FeMn-MOF/CN异质结光芬顿催化剂制备及性能研究

doi:10.19964/j.issn.1006-4990.2022-0146

摘要/Abstract

摘要：

通过一种简便的原位负载策略制备了铁锰双金属有机骨架/氮化碳异质结光芬顿催化剂FeMn-MOF/CN，并利用X射线衍射（XRD）、红外光谱（FT-IR）、扫描电镜（SEM）、光致发光（PL）光谱等测试手段对催化剂的组成、结构及光电化学性质进行了表征。以降解高浓度左氧氟沙星（LEV，100 mg/L）为模型反应评价了催化剂的光芬顿反应性能，并提出了可能的光芬顿反应机理。由于光催化和芬顿反应之间的协同作用，5%FeMn-MOF/CN（FeMn-MOF与CN的质量比为5%）异质结表现出优异的光芬顿反应性能，在40 min内对LEV的移除率达到98.8%。基于原位合成的策略，FeMn-MOF和CN之间形成了紧密的异质结界面，不但极大地提高了光生载流子的分离和传递效率，而且显著地促进了Fe（Ⅲ）/Fe（Ⅱ）和Mn（Ⅲ）/Mn（Ⅱ）的循环。该工作为高效光芬顿催化材料的设计和制备提供了新思路。

关键词: 光芬顿, 氮化碳, 双金属有机骨架, 异质结, 协同效应

Abstract:

The bimetal Fe，Mn-organic framework/carbon nitride heterojunction photo-Fenton catalysts（FeMn-MOF/CN） were prepared by a facile in-situ loading strategy，and the composition，structure and optoelectronic properties of the catalysts were characterized by X-ray diffraction（XRD），infrared spectroscopy（FT-IR），scanning electron microscopy（SEM），photoluminescence（PL） spectroscopy and etc.The photo-Fenton performance of the catalysts was evaluated by using the degradation of high concentration levofloxacin（LEV，100 mg/L） as model reaction，and the possible photo-Fenton reaction mechanism was proposed.Due to the synergistic effect between photocatalysis and Fenton reactions，5%FeMn-MOF/CN（mass ratio of FeMn-MoF/CN was 5%） exhi-bited excellent photo-Fenton performance，with the LEV removal efficiency of 98.8% within 40 min.An intimate heterojunction interface was formed between FeMn-MOF and CN via the in-situ loading strategy，which not only significantly improved the separation and transfer efficiency of photogenerated carriers，but also promoted the cycling of the Fe（Ⅲ）/Fe（Ⅱ）and Mn（Ⅲ）/Mn（Ⅱ）.This study provided a new idea for the design and preparation of efficient photo-Fenton catalytic materials.

Key words: photo-Fenton, carbon nitride, bimetallic MOF, heterojunction, synergistic effect

中图分类号:

O643.36

李向阳,刘紫威,李克艳,郭新闻. FeMn-MOF/CN异质结光芬顿催化剂制备及性能研究[J]. 无机盐工业, 2022, 54(12): 126-132.

LI Xiangyang,LIU Ziwei,LI Keyan,GUO Xinwen. Study on preparation and performance of FeMn-MOF/CN heterojunction photo-Fenton catalyst[J]. Inorganic Chemicals Industry, 2022, 54(12): 126-132.

