Chang Ziyong, Li Fangxu, Qi Xiaoyue, Jiang Bo, Kou Jue, Sun Chunbao
Civil and Resource Engineering School, University of Science and Technology Beijing, Beijing, 100083, China.
Guangdong Institute of Resources Comprehensive Utilization, 363 Changxing Road, Guangzhou, 510650, China; State Key Laboratory of Rare Metals Separation and Comprehensive Utilization, 363 Changxing Road, Guangzhou, 510650, China.
J Hazard Mater. 2020 Jun 5;391:122175. doi: 10.1016/j.jhazmat.2020.122175. Epub 2020 Jan 22.
Recycling precious metals from secondary resources is of great environmental and economic significance. In this study, the Zr-based MOFs UiO-66-NH was synthesized and used to adsorb Au (III) in aqueous solution. The ultrafine particle size (∼50 nm), excellent crystallinity and huge specific surface area (1039.2 m ·g) were verified by transmission electron microscope (TEM), powder X-ray diffraction (PXRD) and surface area analysis. About 50 % Au (III) was adsorbed within 6 min and the maximum adsorption capacity at 298 K reached up to 650 mg·g, showing superiority to traditional adsorbents. The general order kinetics model and Liu equation were suitable to describe the adsorption process, which was spontaneous, endothermic and driven by the increasing system entropy. Electrostatic attraction between -NH and Au (III) anions and inner complexation to Zr-OH played a vital role in adsorption. Au (Ⅲ) was reduced to Au° by amino groups via redox reaction certified by X-ray photoelectron spectroscopy (XPS), PXRD and high-resolution transmission electron microscopy (HRTEM) analysis. Moreover, UiO-66-NH displayed high selectivity, robust stability and excellent reusability, making it an ideal candidate for gold recycling in industrial practice.
从二次资源中回收贵金属具有重大的环境和经济意义。本研究合成了锆基金属有机框架材料UiO-66-NH,并将其用于吸附水溶液中的Au(III)。通过透射电子显微镜(TEM)、粉末X射线衍射(PXRD)和比表面积分析,证实了其具有超细粒径(约50 nm)、优异的结晶度和巨大的比表面积(1039.2 m²·g)。在6分钟内约50%的Au(III)被吸附,298 K时的最大吸附容量高达650 mg·g,显示出优于传统吸附剂的性能。一般的一级动力学模型和刘方程适合描述吸附过程,该过程是自发的、吸热的且由系统熵增加驱动。-NH与Au(III)阴离子之间的静电吸引以及与Zr-OH的内络合作用在吸附中起着至关重要的作用。通过X射线光电子能谱(XPS)、PXRD和高分辨率透射电子显微镜(HRTEM)分析证实,氨基通过氧化还原反应将Au(Ⅲ)还原为Au°。此外,UiO-66-NH表现出高选择性、强稳定性和优异的可重复使用性,使其成为工业实践中黄金回收的理想候选材料。