Pub Date : 2025-01-01DOI: 10.1016/j.advmem.2025.100142
Wenwen Dong , Jiahui Yan , Taotao Ji , Mingming Wu , Kunpeng Yu , Yi Liu , Wenjing Hu , Yi Liu
Zirconium-based MOF membranes exhibit significant potential in energy-efficient desalination. Nevertheless, framework defect elimination, which represents an effective protocol to enhance their molecular sieving capacity and operation stability, remains highly challenging to date. In this study, we proposed a framework defect patching strategy to prepare robust UiO-66-NH2 membrane with Zr6O4(OH)4(OAc)12 cluster source towards high-efficiency desalination. Ion sieving results indicated that increasing reaction temperature and ratio of ligand to Zr6O4(OH)4(OAc)12 cluster contributed to framework defect elimination. UiO-66-NH2 membranes prepared under optimized conditions exhibited superior metal ion rejection rate (Al3+: 97.7 %) and operation stability over 20 days. Particularly, their water/NaCl separation performance well exceeded majority of reported polycrystalline 3D membranes, offering promising prospects for modulating molecular diffusion kinetics in MOF pores.
{"title":"Eliminating lattice defects in UiO-66-NH2 membrane towards high-precision desalination","authors":"Wenwen Dong , Jiahui Yan , Taotao Ji , Mingming Wu , Kunpeng Yu , Yi Liu , Wenjing Hu , Yi Liu","doi":"10.1016/j.advmem.2025.100142","DOIUrl":"10.1016/j.advmem.2025.100142","url":null,"abstract":"<div><div>Zirconium-based MOF membranes exhibit significant potential in energy-efficient desalination. Nevertheless, framework defect elimination, which represents an effective protocol to enhance their molecular sieving capacity and operation stability, remains highly challenging to date. In this study, we proposed a framework defect patching strategy to prepare robust UiO-66-NH<sub>2</sub> membrane with Zr<sub>6</sub>O<sub>4</sub>(OH)<sub>4</sub>(OAc)<sub>12</sub> cluster source towards high-efficiency desalination. Ion sieving results indicated that increasing reaction temperature and ratio of ligand to Zr<sub>6</sub>O<sub>4</sub>(OH)<sub>4</sub>(OAc)<sub>12</sub> cluster contributed to framework defect elimination. UiO-66-NH<sub>2</sub> membranes prepared under optimized conditions exhibited superior metal ion rejection rate (Al<sup>3+</sup>: 97.7 %) and operation stability over 20 days. Particularly, their water/NaCl separation performance well exceeded majority of reported polycrystalline 3D membranes, offering promising prospects for modulating molecular diffusion kinetics in MOF pores.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100142"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.advmem.2025.100172
Yixin Wang , Yingda Huang , Kang Geng , Bin Hu , Ruofei Gao , Erqiang Yang , Junfen Li , Jiandang Xue , Nanwen Li
Anion exchange membrane (AEM) is a core component of potentially more efficient and cost-effective anion exchange membrane water electrolyzers (AEMWEs), which combine the advantages of traditional alkaline water electrolyzers (AWEs) and proton exchange membrane water electrolyzers (PEMWEs). Despite extensive research efforts in recent years, AEMs still face significant challenges, particularly insufficient alkaline stability and limited dimensional/mechanical stability. In this work, we enhanced the mechanical and alkaline stability of AEMs by incorporating the thermoplastic elastomer polystyrene-block-polybutadiene-block-polystyrene (SBS) into the poly (terphenyl piperidinium) (PTP) matrix. The optimal PTP-SBS-2.5 % membrane exhibits outstanding dimensional stability (9.4 % swelling at 20 °C), robust mechanical properties (tensile strength of 51.5 MPa and elongation of 63.1 % at break in wet state), low alkali absorption (0.875 %) and exceptional alkaline stability (92.4 % conductivity retention after 1500 h). Notably, the membrane demonstrates stable operation in AEMWE for over 3000 h with a low voltage decay rate of 41.1 μV h−1. These results highlight the significance of SBS in enhancing both the alkaline stability and mechanical performance of PTP-based AEMs.