图/表 6

图1

图2

图3

图4

图5

图6

参考文献 21

1	QIAO Min, YING Guangguo, SINGER A C, et al. Review of antibiotic resistance in China and its environment[J]. Environment International, 2018, 110: 160-172.
2	GOPAL G, ALEX S A, CHANDRASEKARAN N, et al. A review on tetracycline removal from aqueous systems by advanced treatment techniques[J]. RSC Advances, 2020, 10(45)：27081-27095.
3	LIU Xiaohui, ZHANG Guodong, LIU Ying, et al. Occurrence and fate of antibiotics and antibiotic resistance genes in typical urban water of Beijing，China[J]. Environmental Pollution, 2019, 246: 163-173.
4	ZHU Yanping, ZHU Runliang, XI Yunfei, et al. Strategies for enhancing the heterogeneous Fenton catalytic reactivity：A review[J]. Applied Catalysis B：Environmental, 2019, 255.Doi：10.1016/j.apcatb.2019.05.041 .
5	舒弋芮, 张攀, 王玮, 等. 钛白副产硫酸亚铁光芬顿氧化降解甲基橙的研究[J]. 无机盐工业, 2021, 53(3)：68-72.
	SHU Yirui, ZHANG Pan, WANG Wei, et al. Titanium white by-pro-duct ferrous sulfate photofenton oxidation degradation of methyl orange in wastewater[J]. Inorganic Chemicals Industry, 2021, 53(3)：68-72.
6	WEI Zhidong, LIU Junying, SHANGGUAN Wenfeng. A review on photocatalysis in antibiotic wastewater：Pollutant degradation and hydrogen production[J]. Chinese Journal of Catalysis, 2020, 41(10)：1440-1450.
7	李佳慧, 李克艳, 宋春山, 等. 聚合氮化碳的制备、改性及光催化还原二氧化碳性能研究[J]. 无机盐工业, 2021, 53(12)：21-28.
	LI Jiahui, LI Keyan, SONG Chunshan, et al. Study on preparation，modification and carbon dioxide photocatalytic reduction performance of polymeric carbon nitride[J]. Inorganic Chemicals Industry, 2021, 53(12)：21-28.
8	YANG Xingxing, YE Yongli, SUN Jiadi, et al. Recent advances in g-C3N4-based photocatalysts for pollutant degradation and bacterial disinfection：Design strategies，mechanisms，and applicatio-ns[J]. Small, 2022, 18(9).Doi：10.1002/smll.202105089 .
9	ONG W J, TAN L L, NG Y H, et al. Graphitic carbon nitride（g-C₃N₄）-based photocatalysts for artificial photosynthesis and environmental remediation：Are we a step closer to achieving sustainability？[J]. Chemical Reviews, 2016, 116(12)：7159-7329.
10	CHENG Lei, ZHANG Huaiwu, LI Xin, et al. Carbon-graphitic carbon nitride hybrids for heterogeneous photocatalysis[J]. Sm- all, 2021, 17(1).Doi：10.1002/smll.202005231 .
11	LI Yuanyuan, FANG Yu, CAO Zhenlei, et al. Construction of g-C₃N₄/PDI@MOF heterojunctions for the highly efficient visible light-driven degradation of pharmaceutical and phenolic micropollutants[J]. Applied Catalysis B：Environmental, 2019, 250: 150-162.
12	LI Yuxuan, HAN Yongchun, WANG Chongchen. Fabrication strategies and Cr（Ⅵ） elimination activities of the MOF-derivati-ves and their composites[J]. Chemical Engineering Journal, 2021, 405.Doi：10.1016/j.cej.2020.126648 .
13	WU Qiangshun, YANG Hanpei, KANG Li, et al. Fe-based metal-organic frameworks as Fenton-like catalysts for highly efficient degradation of tetracycline hydrochloride over a wide pH range：Acceleration of Fe（Ⅱ）/Fe（Ⅲ） cycle under visible light irradiation[J]. Applied Catalysis B：Environmental, 2020, 263.Doi：10.1016/j.apcatb.2019.118282 .
14	WU Qiangshun, SIDDIQUE M S, GUO Yuling, et al. Low-crystalline bimetallic metal-organic frameworks as an excellent platform for photo-Fenton degradation of organic contaminants：Intensified synergism between hetero-metal nodes[J]. Applied Catalysis B：Environmental, 2021, 286.Doi10.1016/j.apcatb.2021.119950.
15	HE Wenjuan, LI Zuopeng, LV Shengchen, et al. Facile synthesis of Fe₃O₄@MIL-100（Fe） towards enhancing photo-Fenton like degradation of levofloxacin via a synergistic effect between Fe₃O₄ and MIL-100（Fe）[J]. Chemical Engineering Journal, 2021, 409.Doi：10.1016/j.cej.2020.128274 .
16	ZHAO Feiping, LIU Yongpeng, HAMMOUDA S B, et al. MIL-101（Fe）/g-C3N4 for enhanced visible-light-driven photocatalysis toward simultaneous reduction of Cr（Ⅵ） and oxidation of bisphenol A in aqueous media[J]. Applied Catalysis B：Environmental, 2020, 272.Doi：10.1016/j.apcatb.2020.119033 .
17	WANG Xinchen, MAEDA K, THOMAS A, et al. A metal-free poly-meric photocatalyst for hydrogen production from water under visible light[J]. Nature Materials, 2009, 8(1)：76-80.
18	LI Qiansong, XU Hao, ZHOU Guanyu, et al. Sulfite activation by Fe-doped g-C3N4 for metronidazole degradation[J]. Separation and Purification Technology, 2021, 272.Doi：10.1016/j.seppur.2021.118928 .
19	ZHAO Binbin, XU Jiachao, LIU Yongping, et al. Amino group-rich porous g-C3N4 nanosheet photocatalyst：Facile oxalic acid-induced synthesis and improved H2-evolution activity[J]. Ceramics International, 2021, 47(13)：18295-18303.
20	ZHAO Shuangchao, LI Keyan, DU Jun, et al. Facile construction of a hollow In2S3/polymeric carbon nitride heterojunction for efficient visible-light-driven CO2 reduction[J]. ACS Sustainable Che- mistry & Engineering, 2021, 9(17)：5942-5951.
21	ZHOU Liang, LIU Zhihang, GUAN Zhipeng, et al. 0D/2D plasmonic Cu_2- _x S/g-C₃N₄nanosheets harnessing UV-vis-NIR broad spectrum for photocatalytic degradation of antibiotic pollutant[J]. Applied Catalysis B：Environmental, 2020, 263.Doi：10.1016/j.apcatb.2019.118326 .

