Wang Yanhong, Han Dongmei, Wang Zhihua, Gu Fubo
State Key Laboratory of Chemical Resources Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
ACS Appl Mater Interfaces. 2023 May 10;15(18):22085-22100. doi: 10.1021/acsami.3c01255. Epub 2023 Apr 27.
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.
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。