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新型 II 型 MnNbO/g-CN 肖特基异质结光催化剂的合成:基于氟喹诺酮类抗生素的优异光催化性能和降解机制。

Synthesis of novel Type-II MnNbO/g-CN Mott-Schottky heterojunction photocatalyst: Excellent photocatalytic performance and degradation mechanism of fluoroquinolone-based antibiotics.

机构信息

Department of Materials Science and Engineering, National Taiwan University of Science and Technology, Taipei, 10607, Taiwan, ROC.

Department of Materials Science and Engineering, National Taiwan University of Science and Technology, Taipei, 10607, Taiwan, ROC.

出版信息

Chemosphere. 2023 Apr;321:138027. doi: 10.1016/j.chemosphere.2023.138027. Epub 2023 Jan 31.

Abstract

Fluoroquinolone antibiotics have been encountered in aquatic environments in quantities giving rise to significant concern recently. To cope with this problem, it is necessary to design a semiconductor photocatalyst having excellent photocatalytic efficiency to eliminate the antibiotics. The heterojunction is a likely situate where the efficiency of relevant photocatalyst can be strengthened. In this study, the performance of MnNbO/g-CN (MNO/g-CN) composites in the photocatalytic degradation of ciprofloxacin (CIP) and tetracycline-HCl (TCH) antibiotics was explored. Enhanced photocatalytic activity of MNO/g-CN was found to be owing to electron's shifting between the MNO, and g-CN sheets, which promotes the formation of photo-generated e⁻/h⁺ pairs. This shows a low-waste, high-performance material exists to eradicate CIP and TCH from wastewater. Further, the structural, photochemical and light interacted properties of the MNO/g-CN photocatalyst, prepared by solvothermal method and sonication, were described using photochemical, physiochemical and electrochemical approaches. The synthesized photocatalyst owes its particular efficiency to its methodical photo-degradation of CIP and TC using visible light. The optimum composite 15% MNO/g-CN evinced the greatest photocatalytic efficiency with CIP and TCH photo-degradation of 94.10%, and 98.50%, respectively, and degradation mechanism were investigated using LC-MS spectroscopy. The suitable photocatalytic activity is ascribed to lower the recombination's rate of e⁻/h⁺ pairs. The scavenging evaluations proved that the h and O were two major photoactive species accomplishing the CIP and TCH photodegradation over MNO/g-CN under visible region. Our findings pave the way for the construction of efficient binary photocatalysts for antibiotic restitution.

摘要

氟喹诺酮类抗生素在最近已在水生环境中被发现,其含量引起了人们的极大关注。为了解决这个问题,有必要设计一种具有优异光催化效率的半导体光催化剂来消除抗生素。异质结是提高相关光催化剂效率的可能位置。在这项研究中,探讨了 MnNbO/g-CN(MNO/g-CN)复合材料在环丙沙星(CIP)和盐酸四环素(TCH)抗生素光催化降解中的性能。发现 MNO/g-CN 的增强光催化活性归因于 MNO 和 g-CN 片之间电子的转移,这促进了光生电子空穴对的形成。这表明存在一种低废物、高性能的材料,可以从废水中消除 CIP 和 TCH。此外,通过光化学、物理化学和电化学方法描述了通过溶剂热法和超声法制备的 MNO/g-CN 光催化剂的结构、光化学和光相互作用特性。该合成光催化剂由于其使用可见光对 CIP 和 TC 的有针对性的光降解而具有特殊的效率。最佳复合 15% MNO/g-CN 对 CIP 和 TCH 的光降解效率最高,分别为 94.10%和 98.50%,并使用 LC-MS 光谱研究了降解机制。适当的光催化活性归因于降低了电子空穴对的复合率。清除评价证明,在可见光区域下,h 和 O 是两种主要的光活性物质,它们可以完成 MNO/g-CN 上的 CIP 和 TCH 光降解。我们的研究结果为构建用于抗生素恢复的高效二元光催化剂铺平了道路。

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