首页|一种C3N4光催化剂的制备及其对四环素类抗生素的降解

一种C3N4光催化剂的制备及其对四环素类抗生素的降解

扫码查看
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.
Preparation of a C3N4 photocatalyst and its degradation of tetracycline antibiotics
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.

photocatalysisC3N4tetracycline hydrochloride(TCH)theoretical calculation

高艺芳、郭瑞、焦媛、刘晓娜、钱天伟

展开 >

太原理工大学环境科学与工程学院,山西晋中 030606

光催化 C3N4 四环素 理论计算

山西省科技厅基金资助项目山西省科技厅基金资助项目山西省教育厅基金资助项目中国博士后科学基金

202103021223088202103021240562021L0302023M743771

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
年,卷(期):2024.44(4)
  • 38