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一锅法合成富氧空位的 Cu 掺杂 UiO-66 用于协同吸附和光催化降解环丙沙星。

One-pot synthesis of oxygen-vacancy-rich Cu-doped UiO-66 for collaborative adsorption and photocatalytic degradation of ciprofloxacin.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

出版信息

Sci Total Environ. 2022 Apr 1;815:151962. doi: 10.1016/j.scitotenv.2021.151962. Epub 2021 Nov 27.

Abstract

UiO-66, as one of the most stable metal-organic frameworks (MOFs), has attracted a lot of attention in the field of adsorption and photocatalysis. However, this application of UiO-66 is still limited due to either the low accessibility of micropores or the poor electron-hole charge separation capability. This study aims to promote UiO-66 accessibility of micropores and charge separation through the construction of oxygen vacancies (OVs) and mesopore defects as well as copper incorporation. Herein, mesopore Cu doped UiO-66 with rich OVs was synthesized by a one-pot method and demonstrated high efficiency for the removal of ciprofloxacin (CIP) from the aquatic system. First of all, denatured mesopore defects were produced in Cu doped UiO-66 which possessed a 58% increase in specific surface area compared to UiO-66, facilitating the adsorption of molecular oxygen. Secondly, e was preferentially trapped by OVs under light irradiation. Electron (e) reacted rapidly with the surface adsorbed oxygen to generate superoxide radical (O). Meanwhile, copper incorporation increased the photocurrent and reduced the interfacial charge transfer resistance, thereby improving the charge separation efficiency. As a result, the adsorption efficiency and photocatalytic performance of mesopore Cu doped UiO-66 with OVs were 8.1 and 3.7 times higher than those of UiO-66, respectively. This study paved a way for the one-step synthesis of MOFs containing OVs and broadened the possibilities of practical applications for photo-induced removal of antibiotics from effluent.

摘要

UiO-66 作为最稳定的金属有机骨架(MOFs)之一,在吸附和光催化领域引起了广泛关注。然而,由于微孔的可及性低或电子空穴电荷分离能力差,UiO-66 的这种应用仍然受到限制。本研究旨在通过构建氧空位(OVs)和中孔缺陷以及铜的掺入来提高 UiO-66 的微孔可及性和电荷分离效率。本文通过一锅法合成了具有丰富氧空位的中孔掺杂铜 UiO-66,该材料在去除水系统中的环丙沙星(CIP)方面表现出高效。首先,在 Cu 掺杂的 UiO-66 中产生了变性的中孔缺陷,与 UiO-66 相比,其比表面积增加了 58%,有利于分子氧的吸附。其次,在光照下,电子(e)优先被 OVs 捕获。电子(e)与表面吸附的氧迅速反应生成超氧自由基(O)。同时,铜的掺入增加了光电流并降低了界面电荷转移电阻,从而提高了电荷分离效率。因此,中孔掺杂铜 UiO-66 的吸附效率和光催化性能分别比 UiO-66 提高了 8.1 倍和 3.7 倍。本研究为含有 OVs 的 MOFs 的一步合成开辟了道路,并拓宽了从废水中光诱导去除抗生素的实际应用的可能性。

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