阴离子交换膜（AEM）结合了传统碱性水电解槽（awe）和质子交换膜水电解槽（PEMWEs）的优点，是具有更高效率和成本效益的阴离子交换膜水电解槽（AEMWEs）的核心部件。尽管近年来进行了广泛的研究，但AEMs仍然面临着重大挑战，特别是碱性稳定性不足和尺寸/机械稳定性有限。在这项工作中，我们通过将热塑性弹性体聚苯乙烯-嵌段聚丁二烯-嵌段聚苯乙烯（SBS）加入聚terphenyl胡椒啶（PTP）基体中来提高AEMs的机械稳定性和碱性稳定性。最佳的ptp - sbs - 2.5%膜具有出色的尺寸稳定性（在20°C时溶胀率为9.4%），良好的机械性能（湿态断裂时拉伸强度为51.5 MPa，伸长率为63.1%），低碱吸收率（0.875%）和优异的碱稳定性（1500 h后电导率保持率为92.4%）。值得注意的是，该膜在AEMWE中稳定运行超过3000 h，电压衰减率为41.1 μV h−1。这些结果突出了SBS在提高ptp基AEMs的碱性稳定性和力学性能方面的重要意义。
{"title":"Mechanically robust and chemically stable poly(aryl piperidinium)-SBS copolymer anion exchange membranes for 3000-h durable alkaline water electrolyzers","authors":"Yixin Wang , Yingda Huang , Kang Geng , Bin Hu , Ruofei Gao , Erqiang Yang , Junfen Li , Jiandang Xue , Nanwen Li","doi":"10.1016/j.advmem.2025.100172","DOIUrl":"10.1016/j.advmem.2025.100172","url":null,"abstract":"<div><div>Anion exchange membrane (AEM) is a core component of potentially more efficient and cost-effective anion exchange membrane water electrolyzers (AEMWEs), which combine the advantages of traditional alkaline water electrolyzers (AWEs) and proton exchange membrane water electrolyzers (PEMWEs). Despite extensive research efforts in recent years, AEMs still face significant challenges, particularly insufficient alkaline stability and limited dimensional/mechanical stability. In this work, we enhanced the mechanical and alkaline stability of AEMs by incorporating the thermoplastic elastomer polystyrene-block-polybutadiene-block-polystyrene (SBS) into the poly (terphenyl piperidinium) (PTP) matrix. The optimal PTP-SBS-2.5 % membrane exhibits outstanding dimensional stability (9.4 % swelling at 20 °C), robust mechanical properties (tensile strength of 51.5 MPa and elongation of 63.1 % at break in wet state), low alkali absorption (0.875 %) and exceptional alkaline stability (92.4 % conductivity retention after 1500 h). Notably, the membrane demonstrates stable operation in AEMWE for over 3000 h with a low voltage decay rate of 41.1 μV h<sup>−1</sup>. These results highlight the significance of SBS in enhancing both the alkaline stability and mechanical performance of PTP-based AEMs.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100172"},"PeriodicalIF":9.5,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145120843","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.advmem.2025.100137
Shihang Wei , Anqi Fu , Huaying Li , Wenyi Dong , Feiyun Sun , Hongjie Wang , Ding Yu Xing , Yuexing Wang
The treatment of landfill leachate concentrate poses significant environmental challenges, particularly in the separation and recovery of valuable humic substances from high salt concentrations. In this study, a novel loose nanofiltration (LNF) membrane was fabricated using 0.5 wt% triethanolamine (TEOA) and 0.1 wt% trimesoyl chloride (TMC) via interfacial polymerization for the accurate separation of humic substances from inorganic salts in landfill leachate concentrate. The optimized TEOA membrane exhibited high permeate flux about 67.6 L m−2 h−1·bar−1 and over 90 % transmission for ions, while achieving the rejection of humic substances above 92 %. The effects of operating conditions were investigated. Results showed that increasing inorganic salt concentration led to a notable decrease in inorganic salt rejection due to intensified concentration polarization and weakened electrostatic interactions. Rising humic substance concentration further intensified membrane fouling and concentration polarization, resulting in reduced flux and increased humic substance and inorganic salt rejections. Higher temperatures and alkaline pH increased flux and maintained stable rejections. In addition, a two-stage membrane filtration process was subsequently applied to actual landfill leachate concentrate samples. The humic substance concentration was enriched from 1.5 to 37.4 g L−1, achieving a recovery rate over 60 % at a concentration factor of 12.5. The recovered humic substances complied with the standards of water-soluble fertilizers containing humic-acids (NY1106-2010), highlighting the LNF membrane's potential in sustainable landfill leachate concentrate management and resource recovery.
