{"title":"定制l-精氨酸修饰聚哌嗪酰胺纳滤膜,增强透水性,高效分离Li+/Mg2+","authors":"Amir Aghaei, Ahmad Rahimpour, Mohtada Sadrzadeh","doi":"10.1016/j.memsci.2025.124140","DOIUrl":null,"url":null,"abstract":"<div><div>In recent years, there has been a growing focus on lithium recovery from water resources using thin-film composite (TFC) nanofiltration (NF) membranes. In this study, a poly(piperazine-amide) NF membrane was fabricated via interfacial polymerization (IP) between piperazine (PIP) and trimesoyl chloride (TMC) to effectively separate Li<sup>+</sup> from Mg<sup>2+</sup>. However, the trade-off between water permeability and Li<sup>+</sup>/Mg<sup>2+</sup> selectivity presented a challenge, requiring additional surface modification to optimize performance. The surface of the poly(PIP-amide) membrane was modified with ARG amine-based hydrophilic monomer, followed by crosslinking with glutaraldehyde (GLA). The amine groups of ARG are expected to interact with the unreacted acyl chloride groups of TMC, increasing the positive surface charge and thereby improving Li<sup>+</sup>/Mg<sup>2+</sup> selectivity. The membrane modified with ARG and GLA (A2-G0.3) exhibited a significantly improved Li<sup>+</sup>/Mg<sup>2+</sup> selectivity of 17.11, compared to 5.14 for the unmodified membrane when tested in a solution containing 2000 ppm of salts (Li<sup>+</sup>/Mg<sup>2+</sup> of 1:20). Notably, the A2-G0.3 membrane demonstrated a Li<sup>+</sup> rejection of −45.4 and Mg<sup>2+</sup> rejection of 91.5 %, with a water flux of 47.0 Lm<sup>−2</sup>h<sup>−1</sup> at 70 psi. When tested with a simulated brine with a total salt concentration exceeding 21,000 ppm, the membrane exhibited a Li<sup>+</sup> rejection of 9.5 % and Mg<sup>2+</sup> rejection of 90.1 %, along with a water flux of 18.6 Lm<sup>−2</sup>h<sup>−1</sup> at low pressure of 70 psi. The membrane maintained consistent performance over 200 h of simulated feed filtration, demonstrating its long-term stability. Moreover, the antifouling performance of the membrane was greatly improved by grafting the ARG-GLA layer onto its surface. These findings highlight the modified membrane's potential for effective lithium recovery in high-salinity environments.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"728 ","pages":"Article 124140"},"PeriodicalIF":8.4000,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tailored l-Arginine modified Poly(piperazine-amide) nanofiltration membrane with enhanced water permeability for efficient Li+/Mg2+ separation\",\"authors\":\"Amir Aghaei, Ahmad Rahimpour, Mohtada Sadrzadeh\",\"doi\":\"10.1016/j.memsci.2025.124140\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In recent years, there has been a growing focus on lithium recovery from water resources using thin-film composite (TFC) nanofiltration (NF) membranes. In this study, a poly(piperazine-amide) NF membrane was fabricated via interfacial polymerization (IP) between piperazine (PIP) and trimesoyl chloride (TMC) to effectively separate Li<sup>+</sup> from Mg<sup>2+</sup>. However, the trade-off between water permeability and Li<sup>+</sup>/Mg<sup>2+</sup> selectivity presented a challenge, requiring additional surface modification to optimize performance. The surface of the poly(PIP-amide) membrane was modified with ARG amine-based hydrophilic monomer, followed by crosslinking with glutaraldehyde (GLA). The amine groups of ARG are expected to interact with the unreacted acyl chloride groups of TMC, increasing the positive surface charge and thereby improving Li<sup>+</sup>/Mg<sup>2+</sup> selectivity. The membrane modified with ARG and GLA (A2-G0.3) exhibited a significantly improved Li<sup>+</sup>/Mg<sup>2+</sup> selectivity of 17.11, compared to 5.14 for the unmodified membrane when tested in a solution containing 2000 ppm of salts (Li<sup>+</sup>/Mg<sup>2+</sup> of 1:20). Notably, the A2-G0.3 membrane demonstrated a Li<sup>+</sup> rejection