漂浮型氮化碳光催化剂CNx@mEP的制备及性能

doi:10.16085/j.issn.1000-6613.2022-0414

摘要/Abstract

摘要：

针对氮化碳粉末光催化剂在应用过程中存在难以回收、光催化效率不高的问题，本研究采用“浸渍-煅烧”方法，以膨胀珍珠岩为载体，制备了一种方便回收、可多次利用的漂浮型氮化碳光催化剂CNx@mEP。采用扫描电镜（SEM）、X射线衍射仪（XRD）、X射线光电子能谱仪（XPS）、全自动比表面及孔径分析仪（BET）、傅里叶红外光谱仪（FTIR）以及紫外可见近红外漫反射测试（UV-vis）对CNx@mEP进行了分析。分别通过染料降解实验和有害藻类去除实验考察了催化剂的光催化性能。当双氰胺使用量与膨胀珍珠岩载体的质量比为2∶1时得到的CN2@mEP材料光催化性能最好，当催化剂使用量为4g/L时，在可见光下4h降解67.2%的罗丹明B、86.8%的刚果红、31.2%的甲基橙染料和35%的铜绿微囊藻。漂浮型氮化碳光催化剂经过3次重复利用后，仍保持较为稳定的去除效率。

关键词: 氮化碳, 漂浮载体, 可见光, 染料降解, 藻类灭活

Abstract:

A floating carbon nitride photocatalyst, CNx@mEP, was prepared by the “impregnation-calcination” method using expanded perlite as the carrier, which can be easily recycled and reused. The CNx@mEP was analyzed by Scanning electric microscopic (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Automatic specific surface and aperture analyzer (BET), Fourier transform infrared spectroscopy (FTIR) and UV-vis absorption spectroscopy (UV-vis). The photocatalytic performance of the catalysts was investigated by dye degradation experiments and harmful algae removal experiments. The best photocatalytic performance of the CN2@mEP material was obtained when the mass ratio of dicyandiamide used to the expanded perlite carrier was 2∶1. At a dosage of 4g/L, 67.2% of Rhodamine B, 86.8% of Congo red, 31.2% of Methyl orange dye and 35% of Microcystis aeruginosa were degraded under visible light irradiation for 4h. The floating carbon nitride photocatalyst maintained a relatively stable removal efficiency after 3 reuse cycles.

Key words: carbon nitride, floating carrier, visible-light, dye degradation, algal inactivation

中图分类号:

陈毓, 王佳佳, 汤琳. 漂浮型氮化碳光催化剂CNx@mEP的制备及性能[J]. 化工进展, 2022, 41(12): 6477-6488.

CHEN Yu, WANG Jiajia, TANG Lin. Preparation and performance of floating carbon nitride photocatalyst CNx@mEP[J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6477-6488.

图/表 13

图1 实验材料及实验条件

图2 染料标准曲线及藻类生长曲线

表1 三维荧光光谱积分区域分类

区域	有机物种类	典型代表物质	激发波长 /nm	发射波长 /nm
Ⅰ	芳香蛋白类物质	酪氨酸、色氨酸	220～250	280～330
Ⅱ	芳香蛋白类物质		220～250	330～380
Ⅲ	富里酸类物质	富里酸	220～250	380～500
Ⅳ	溶解性微生物代谢产物	蛋白质	250～280	280～380
Ⅴ	腐殖酸类物质	腐殖酸	250～400	380～500

图3 EP、mEP和CN2@mEP的SEM图及CN2@mEP的元素Mapping图

图4 BET和XRD测试结果

图5 CN2@mEP的XPS测试结果

图6 FTIR谱图、UV-vis吸收光谱及CN2@mEP的能带结构分析

图7 光致发光光谱图及光催化剂瞬态光电流响应图

图8 CN2@mEP在可见光照射下对50mL初始浓度为10mg/L的不同种类染料废水的降解效果比较，材料稳定性实验及材料吸附与降解行为比较

图9 CN2@mEP在可见光照射下对50mL初始浓度为2.06×106个细胞/mL藻液的降解效果及溶液中叶绿素a含量变化

图10 细胞形态的变化

图11 光催化反应过程中溶液的EEM图

图12 溶液荧光指数变化

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