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以金属银作为电荷传输桥的全固态Z型AgPO₄/MIL-101(Cr)异质结构在可见光下对四环素的高效光催化降解

Efficient Photocatalytic Degradation of Tetracycline under Visible Light by an All-Solid-State Z-Scheme AgPO/MIL-101(Cr) Heterostructure with Metallic Ag as a Charge Transmission Bridge.

作者信息

Wang Yanhong, Han Dongmei, Wang Zhihua, Gu Fubo

机构信息

State Key Laboratory of Chemical Resources Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

出版信息

ACS Appl Mater Interfaces. 2023 May 10;15(18):22085-22100. doi: 10.1021/acsami.3c01255. Epub 2023 Apr 27.

Abstract

The Z-type Ag/AgPO/MIL-101(Cr) heterojunction photocatalyst (referred to as AAM-x) was successfully prepared by a simple in situ precipitation method. The photocatalytic activity of the AAM-x samples was evaluated using a common tetracycline (TC) antibiotic. All AAM-x materials are more effective in removing TC than AgPO and MIL-101(Cr). Among them, AAM-3 exhibited efficient photodegradation efficiency and excellent structural stability, and the removal rate of TC (20 mg L) by AAM-3 (0.5 g L) under 60 min of visible light was 97.9%. The effects of photocatalyst dosage, pH, and inorganic anions were also systematically investigated. According to the X-ray photoelectron spectroscopy analysis, metallic silver particles appeared on the surface of the AgPO/MIL-101(Cr) mixture during the catalyst synthesis. The results of photoluminescence spectra, photocurrent response, EIS, and fluorescence lifetime showed that AAM-3 has a high photogenic charge separation efficiency. An all-solid-state Z-type heterojunction mechanism including AgPO, metallic Ag, and MIL-101(Cr) is proposed to rationalize the excellent photocatalytic performance and photostability of AAM-x composites and to explain the effect of metallic Ag acting as a charge transfer bridge. The TC intermediates were identified using liquid chromatography-mass spectrometry and possible routes of TC degradation were also discussed. This work provides a viable idea for removing antibiotics by an AgPO/MOF-based heterogeneous structured photocatalyst.

摘要

通过简单的原位沉淀法成功制备了Z型Ag/AgPO/MIL-101(Cr)异质结光催化剂(简称AAM-x)。使用常见的四环素(TC)抗生素评估了AAM-x样品的光催化活性。所有AAM-x材料在去除TC方面都比AgPO和MIL-101(Cr)更有效。其中,AAM-3表现出高效的光降解效率和优异的结构稳定性,在可见光下60分钟内,AAM-3(0.5 g/L)对20 mg/L的TC去除率为97.9%。还系统研究了光催化剂用量、pH值和无机阴离子的影响。根据X射线光电子能谱分析,在催化剂合成过程中,金属银颗粒出现在AgPO/MIL-101(Cr)混合物表面。光致发光光谱、光电流响应、电化学阻抗谱和荧光寿命的结果表明,AAM-3具有高光生电荷分离效率。提出了一种包括AgPO、金属Ag和MIL-101(Cr)的全固态Z型异质结机理,以解释AAM-x复合材料优异的光催化性能和光稳定性,并解释金属Ag作为电荷转移桥的作用。使用液相色谱-质谱法鉴定了TC中间体,并讨论了TC降解的可能途径。这项工作为基于AgPO/MOF的异质结构光催化剂去除抗生素提供了一个可行的思路。

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