Xiaoyang Liu , Na Zhang , Zhen Dong , Jifu Du , Lifang Peng , Long Zhao , Miao Yang
{"title":"利用辐射诱导raft介导接枝聚合技术制备咪唑离子液体负载二氧化硅材料,高效捕获TcO4-/ReO4-","authors":"Xiaoyang Liu , Na Zhang , Zhen Dong , Jifu Du , Lifang Peng , Long Zhao , Miao Yang","doi":"10.1016/j.seppur.2025.131442","DOIUrl":null,"url":null,"abstract":"<div><div>Technetium (<sup>99</sup>Tc) is a main long-lived radionuclide of nuclear waste, which poses a great threat to the environment and human health. The reasonable disposal of <sup>99</sup>Tc is vital important. In this paper, a series of novel materials (SMILR<sub>m</sub>, m = 0, 1/500, 1/200, m is the molar ratio of IL to RAFT reagent) was synthesized by radiation-induced grafting combined with reversible addition-fragmentation chain transfer (RAFT) polymerization. The adsorption performance of SMILR<sub>m</sub> to <sup>99</sup>Tc were investigated. The graft polymerization process is controlled by the RAFT reagent, resulting in a restricted dispersion of SMILR<sub>m</sub> molecular weight. With the increase of RAFT reagent content, the grafting yield (GY) decreased. The addition of RAFT reagent increases the specific surface area of the adsorbent, accelerates the adsorption rate, increases the adsorption capacity, but reduces the adsorption selectivity. Especially, the adsorption of SMILR<sub>0</sub> was a single step adsorption and obeyed Langmuir adsorption model, while SMILR<sub>m</sub> (1/500, 1/200) showed a stepwise adsorption isotherm model. SMILR<sub>m</sub> exhibited excellent recyclability and could efficiently capture <span><math><mrow><mtext>Re</mtext><msubsup><mtext>O</mtext><mrow><mtext>4</mtext></mrow><mo>-</mo></msubsup></mrow></math></span> from a simulated Beishan groundwater in dynamic experiments. Finally, XPS and FT-IR analysis confirmed that the adsorption was an ion exchange mechanism. The results showed that SMILR<sub>m</sub> are suitable for the effective removal of <span><math><mrow><mtext>Re</mtext><msubsup><mtext>O</mtext><mrow><mtext>4</mtext></mrow><mo>-</mo></msubsup><mo>/</mo><mi>T</mi><mi>c</mi><msubsup><mi>O</mi><mrow><mn>4</mn></mrow><mo>-</mo></msubsup></mrow></math></span> from radioactive wastewater with complex composition.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"361 ","pages":"Article 131442"},"PeriodicalIF":9.0000,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Highly efficient capture of TcO4-/ReO4- by imidazolium ionic liquid supported silica materials prepared by radiation induced RAFT-mediated graft polymerization technology\",\"authors\":\"Xiaoyang Liu , Na Zhang , Zhen Dong , Jifu Du , Lifang Peng , Long Zhao , Miao Yang\",\"doi\":\"10.1016/j.seppur.2025.131442\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Technetium (<sup>99</sup>Tc) is a main long-lived radionuclide of nuclear waste, which poses a great threat to the environment and human health. The reasonable disposal of <sup>99</sup>Tc is vital important. In this paper, a series of novel materials (SMILR<sub>m</sub>, m = 0, 1/500, 1/200, m is the molar ratio of IL to RAFT reagent) was synthesized by radiation-induced grafting combined with reversible addition-fragmentation chain transfer (RAFT) polymerization. The adsorption performance of SMILR<sub>m</sub> to <sup>99</sup>Tc were investigated. The graft polymerization process is controlled by the RAFT reagent, resulting in a restricted dispersion of SMILR<sub>m</sub> molecular weight. With the increase of RAFT reagent content, the grafting yield (GY) decreased. The addition of RAFT reagent increases the