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定制NH-UiO-66金属有机框架的不对称结构用于光促进选择性高效金提取与分离

Tailoring the Asymmetric Structure of NH -UiO-66 Metal-Organic Frameworks for Light-promoted Selective and Efficient Gold Extraction and Separation.

作者信息

Cao Jiazhen, Xu Zhenmin, Chen Yao, Li Shuangjun, Jiang Yue, Bai Lele, Yu Han, Li Hexing, Bian Zhenfeng

机构信息

MOE Key Laboratory of Resource Chemistry and Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University, Shanghai, 200234, China.

School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai, 201418, China.

出版信息

Angew Chem Int Ed Engl. 2023 Apr 24;62(18):e202302202. doi: 10.1002/anie.202302202. Epub 2023 Mar 22.

Abstract

Designing adsorption materials with high adsorption capacities and selectivities is highly desirable for precious metal recovery. Desorption performance is also particularly crucial for subsequent precious metal recovery and adsorbent regeneration. Herein, a metal-organic framework (MOF) material (NH -UiO-66) with an asymmetric electronic structure of the central zirconium oxygen cluster has an exceptional gold extraction capacity of 2.04 g g under light irradiation. The selectivity of NH -UiO-66 for gold ions is up to 98.8 % in the presence of interfering ions. Interestingly, the gold ions adsorbed on the surface of NH -UiO-66 spontaneously reduce in situ, undergo nucleation and growth and finally achieve the phase separation of high-purity gold particles from NH -UiO-66. The desorption and separation efficiency of gold particles from the adsorbent surface reaches 89 %. Theoretical calculations indicate that -NH functions as a dual donor of electrons and protons, and the asymmetric structure of NH -UiO-66 leads to energetically advantageous multinuclear gold capture and desorption. This adsorption material can greatly facilitate the recovery of gold from wastewater and can easily realize the recycling of the adsorbent.

摘要

设计具有高吸附容量和选择性的吸附材料对于贵金属回收非常有必要。解吸性能对于后续的贵金属回收和吸附剂再生也尤为关键。在此,一种具有中心锆氧簇不对称电子结构的金属有机框架(MOF)材料(NH -UiO-66)在光照下具有2.04 g g的优异金提取能力。在存在干扰离子的情况下,NH -UiO-66对金离子的选择性高达98.8 %。有趣的是,吸附在NH -UiO-66表面的金离子会原位自发还原,经历成核和生长,最终实现高纯度金颗粒与NH -UiO-66的相分离。金颗粒从吸附剂表面的解吸和分离效率达到89 %。理论计算表明,-NH作为电子和质子的双供体,NH -UiO-66的不对称结构导致在能量上有利于多核金的捕获和解吸。这种吸附材料可以极大地促进从废水中回收金,并能轻松实现吸附剂的循环利用。

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