entrapping modification","authors":"Song Liu , Qianqian Liu , Yun Cai , Xuemei Bao , Wenyao Zhou , Yang Yang","doi":"10.1016/j.memsci.2025.123886","DOIUrl":"10.1016/j.memsci.2025.123886","url":null,"abstract":"<div><div>Combining membrane ultrafiltration with adsorption and advanced oxidation processes is considered to be an efficient strategy to improve removal capacity, alleviate membrane fouling and extend membrane lifespan for the treatment of wastewater with complex organic pollutants. The removal efficiency of small-molecule pollutants is closely related to the amount of adsorption sites, which is limited with the loading level of adsorbents. Herein, we proposed a blending-to-entrapping two-step method to load spherical resorcinol-formaldehyde (RF) resins, a metal-free photocatalyst with phenolic hydroxyl groups on surface, utmost possibly in the polyethersulfone (PES) membrane for removing small-molecule cationic pollutants from aqueous solution in an ultrafiltration process. By entrapping adequate RF resin microspheres in the finger-like pores of a PES ultrafiltration (UF) membrane blended with the RF resin microspheres, the obtained membrane possessed ultrafiltration and adsorption simultaneously based on pore size exclusion effect and electrostatic attraction, respectively. Owning to the photocatalytic <em>in situ</em> H<sub>2</sub>O<sub>2</sub> production ability of RF resins, the membrane also showed good reusability through a visible-light-induced self-cleaning process based on Fenton reaction. This work provides a feasible strategy to construct renewable adsorptive composite UF membranes for complex wastewater treatment.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123886"},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143487560","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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