College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, PR China.
College of Environmental & Energy Engineering, Beijing University of Technology, Beijing, 100124, PR China.
Chemosphere. 2021 Apr;268:129157. doi: 10.1016/j.chemosphere.2020.129157. Epub 2020 Dec 7.
Antibiotic contamination has already been one of hazards to aquatic environment due to the abuse of antibiotics. Metal-organic frameworks (MOFs) are known as a kind of promising porous material for solving the environmental deterioration. In this article, the physicochemical and electrochemical properties of a series of porous copper oxide carbon materials (CuOx-C) synthesized by carbonizing Cu-BTC were compared. Due to the suitable carbonization temperature, CuOx-C-550 N, whose geometric structure was similar to Cu-BTC, possessed a multiscale pore structure containing many mesopores and partial macropores in accordance with the pore size distribution curves. More copper/copper oxides were introduced toimproving the electrochemical ability, evidence by XRD, XPS, CV and EIS characterization. Moreover, the degradation of ceftazidime (CAZ) through anodic oxidation was discussed. In AO/CuOx-C-550 N system, the effects of current, solution pH, initial CAZ concentration and NaSO concentration were analyzed. CAZ removal rate reached 100% within 20 min under the optimal condition and a good electrocatalytic ability with 90% CAZ removal after 20 runs indicated a good electrochemical stability of CuOx-C-550 N. Furthermore, the degradation mechanism and pathway of CAZ were proposed. The Cu(II)/Cu(I) oxidation-reduction couples on the anodic surface contribute to the efficiently selective degradation of cephalosporins for CuOx-C-550 N. Overall, this study shows a good method to design and prepare a new MOF derivative for the remediation of aquatic contamination.
抗生素的滥用导致其污染已经成为了水生环境的危害之一。金属-有机骨架(MOFs)作为一种有前途的多孔材料,被广泛应用于解决环境恶化问题。本文比较了一系列通过碳化 Cu-BTC 合成的多孔氧化铜碳材料(CuOx-C)的物理化学和电化学性质。由于合适的碳化温度,CuOx-C-550N 的几何结构与 Cu-BTC 相似,具有包含许多中孔和部分大孔的多尺度孔结构,符合孔径分布曲线。更多的铜/氧化铜被引入以提高电化学性能,这可以通过 XRD、XPS、CV 和 EIS 表征来证明。此外,还讨论了通过阳极氧化降解头孢他啶(CAZ)的过程。在 AO/CuOx-C-550N 体系中,分析了电流、溶液 pH、初始 CAZ 浓度和 NaSO4 浓度的影响。在最佳条件下,CAZ 的去除率在 20 分钟内达到 100%,经过 20 次运行后,CAZ 的去除率仍高达 90%,表明 CuOx-C-550N 具有良好的电化学稳定性。此外,还提出了 CAZ 的降解机制和途径。阳极表面上的 Cu(II)/Cu(I)氧化还原对有助于 CuOx-C-550N 对头孢菌素的高效选择性降解。总的来说,这项研究为设计和制备用于修复水环境污染的新型 MOF 衍生物提供了一种很好的方法。