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0D/3D NiCoO/缺陷 UiO-66 催化剂用于过一硫酸盐/模拟太阳光体系中增强四环素的降解:降解机制和途径。

0D/3D NiCoO/defected UiO-66 catalysts for enhanced degradation of tetracycline in peroxymonosulfate/simulated sunlight systems: Degradation mechanisms and pathways.

机构信息

School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, PR China.

School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, PR China.

出版信息

Chemosphere. 2022 Jul;299:134322. doi: 10.1016/j.chemosphere.2022.134322. Epub 2022 Mar 16.

DOI:10.1016/j.chemosphere.2022.134322
PMID:35306056
Abstract

Developing synergistic systems and taking environmental risks into account are two necessary aspects of being considered to remove persistent organic pollutants efficiently. Thus, a combined catalytic system uniting the Fenton-like process and simulated solar-light photocatalysis has been constructed. Moreover, a series of NiCoO/HP-UiO-66 catalysts (yNiCo-DUx) were also fabricated to improve tetracycline (TC) removal efficiency. The NiCoO nanoparticles (NPs) and hierarchically porous metal-organic frameworks (HP-MOFs) were synthesised using one-step calcination. The Z-scheme structure of the catalysts was confirmed by ESR, XPS, DRS, time-resolved PL (TR-PL) spectra and the quenching experiments. The NiCoO nanoparticles could be embedded and fixed into the defects of the MOF structure, and the leaching of toxic metals was also significantly suppressed. In the optimal reaction condition with 15NiCo-DU50, sunlight, and peroxymonosulfate (PMS), the total removal efficiency of TC could reach 98.5% within 8 min of irradiation, and the highest % RSE could reach 11.2%. Moreover, the corresponding reaction rate was 28.7, 3.6 and 1.3-10.2 times higher than photocatalysis, Fenton-like processes and other catalysts. Furthermore, the possible degradation mechanism, generation of reactive species and PMS excitation pathways were also investigated in depth. The present study sheds light on the fabrication of HP-MOFs based catalysts and the combination of various methods to eliminate organic pollutants.

摘要

开发协同系统并考虑环境风险是高效去除持久性有机污染物的两个必要方面。因此,构建了结合类芬顿和模拟太阳光光催化的联合催化体系。此外,还制备了一系列 NiCoO/HP-UiO-66 催化剂(yNiCo-DUx)以提高四环素(TC)去除效率。通过一步煅烧合成了 NiCoO 纳米颗粒(NPs)和分级多孔金属有机骨架(HP-MOFs)。通过 ESR、XPS、DRS、时间分辨光致发光(TR-PL)光谱和淬灭实验证实了催化剂的 Z 型结构。NiCoO 纳米颗粒可以嵌入并固定在 MOF 结构的缺陷中,并且明显抑制了有毒金属的浸出。在最佳反应条件下,采用 15NiCo-DU50、阳光和过一硫酸盐(PMS),在辐照 8 分钟内 TC 的总去除效率可达到 98.5%,最高 % RSE 可达到 11.2%。此外,相应的反应速率分别比光催化、类芬顿过程和其他催化剂高 28.7、3.6 和 1.3-10.2 倍。此外,还深入研究了可能的降解机制、活性物质的生成和 PMS 激发途径。本研究为基于 HP-MOFs 的催化剂的制备和各种方法的结合提供了启示,以消除有机污染物。

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引用本文的文献

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Sulfate Radical-Based Degradation of Organic Pollutants: A Review on Application of Metal-Organic Frameworks as Catalysts.基于硫酸根自由基的有机污染物降解:金属有机框架材料作为催化剂的应用综述
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