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钴/铜基双金属有机框架材料的制备及其对过氧乙酸活化降解磺胺甲恶唑的研究

Preparation of Co/Cu-based bi-MOFs and the degradation of sulfamethoxazole by activated peracetic acid.

作者信息

Liu Zhenzhong, Wu Yang, Wan Siwen, Wang Boyan, Ji Hongliang, Xiang Xiaofang

机构信息

School of Resources and Environment, Nanchang University, Nanchang 330031, China E-mail:

School of Infrastructure Engineering, Nanchang University, Nanchang 330031, China.

出版信息

Water Sci Technol. 2023 Mar;87(5):1202-1213. doi: 10.2166/wst.2023.055.

Abstract

Compared with the common synthesis methods of metal-organic frameworks (MOFs), Co/Cu-based bi-MOFs composite catalyst CoCu-MOFs (X = 2, 4, 6, and 8) was prepared by a facile synthesis method at room temperature. The bi-MOFs composite catalyst was characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD). The removal ability of sulfamethoxazole (SMX) by different Co:Cu rate bi-MOFs composite catalysts, single Co-based MOFs (zeolitic imidazolate framework-67, ZIF-67), and Cu-based MOFs (Hong Kong University of Science and Technology-1, HKUST-1) were investigated and the effects of peracetic acid (PAA) concentration, catalyst dosage, the common interfering substances (Cl, HCO, SO, HA) in water, and SMX removal were investigated. Through the analysis of different free radical scavengers and the changes of surface elements before and after the reaction, the oxidation mechanism was further explored, and the stability of CoCu-MOFs was explored through repeated recycling. The experimental results demonstrate that CoCu-MOFs have a high catalytic activity for PAA. CoCu-MOFs/PAA show the best removal effect of SMX under neutral conditions and the presence of Cl and HCO can promote the removal of SMX.

摘要

与金属有机框架(MOFs)的常见合成方法相比,通过室温下简便的合成方法制备了基于Co/Cu的双金属有机框架复合催化剂CoCu-MOFs(X = 2、4、6和8)。采用扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FTIR)和X射线衍射(XRD)对双金属有机框架复合催化剂进行了表征。研究了不同Co:Cu比例的双金属有机框架复合催化剂、单一Co基金属有机框架(沸石咪唑酯骨架-67,ZIF-67)和Cu基金属有机框架(香港科技大学-1,HKUST-1)对磺胺甲恶唑(SMX)的去除能力,以及过氧乙酸(PAA)浓度、催化剂用量、水中常见干扰物质(Cl、HCO、SO、HA)对SMX去除效果的影响。通过分析不同自由基清除剂以及反应前后表面元素的变化,进一步探究了氧化机理,并通过重复循环考察了CoCu-MOFs的稳定性。实验结果表明,CoCu-MOFs对PAA具有较高的催化活性。CoCu-MOFs/PAA在中性条件下对SMX的去除效果最佳,Cl和HCO的存在可促进SMX的去除。

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