Chuiko Institute of Surface Chemistry of National Academy of Sciences of Ukraine , 17 General Naumov Street, 03164 Kyiv, Ukraine.
KTH Royal Institute of Technology , Teknikringen 56-58, SE-100 44 Stockholm, Sweden.
ACS Appl Mater Interfaces. 2018 Feb 21;10(7):6681-6693. doi: 10.1021/acsami.7b17594. Epub 2018 Feb 8.
A new imidazol-2yl-phosphonic acid/mesoporous silica sorbent (ImP(O)(OH)/SiO) was developed and applied for uranium(VI) ion removal from aqueous solutions. The synthesized material was characterized by fast kinetics and an extra-high adsorption capacity with respect to uranium. The highest adsorption efficiency of U(VI) ions was obtained for the reaction system at pH 4 and exceeded 618 mg/g. The uranium(VI) sorption proceeds quickly in the first step within 60 min of the adsorbent sites and ion interactions. Moreover, the equilibrium time was determined to be 120 min. The equilibrium and kinetic characteristics of the uranium(VI) ions uptake by synthesized sorbent was found to follow the Langmuir-Freundlich isotherm model and pseudo-second-order kinetics rather than the Langmuir, Dubinin-Radushkevich, and Temkin models and pseudo-first-order or intraparticle diffusion sorption kinetics. The adsorption mechanism for uranium on the sorbent was clarified basing on the X-ray photoelectron spectroscopy (XPS) analysis. The model of UO binding to surface of the sorbent was proposed according to the results of XPS, i.e., a 1:1 U-to-P ratio in the sorbed complex was established. The regeneration study confirms the ImP(O)(OH)/SiO sorbent can be reused. A total of 45% of uranium ions was determined as originating from the sorbent leaching in the acidic solutions, whereas when the basic solutions were used, the removal efficiency was 12%.
一种新型的咪唑-2-基膦酸/介孔硅吸附剂(ImP(O)(OH)/SiO)被开发出来,并应用于从水溶液中去除铀(VI)离子。所合成的材料具有快速动力学和超高的铀吸附容量的特点。在 pH 值为 4 的反应体系中,U(VI)离子的吸附效率最高,超过 618mg/g。铀(VI)离子的吸附在第一个步骤中很快进行,在 60 分钟内达到吸附剂位点和离子相互作用的最高效率。此外,平衡时间确定为 120 分钟。合成吸附剂对铀(VI)离子的吸附平衡和动力学特性符合 Langmuir-Freundlich 等温线模型和准二级动力学,而不是 Langmuir、Dubinin-Radushkevich 和 Temkin 模型以及准一级或内扩散吸附动力学。基于 X 射线光电子能谱(XPS)分析,阐明了铀在吸附剂上的吸附机理。根据 XPS 的结果,提出了UO 与吸附剂表面结合的模型,即在吸附复合物中建立了 U 与 P 的 1:1 比例。再生研究证实了 ImP(O)(OH)/SiO 吸附剂可以重复使用。在酸性溶液中,确定有 45%的铀离子来自于吸附剂的浸出,而在使用碱性溶液时,去除效率为 12%。