specific surface area of the adsorbent, accelerates the adsorption rate, increases the adsorption capacity, but reduces the adsorption selectivity. Especially, the adsorption of SMILR<sub>0</sub> was a single step adsorption and obeyed Langmuir adsorption model, while SMILR<sub>m</sub> (1/500, 1/200) showed a stepwise adsorption isotherm model. SMILR<sub>m</sub> exhibited excellent recyclability and could efficiently capture <span><math><mrow><mtext>Re</mtext><msubsup><mtext>O</mtext><mrow><mtext>4</mtext></mrow><mo>-</mo></msubsup></mrow></math></span> from a simulated Beishan groundwater in dynamic experiments. Finally, XPS and FT-IR analysis confirmed that the adsorption was an ion exchange mechanism. The results showed that SMILR<sub>m</sub> are suitable for the effective removal of <span><math><mrow><mtext>Re</mtext><msubsup><mtext>O</mtext><mrow><mtext>4</mtext></mrow><mo>-</mo></msubsup><mo>/</mo><mi>T</mi><mi>c</mi><msubsup><mi>O</mi><mrow><mn>4</mn></mrow><mo>-</mo></msubsup></mrow></math></span> from radioactive wastewater with complex composition.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"361 \",\"pages\":\"Article 131442\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-01-04\",\"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/S1383586625000395\",\"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/S1383586625000395","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}
引用次数: 0
摘要
锝(99Tc)是核废料中主要的长寿命放射性核素,对环境和人类健康构成极大威胁。99Tc的合理处置至关重要。本文采用辐射诱导接枝结合可逆加成-破碎链转移(RAFT)聚合的方法合成了一系列新型材料(SMILRm, m = 0,1 /500,1/200,m为IL与RAFT试剂的摩尔比)。研究了SMILRm对99Tc的吸附性能。接枝聚合过程由RAFT试剂控制,导致SMILRm分子量的分散受到限制。随着RAFT试剂含量的增加,接枝收率(GY)降低。RAFT试剂的加入增加了吸附剂的比表面积,加快了吸附速率,增加了吸附容量,但降低了吸附选择性。其中,SMILR0的吸附为单步吸附,服从Langmuir吸附模型,而SMILRm(1/ 500,1 /200)的吸附为逐步等温吸附模型。在动态实验中,SMILRm具有良好的可回收性,可有效捕获模拟北山地下水中的ReO4-ReO4-。最后,通过XPS和FT-IR分析证实了吸附是一种离子交换机制。结果表明,SMILRm适用于复杂成分放射性废水中ReO4-/TcO4- -ReO4-/TcO4-的有效去除。
Highly efficient capture of TcO4-/ReO4- by imidazolium ionic liquid supported silica materials prepared by radiation induced RAFT-mediated graft polymerization technology
Technetium (99Tc) is a main long-lived radionuclide of nuclear waste, which poses a great threat to the environment and human health. The reasonable disposal of 99Tc is vital important. In this paper, a series of novel materials (SMILRm, m = 0, 1/500, 1/200, m is the molar ratio of IL to RAFT reagent) was synthesized by radiation-induced grafting combined with reversible addition-fragmentation chain transfer (RAFT) polymerization. The adsorption performance of SMILRm to 99Tc were investigated. The graft polymerization process is controlled by the RAFT reagent, resulting in a restricted dispersion of SMILRm molecular weight. With the increase of RAFT reagent content, the grafting yield (GY) decreased. The addition of RAFT reagent increases the specific surface area of the adsorbent, accelerates the adsorption rate, increases the adsorption capacity, but reduces the adsorption selectivity. Especially, the adsorption of SMILR0 was a single step adsorption and obeyed Langmuir adsorption model, while SMILRm (1/500, 1/200) showed a stepwise adsorption isotherm model. SMILRm exhibited excellent recyclability and could efficiently capture from a simulated Beishan groundwater in dynamic experiments. Finally, XPS and FT-IR analysis confirmed that the adsorption was an ion exchange mechanism. The results showed that SMILRm are suitable for the effective removal of from radioactive wastewater with complex composition.
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.