State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang 330013, China; School of Water Resources & Environmental Engineering, East China University of Technology, Nanchang 330013, China.
Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou 450001, China.
J Hazard Mater. 2022 Mar 15;426:127834. doi: 10.1016/j.jhazmat.2021.127834. Epub 2021 Nov 18.
In this work, nanoscale hydroxyapatite (HAP)-modified ZIF-67 composite, HAP/ZIF-67, with abundant functional groups for uranium(VI) binding was synthesized via a facile ultrasound-assisted synthesis method. The prepared HAP/ZIF-67 was characterized by XRD, SEM, TEM, BET, FT-IR and XPS techniques, and was applied to eliminate uranium(VI) from aqueous solutions under various conditions, i.e., pH, coexisting ions, temperature and contact time. The results indicate that the abundant Co-OH, -CN- and -NH- binding groups originating from the ZIF-67 and the Ca-OH and PO derived from loaded nanoscale HAP synergistically endowed HAP/ZIF-67 with the excellent U(VI) adsorption capacity of 453.1 mg/g, which is 2.55 and 1.78 times that of pristine HAP and ZIF-67. HAP/ZIF-67 showed high adsorption selectivity toward U(VI), and the U(VI) elimination efficiency for real wastewater by HAP/ZIF-67 reached 97.29%. The adsorption kinetics and isotherms were well simulated by the pseudo-second-order model and Langmuir isotherm model, respectively, suggesting that U(VI) adsorption was an endothermic monolayer chemisorption process. The adsorption mechanism of U (VI) by HAP/ZIF-67 was dominated by surface complexation process. This work is expected to provide an effective strategy for developing HAP-modified MOFs absorbent to be used for the highly efficient elimination of radionuclides from wastewater.
在这项工作中,通过简便的超声辅助合成方法合成了纳米羟基磷灰石(HAP)修饰的 ZIF-67 复合材料 HAP/ZIF-67,其具有丰富的用于铀(VI)结合的官能团。通过 XRD、SEM、TEM、BET、FT-IR 和 XPS 技术对制备的 HAP/ZIF-67 进行了表征,并在各种条件下,即 pH、共存离子、温度和接触时间下,将其应用于从水溶液中消除铀(VI)。结果表明,源自 ZIF-67 的丰富的 Co-OH、-CN-和-NH-结合基团以及负载的纳米级 HAP 衍生的 Ca-OH 和 PO 协同赋予 HAP/ZIF-67 具有 453.1 mg/g 的优异 U(VI)吸附能力,是原始 HAP 和 ZIF-67 的 2.55 和 1.78 倍。HAP/ZIF-67 对 U(VI)表现出高吸附选择性,HAP/ZIF-67 对实际废水的 U(VI)去除效率达到 97.29%。吸附动力学和等温线分别通过拟二级模型和 Langmuir 等温线模型很好地模拟,表明 U(VI)吸附是一个吸热的单层化学吸附过程。HAP/ZIF-67 吸附 U(VI)的机制主要是表面络合过程。这项工作有望为开发 HAP 修饰的 MOFs 吸附剂提供一种有效策略,用于从废水中高效去除放射性核素。