of −45.4 and Mg<sup>2+</sup> rejection of 91.5 %, with a water flux of 47.0 Lm<sup>−2</sup>h<sup>−1</sup> at 70 psi. When tested with a simulated brine with a total salt concentration exceeding 21,000 ppm, the membrane exhibited a Li<sup>+</sup> rejection of 9.5 % and Mg<sup>2+</sup> rejection of 90.1 %, along with a water flux of 18.6 Lm<sup>−2</sup>h<sup>−1</sup> at low pressure of 70 psi. The membrane maintained consistent performance over 200 h of simulated feed filtration, demonstrating its long-term stability. Moreover, the antifouling performance of the membrane was greatly improved by grafting the ARG-GLA layer onto its surface. These findings highlight the modified membrane's potential for effective lithium recovery in high-salinity environments.</div></div>\",\"PeriodicalId\":368,\"journal\":{\"name\":\"Journal of Membrane Science\",\"volume\":\"728 \",\"pages\":\"Article 124140\"},\"PeriodicalIF\":8.4000,\"publicationDate\":\"2025-04-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Membrane Science\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0376738825004533\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Membrane Science","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0376738825004533","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Tailored l-Arginine modified Poly(piperazine-amide) nanofiltration membrane with enhanced water permeability for efficient Li+/Mg2+ separation
In recent years, there has been a growing focus on lithium recovery from water resources using thin-film composite (TFC) nanofiltration (NF) membranes. In this study, a poly(piperazine-amide) NF membrane was fabricated via interfacial polymerization (IP) between piperazine (PIP) and trimesoyl chloride (TMC) to effectively separate Li+ from Mg2+. However, the trade-off between water permeability and Li+/Mg2+ selectivity presented a challenge, requiring additional surface modification to optimize performance. The surface of the poly(PIP-amide) membrane was modified with ARG amine-based hydrophilic monomer, followed by crosslinking with glutaraldehyde (GLA). The amine groups of ARG are expected to interact with the unreacted acyl chloride groups of TMC, increasing the positive surface charge and thereby improving Li+/Mg2+ selectivity. The membrane modified with ARG and GLA (A2-G0.3) exhibited a significantly improved Li+/Mg2+ selectivity of 17.11, compared to 5.14 for the unmodified membrane when tested in a solution containing 2000 ppm of salts (Li+/Mg2+ of 1:20). Notably, the A2-G0.3 membrane demonstrated a Li+ rejection of −45.4 and Mg2+ rejection of 91.5 %, with a water flux of 47.0 Lm−2h−1 at 70 psi. When tested with a simulated brine with a total salt concentration exceeding 21,000 ppm, the membrane exhibited a Li+ rejection of 9.5 % and Mg2+ rejection of 90.1 %, along with a water flux of 18.6 Lm−2h−1 at low pressure of 70 psi. The membrane maintained consistent performance over 200 h of simulated feed filtration, demonstrating its long-term stability. Moreover, the antifouling performance of the membrane was greatly improved by grafting the ARG-GLA layer onto its surface. These findings highlight the modified membrane's potential for effective lithium recovery in high-salinity environments.
期刊介绍:
The Journal of Membrane Science is a publication that focuses on membrane systems and is aimed at academic and industrial chemists, chemical engineers, materials scientists, and membranologists. It publishes original research and reviews on various aspects of membrane transport, membrane formation/structure, fouling, module/process design, and processes/applications. The journal primarily focuses on the structure, function, and performance of non-biological membranes but also includes papers that relate to biological membranes. The Journal of Membrane Science publishes Full Text Papers, State-of-the-Art Reviews, Letters to the Editor, and Perspectives.