垃圾填埋场渗滤液浓缩液的处理对环境构成重大挑战，特别是在从高浓度盐中分离和回收有价值的腐殖质物质方面。本研究以0.5 wt%的三乙醇胺（TEOA）和0.1 wt%的三甲基氯（TMC）为原料，通过界面聚合制备了一种新型的松散纳滤（LNF）膜，用于准确分离垃圾渗滤液浓缩物中的腐殖质和无机盐。优化后的TEOA膜具有较高的渗透通量，约为67.6 L m−2 h−1·bar−1，离子透过率超过90%，腐殖质截留率达到92%以上。考察了操作条件的影响。结果表明：随着无机盐浓度的增加，由于浓度极化加剧，静电相互作用减弱，无机盐截留率显著降低；腐殖质浓度的升高进一步加剧了膜污染和浓度极化，导致通量降低，腐殖质和无机盐的丢弃量增加。较高的温度和碱性pH值增加了通量并保持了稳定的排出物。此外，随后将两级膜过滤工艺应用于实际的垃圾渗滤液浓缩液样品。腐殖质浓度从1.5 g L−1富集到37.4 g L−1，在12.5的浓度系数下，回收率达到60%以上。回收的腐植酸物质符合含腐植酸水溶性肥料标准（NY1106-2010），突出了LNF膜在垃圾渗滤液浓缩液可持续管理和资源回收方面的潜力。
{"title":"Accurate separation and recovery of humic substances from landfill leachate concentrate by triethanolamine-based loose nanofiltration membranes","authors":"Shihang Wei , Anqi Fu , Huaying Li , Wenyi Dong , Feiyun Sun , Hongjie Wang , Ding Yu Xing , Yuexing Wang","doi":"10.1016/j.advmem.2025.100137","DOIUrl":"10.1016/j.advmem.2025.100137","url":null,"abstract":"<div><div>The treatment of landfill leachate concentrate poses significant environmental challenges, particularly in the separation and recovery of valuable humic substances from high salt concentrations. In this study, a novel loose nanofiltration (LNF) membrane was fabricated using 0.5 wt% triethanolamine (TEOA) and 0.1 wt% trimesoyl chloride (TMC) via interfacial polymerization for the accurate separation of humic substances from inorganic salts in landfill leachate concentrate. The optimized TEOA membrane exhibited high permeate flux about 67.6 L m<sup>−2</sup> h<sup>−1</sup>·bar<sup>−1</sup> and over 90 % transmission for ions, while achieving the rejection of humic substances above 92 %. The effects of operating conditions were investigated. Results showed that increasing inorganic salt concentration led to a notable decrease in inorganic salt rejection due to intensified concentration polarization and weakened electrostatic interactions. Rising humic substance concentration further intensified membrane fouling and concentration polarization, resulting in reduced flux and increased humic substance and inorganic salt rejections. Higher temperatures and alkaline pH increased flux and maintained stable rejections. In addition, a two-stage membrane filtration process was subsequently applied to actual landfill leachate concentrate samples. The humic substance concentration was enriched from 1.5 to 37.4 g L<sup>−1</sup>, achieving a recovery rate over 60 % at a concentration factor of 12.5. The recovered humic substances complied with the standards of water-soluble fertilizers containing humic-acids (NY1106-2010), highlighting the LNF membrane's potential in sustainable landfill leachate concentrate management and resource recovery.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100137"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143593665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.advmem.2025.100150
Zhibin Ma , Peitong Lian , Jie Li , Yanxiong Ren , Yonghui Shi , Hanze Ma , Yuhang Guo , Qianfeng Pan , Sheng Yuan , Yutong Wang , Heyang Liu , Lixuan Liu , Yuao Dong , Yanlei Su , Jing Zhao , Quanfu An , Guangwei He , Zhongyi Jiang
