College of Environmental Science and Engineering, and Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China.
Guangzhou Association of Circular Economy and Cleaner Production, Guangzhou 510006, China.
J Environ Sci (China). 2023 Feb;124:268-280. doi: 10.1016/j.jes.2021.10.010. Epub 2022 Feb 2.
Zr-based metal-organic frameworks (MOFs) have been developed in recent years to treat heavy metals, e.g. hexavalent chromium Cr pollution, which damages the surrounding ecosystem and threaten human health. This kind of MOF is stable and convenient to prepare, but has the disadvantage of low adsorption capacity, limiting its wide application. To this end, a novel formic acid and amino modified MOFs were prepared, referred to as Form-UiO-66-NH. Due to the modification of formic acid, its specific surface area, pore size, and crystal size were effectively expanded, and the adsorption capacity of Cr was significantly enhanced. Under optimal conditions, Form-UiO-66-NH exhibited an excellent adsorption capacity (338.98 mg/g), ∼10 times higher than that reported for unmodified Zr-based MOFs and most other adsorbents. An in-depth study on the photoelectronic properties and pH confirmed that the adsorption mechanism of Form-UiO-66-NH to Cr was electrostatic adsorption. After modification, the improvement of Cr adsorption capacity by Form-UiO-66-NH was attributed to the expansion of its specific surface area and the increase in its surface charge. The present study revealed an important finding that Form-UiO-66-NH elucidated selective adsorption to Cr in mixed wastewater containing toxic heavy metal ions and common nonmetallic water quality factors. This research provided a new acid and amino functionalization perspective for improving the adsorption capacity of Zr-based MOF adsorbents while simultaneously demonstrating their pertinence to target contaminant adsorption.
近年来,人们开发了基于锆的金属有机骨架(MOF)来处理重金属,例如六价铬 Cr 污染,这会破坏周围的生态系统并威胁人类健康。这种 MOF 稳定且易于制备,但存在吸附容量低的缺点,限制了其广泛应用。为此,制备了一种新型甲酸和氨基改性的 MOF,称为 Form-UiO-66-NH。由于甲酸的改性,其比表面积、孔径和晶体尺寸得到了有效扩展,Cr 的吸附能力显著增强。在最佳条件下,Form-UiO-66-NH 表现出优异的吸附容量(338.98 mg/g),约为未改性 Zr 基 MOF 和大多数其他吸附剂的 10 倍。对光电性能和 pH 值的深入研究证实,Form-UiO-66-NH 对 Cr 的吸附机制是静电吸附。改性后,Form-UiO-66-NH 对 Cr 吸附容量的提高归因于其比表面积的扩大和表面电荷的增加。本研究揭示了一个重要发现,即 Form-UiO-66-NH 对含有有毒重金属离子和常见非金属水质因素的混合废水中的 Cr 具有选择性吸附。这项研究为提高 Zr 基 MOF 吸附剂的吸附容量提供了一种新的酸和氨基功能化视角,同时证明了它们对目标污染物吸附的针对性。