采用溶胶凝胶-碳热还原法制备3C-SiC,通过水热法合成BiVO4/SiC复合材料.构建Vis+BiVO4/SiC+PMS体系降解CIP,在最佳实验条件下:1.0-BiVO4/SiC投加量为300mg/L、PMS浓度为2mmol/L、反应初始pH值为7时,40min时CIP的降解率为93.63%,反应速率常数k为0.05456min-1,分别是单独加入BiVO4和SiC的3.34和3.27倍.通过SEM、XRD、XPS、UV-Vis DRS及电化学工作站等方式对催化剂进行表征,BiVO4/SiC优异的光催化性能归因于形成的Z型异质结能够促进电子-空穴对分离的同时,保留催化剂高氧化还原性.因此,BiVO4/SiC形成的Z型异质结能有效的促进PMS的活化,生成更多的活性物种,从而加速了CIP的降解过程.通过自由基的猝灭实验,确定体系中的活性物种为h+、1O2、•O2-、•OH、SO4•−,通过自由基和非自由基的共同作用实现CIP的高效降解.最后,催化剂经过5次循环使用,CIP的降解率仍保持在89.49%.本文的研究成果不仅为光催化剂活化PMS提出新的解决方案,还能成功应用于抗生素的高效降解,为水体中有机污染物的治理提供一种新思路.
Abstract
3C-SiC was synthesized via the sol-gel carbothermal reduction method, and BiVO4/SiC composites were prepared using a hydrothermal approach. The Vis+BiVO4/SiC+PMS system was constructed for the degradation of CIP. Under optimized conditions, 1.0-BiVO4/SiC was added with a dosage of 300mg/L, PMS concentration of 2mmol/L, and initial pH of the reaction of 7—the system achieved a 93.63% CIP degradation rate within 40minutes, with the k of 0.05456min-1. These values represented 3.34 times and 3.27 times enhancement compared to BiVO4 and SiC, respectively. The catalyst was characterized by SEM, XRD, XPS, UV-Vis DRS and electrochemical workstation. The excellent photocatalytic performance of BiVO4/SiC was attributed to the formation of a Z-scheme heterojunction, which could promote the separation of electron-hole pairs while maintaining the high redox activity of the catalyst. Therefore, the Z-Scheme heterojunction formed by BiVO4/SiC could effectively promote the activation of PMS and generate more active species, thus accelerating the degradation process of CIP. The active species in the system were identified as h+、1O2、•O2-、•OH、SO4•−−− through the free radical quenching experiment. The efficient degradation of CIP was realized through the interaction of free radicals and non-free radicals. Notably, the catalyst exhibited excellent stability, retaining 89.49% of its initial degradation efficiency after five consecutive cycles. This study not only presents a novel strategy for PMS activation using photocatalysts but also demonstrates its successful application in antibiotic degradation, offering a promising approach for the remediation of organic pollutants in aquatic environments.
关键词
BiVO4 /
SiC /
Z型异质结 /
过硫酸盐 /
环丙沙星
Key words
BiVO4 /
SiC /
Z-Scheme heterojunction /
peroxymonosulfate /
ciprofloxacin
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基金
国家环境保护饮用水水源地保护重点实验室2022年度开放基金资助项目(2022YYSYKFYB1)