Polydimethylsiloxane (PDMS) membranes are commonly utilized for ethanol-water separation. However, the separation performance is insufficient owing to the inherent trade-off between permeability and selectivity. In this study, we reported the incorporation of methyl-functionalized covalent organic framework (COF, TpBD-CH3) into PDMS membranes to prepare mixed matrix membranes (MMMs), greatly increasing ethanol flux by 2.7 times. Under testing conditions of 60 °C with a feed solution containing 5 wt% ethanol in water, the permeation flux of the membrane incorporating 0.1 wt% TpBD-CH3 significantly increased from 1738 g/(m2·h) to 4648 g/(m2·h) compared to the original PDMS membrane, while the separation factor improved from 7.32 to 8.40. The improved separation performance is attributed to that the incorporation of the COF enhances the hydrophobicity as well as the free volume cavities of the membranes as evidenced by the significantly increased gas permeability (CO2 permeability reaches 26,720 Barrer). This study indicates the potential of COF in the development of PDMS-based MMMs for the separation of organic aqueous solutions or gas components.
{"title":"Mixed matrix membranes by incorporating methyl-functionalized covalent organic framework into PDMS for high flux ethanol/water separation","authors":"Zhibin Ma , Peitong Lian , Jie Li , Yanxiong Ren , Yonghui Shi , Hanze Ma , Yuhang Guo , Qianfeng Pan , Sheng Yuan , Yutong Wang , Heyang Liu , Lixuan Liu , Yuao Dong , Yanlei Su , Jing Zhao , Quanfu An , Guangwei He , Zhongyi Jiang","doi":"10.1016/j.advmem.2025.100150","DOIUrl":"10.1016/j.advmem.2025.100150","url":null,"abstract":"<div><div>Polydimethylsiloxane (PDMS) membranes are commonly utilized for ethanol-water separation. However, the separation performance is insufficient owing to the inherent trade-off between permeability and selectivity. In this study, we reported the incorporation of methyl-functionalized covalent organic framework (COF, TpBD-CH<sub>3</sub>) into PDMS membranes to prepare mixed matrix membranes (MMMs), greatly increasing ethanol flux by 2.7 times. Under testing conditions of 60 °C with a feed solution containing 5 wt% ethanol in water, the permeation flux of the membrane incorporating 0.1 wt% TpBD-CH<sub>3</sub> significantly increased from 1738 g/(m<sup>2</sup>·h) to 4648 g/(m<sup>2</sup>·h) compared to the original PDMS membrane, while the separation factor improved from 7.32 to 8.40. The improved separation performance is attributed to that the incorporation of the COF enhances the hydrophobicity as well as the free volume cavities of the membranes as evidenced by the significantly increased gas permeability (CO<sub>2</sub> permeability reaches 26,720 Barrer). This study indicates the potential of COF in the development of PDMS-based MMMs for the separation of organic aqueous solutions or gas components.</div></div>","PeriodicalId":100033,"journal":{"name":"Advanced Membranes","volume":"5 ","pages":"Article 100150"},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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