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羟基磷灰石修饰的富含结合基团的 ZIF-67 复合材料,可从废水中高效高选择性地去除铀(VI)。

Hydroxyapatite modified ZIF-67 composite with abundant binding groups for the highly efficient and selective elimination of uranium (VI) from wastewater.

机构信息

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.

出版信息

J Hazard Mater. 2022 Mar 15;426:127834. doi: 10.1016/j.jhazmat.2021.127834. Epub 2021 Nov 18.

Abstract

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.

摘要

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。

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