Jiandong Wang, Yuxing Jiang, Zhuangzhuang Tian, Jun Li, Yang Jin, Jianjun Chen, Yubin Wang
{"title":"磷酸净化用高渗透性稳酸聚磺胺脲纳滤膜","authors":"Jiandong Wang, Yuxing Jiang, Zhuangzhuang Tian, Jun Li, Yang Jin, Jianjun Chen, Yubin Wang","doi":"10.1016/j.seppur.2025.131662","DOIUrl":null,"url":null,"abstract":"<div><div>The traditional wet-process phosphoric acid has higher economic benefits than the thermal-process phosphoric acid, but introduces many metal ion impurities, which limits the application of phosphoric acid. In highly concentrated phosphoric acid solutions, phosphoric acid mainly exists in molecular form. Due to the surface charge and appropriate pore size of the nanofiltration (NF) membrane, it exhibits high selectivity for phosphoric acid and its impurities. However, because of the uncontrolled diffusion of monomers and rapid polymerization, the pore size distribution becomes highly uneven. Meanwhile the extremely low pH and high viscosity of the phosphoric acid compromise the stability and permeance of commercial membranes. We identified that the organic monomer benzene-1,3-disulfonyl chloride (BDSC) exhibits a capping effect when reacting with the aqueous phase of branched polyethyleneimine (PEI) which allows the newly formed membrane to regulate the subsequent diffusion and reaction of hexamethylene diisocyanate (HDI), thereby optimizing the membrane structure. By adjusting the concentration of BDSC, the pore size of the membrane layer was optimized. The final average pore size was determined to be 0.33 nm. The membrane exhibited an average ion rejection of over 65 % when tested in a 20 wt% P<sub>2</sub>O<sub>5</sub> solution, while maintaining a very low rejection rate of only 1.74 % for phosphorus. The permeance reached 1.21 L/h m<sup>2</sup> bar, surpassing that of traditional commercial membrane operating at less than 1 L/h m<sup>2</sup> bar under 10 wt% P<sub>2</sub>O<sub>5</sub> conditions. This study employed the capping effect to adjust the membrane structure and pore size, demonstrating that spatial sieving is the main mechanism for ions purification in phosphoric acid. Long-term acid resistance tests confirmed the stability of<!--> <!-->the poly (sulfonamide-urea) NF membrane during phosphoric acid purification process. This work shows that this new nanofiltration membrane exhibits promising prospects for application within acidic high-viscosity systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131662"},"PeriodicalIF":9.0000,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Highly permeable acid-stable poly (sulfonamide-urea) nanofiltration membrane for purifying phosphoric acid\",\"authors\":\"Jiandong Wang, Yuxing Jiang, Zhuangzhuang Tian, Jun Li, Yang Jin, Jianjun Chen, Yubin Wang\",\"doi\":\"10.1016/j.seppur.2025.131662\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The traditional wet-process phosphoric acid has higher economic benefits than the thermal-process phosphoric acid, but introduces many metal ion impurities, which limits the application of phosphoric acid. In highly concentrated phosphoric acid solutions, phosphoric acid mainly exists in molecular form. Due to the surface charge and appropriate pore size of the nanofiltration (NF) membrane, it exhibits high selectivity for phosphoric acid and its impurities. However, because of the uncontrolled diffusion of monomers and rapid polymerization, the pore size distribution becomes highly uneven. Meanwhile the extremely low pH and high viscosity of the phosphoric acid compromise the stability and permeance of commercial membranes. We identified that the organic monomer benzene-1,3-disulfonyl chloride (BDSC) exhibits a capping effect when reacting with the aqueous phase of branched polyethyleneimine (PEI) which allows the newly formed membrane to regulate the subsequent diffusion and reaction of hexamethylene diisocyanate (HDI), thereby optimizing the membrane structure. By adjusting the concentration of BDSC, the pore size of the membrane layer was optimized. The final average pore size was determined to be 0.33 nm. The membrane exhibited an average ion rejection of over 65 % when tested in a 20 wt% P<sub>2</sub>O<sub>5</sub> solution, while maintaining a very low rejection rate of only 1.74 % for phosphorus. The permeance reached 1.21 L/h m<sup>2</sup> bar, surpassing that of traditional commercial membrane operating at less than 1 L/h m<sup>2</sup> bar under 10 wt% P<sub>2</sub>O<sub>5</sub> conditions. This study employed the capping effect to adjust the membrane structure and pore size, demonstrating that spatial sieving is the main mechanism for ions purification in phosphoric acid. Long-term acid resistance tests confirmed the stability of<!--> <!-->the poly (sulfonamide-urea) NF membrane during phosphoric acid purification process. This work shows that this new nanofiltration membrane exhibits promising prospects for application within acidic high-viscosity systems.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"362 \",\"pages\":\"Article 131662\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-01-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S138358662500259X\",\"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":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S138358662500259X","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}
The traditional wet-process phosphoric acid has higher economic benefits than the thermal-process phosphoric acid, but introduces many metal ion impurities, which limits the application of phosphoric acid. In highly concentrated phosphoric acid solutions, phosphoric acid mainly exists in molecular form. Due to the surface charge and appropriate pore size of the nanofiltration (NF) membrane, it exhibits high selectivity for phosphoric acid and its impurities. However, because of the uncontrolled diffusion of monomers and rapid polymerization, the pore size distribution becomes highly uneven. Meanwhile the extremely low pH and high viscosity of the phosphoric acid compromise the stability and permeance of commercial membranes. We identified that the organic monomer benzene-1,3-disulfonyl chloride (BDSC) exhibits a capping effect when reacting with the aqueous phase of branched polyethyleneimine (PEI) which allows the newly formed membrane to regulate the subsequent diffusion and reaction of hexamethylene diisocyanate (HDI), thereby optimizing the membrane structure. By adjusting the concentration of BDSC, the pore size of the membrane layer was optimized. The final average pore size was determined to be 0.33 nm. The membrane exhibited an average ion rejection of over 65 % when tested in a 20 wt% P2O5 solution, while maintaining a very low rejection rate of only 1.74 % for phosphorus. The permeance reached 1.21 L/h m2 bar, surpassing that of traditional commercial membrane operating at less than 1 L/h m2 bar under 10 wt% P2O5 conditions. This study employed the capping effect to adjust the membrane structure and pore size, demonstrating that spatial sieving is the main mechanism for ions purification in phosphoric acid. Long-term acid resistance tests confirmed the stability of the poly (sulfonamide-urea) NF membrane during phosphoric acid purification process. This work shows that this new nanofiltration membrane exhibits promising prospects for application within acidic high-viscosity systems.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.