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Selective recovery of Gd(III) by benzimidazole- and benzoxazole-linked 3D porous polymers
Journal of Water Process Engineering ( IF 6.3 ) Pub Date : 2022-12-10 , DOI: 10.1016/j.jwpe.2022.103378
Lijinhong Huang , Bin Xiao , Lihong Liu , Wenhao Li , Xiaoguang Duan , Wanfu Huang , Chunyan Fan , Yu Dong , Shaomin Liu

Three-dimensional porous benzimidazole- and benzoxazole- linked polymers were successfully prepared through a one-pot method using benzol-1,2,4,5-tetramintetrahydrochlorid (BTD) and 2,5-diamino-1,4-benzediol dihydrochloride (DBD) to react with 4-[tris(4-formyl phenyl)methyl]benzaldehyde (TFPM), respectively. According to nitrogen sorption analysis, TFPM-BTD and TFPM-DBD possessed specific surface areas of 612.60 and 524.90 m2/g, and the total pore volumes (Vtot) of 1.44 and 1.15 cm3/g, respectively. Batch adsorption experiments demonstrated that Gd(III) adsorption processes by TFPM-BTD and TFPM-DBD fit well with the Langmuir isotherm and the pseudo-second-order kinetic model. At 25 °C and pH level of 6, TFPM-BTD showed a much higher adsorption capacity for Gd(III), detected at 173 mg/g, as opposed to TFPM-DBD at 82 mg/g. Associated spectra of N 1s via high-resolution X-ray photoelectron spectroscopy (XPS) revealed the generation of coordination bonds between Gd(III) and (-NH-) of TFPM-BTD polymer during Gd(III) adsorption, while Energy-dispersive X-ray spectroscopy (EDS) analysis proved the uniform adsorption of Gd(III) on TFPM-BTD. TFPM-BTD showed high selectivity toward the adsorption of heavy rare earth ions, in a high-to-low order of Gd3+>Ce3+>Er3+>La3+>Ni2+>Mg2+>Zn2+. Furthermore, TFPM-BTD exhibited excellent cycling stability and regeneration performance. Gd(III) adsorption capacity of TFPM-BTD after five adsorption/elution cycles was retained at 63.9 %. The elution efficiency was extremely high when using 0.1 mol/L hydrochloric acid as the eluent, showing an average five-cycle desorption efficiency over 95 %. The outcomes will provide theoretical and practical guidance to develop high-performance and selective adsorbents for efficient removal of heavy rare earth ions from water.



中文翻译:

苯并咪唑和苯并恶唑连接的 3D 多孔聚合物选择性回收 Gd(III)

三维多孔苯并咪唑-和苯并恶唑-连接的聚合物通过一锅法成功地使用苯并-1,2,4,5-tetramintetrahydrochlorid (BTD) 和 2,5-diamino-1,4-benzediol dihydrochloride (DBD) ) 分别与 4-[三(4-甲酰基苯基)甲基] 苯甲醛 (TFPM) 反应。根据氮吸附分析,TFPM-BTD和TFPM-DBD的比表面积分别为612.60和524.90 m 2 /g,总孔容(V tot )分别为1.44和1.15 cm 3/克,分别。批量吸附实验表明,TFPM-BTD 和 TFPM-DBD 对 Gd(III) 的吸附过程符合 Langmuir 等温线和伪二级动力学模型。在 25 °C 和 pH 值为 6 时,TFPM-BTD 显示出更高的 Gd(III) 吸附能力,检测值为 173 mg/g,而 TFPM-DBD 为 82 mg/g。通过高分辨率 X 射线光电子能谱 (XPS) 获得的 N 1s 相关光谱揭示了在 Gd(III) 吸附过程中,TFPM-BTD 聚合物的 Gd(III) 和 (-NH-) 之间产生了配位键,而能量色散X 射线光谱 (EDS) 分析证明了 Gd(III) 在 TFPM-BTD 上的均匀吸附。TFPM-BTD对重稀土离子具有较高的吸附选择性,从高到低依次为Gd 3+ >Ce 3+ >Er3+ >La 3+ >Ni 2+ >Mg 2+ >Zn 2+。此外,TFPM-BTD表现出优异的循环稳定性和再生性能。五次吸附/洗脱循环后,TFPM-BTD 的 Gd(III) 吸附容量保持在 63.9%。使用0.1 mol/L盐酸作为洗脱液时洗脱效率极高,平均5个循环的脱附效率超过95%。该成果将为开发高性能和选择性吸附剂以有效去除水中的重稀土离子提供理论和实践指导。

更新日期:2022-12-11
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