中国环境科学2024,Vol.44Issue(4) :2073-2082.

一种C3N4光催化剂的制备及其对四环素类抗生素的降解

Preparation of a C3N4 photocatalyst and its degradation of tetracycline antibiotics

高艺芳 郭瑞 焦媛 刘晓娜 钱天伟
中国环境科学2024,Vol.44Issue(4) :2073-2082.

一种C3N4光催化剂的制备及其对四环素类抗生素的降解

Preparation of a C3N4 photocatalyst and its degradation of tetracycline antibiotics

高艺芳 1郭瑞 1焦媛 1刘晓娜 1钱天伟1
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作者信息

  • 1. 太原理工大学环境科学与工程学院,山西晋中 030606
  • 折叠

摘要

以单一尿素为前驱体,通过热聚合制备了 C3N4,并通过SEM、XRD、XPS、FT-IR、UV-Vis等分析表征了所制备的C3N4材料的结构、成分、光学性能和光催化活性.结果发现制备的C3N4具有花状的多孔纳米片结构和大的比表面积.制备的C3N4在氙灯320~780nm的照射下,对盐酸四环素(TCH)的降解表现出良好的光催化活性,60min内降解率达到99.60%.自由基淬灭实验的结果表明,·O2-、1O2和h+是TCH降解的主要原因.对比试验和DFT理论计算分析发现,以尿素为原料制备的C3N4比三聚氰胺为原料制备的M-C3N4光催化效果优异是归因于C3N4具有花状的多孔结构,更大比表面积以更多的活性位点和氧空位.此外,制备的催化剂C3N4对四环素类的抗生素(盐酸金霉素(CTC)和土霉素(OTC))具有类似的催化效果.进一步通过分析光催化氧化中间产物,提出了 TCH可能的降解路径.

Abstract

In this study,C3N4 was fabricated by thermal polymerization using a single urea as a precursor,for which the structure,composition,optical properties and photocatalytic activity of the prepared C3N4 materials were characterized by SEM,XRD,XPS,FT-IR and UV-Vis analyses.The as-fabricated C3N4 was found to display a flower-like porous nanosheet structure and a large specific surface area.The C3N4 exhibited good photocatalytic activity for the degradation of tetracycline hydrochloride(TCH)under the irradiation of xenon lamp at 320~780nm,and the degradation rate reached 99.60%within 60min.The results of free radical quenching experiments showed that*O2、1O2 and h+were the main causes of TCH degradation.Further analysis by comparative tests and DFT theoretical calculations revealed that the superior photocatalytic effect of C3N4 prepared from urea than M-C3N4 prepared from melamine was attributed to the flower-like porous structure of C3N4 with larger specific surface area for more active sites and oxygen vacancies.Furthermore,the prepared catalyst C3N4 showed similar catalytic effect on tetracycline-based antibiotics(chrysomycin hydrochloride(CTC)and oxytetracycline(OTC)).Further,the possible degradation pathways of TCH were proposed by analyzing the photocatalytic oxidation intermediates.

关键词

光催化/C3N4/四环素/理论计算

Key words

photocatalysis/C3N4/tetracycline hydrochloride(TCH)/theoretical calculation

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基金项目

山西省科技厅基金资助项目(202103021223088)

山西省科技厅基金资助项目(20210302124056)

山西省教育厅基金资助项目(2021L030)

中国博士后科学基金(2023M743771)

出版年

2024
中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
参考文献量38
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