[1]	张飞刚, 刘中利. CuO/g-C₃N₄复合材料在有机染料降解和超级电容器中的应用研究[J]. 无机盐工业, 2025, 57(1): 129-136.
[2]	王雅雯, 王芳芳, 耿司宇, 鞠佳, 陈雷, 陈常东. SrTiO₃-SrWO₄的制备及其光催化性能研究[J]. 无机盐工业, 2024, 56(7): 143-149.
[3]	刘敏, 黄秀, 张理元. S型异质结光催化剂的研究进展[J]. 无机盐工业, 2024, 56(7): 18-27.
[4]	李江朋, 张慧斌. 三维多孔LaFeO₃/CeO₂/SrTiO₃光芬顿和光催化协同脱色亚甲基蓝[J]. 无机盐工业, 2024, 56(5): 141-148.
[5]	唐贝. ZnO/g-C₃N₄异质结光催化材料的制备及对吡啶的降解[J]. 无机盐工业, 2024, 56(4): 133-142.
[6]	胡明亮, 周微, 李滨, 赖晓玲. 协同效应催化甲烷二氧化碳重整研究进展[J]. 无机盐工业, 2024, 56(1): 23-32.
[7]	晏超群, 张贤明, 魏娟, 程治良, 徐倩, 张轩. 立方体形α-Fe₂O₃光催化剂的合成及其可见光芬顿降解抗生素[J]. 无机盐工业, 2023, 55(8): 28-35.
[8]	赵炎, 郝雪薇, 时海南, 李佳慧, 李克艳, 郭新闻. 铜掺杂TiO₂/PCN异质结光催化还原二氧化碳性能研究[J]. 无机盐工业, 2023, 55(8): 21-27.
[9]	孙海杰, 程圆, 田源, 柳宏岩, 陈志浩. BiOI/g-C₃N₄催化剂的制备及其光催化降解罗丹明B性能[J]. 无机盐工业, 2023, 55(8): 36-44.
[10]	李宇航, 王银斌, 魏强. Fe₂O₃-Co₃O₄异质结的熔盐法制备及其析氢性能[J]. 无机盐工业, 2023, 55(8): 51-58.
[11]	武讨龙, 张胜江, 刘津洋, 洪晓博, 李丽敏, 覃晓玉, 谭晓英, 周燕. 双金属有机框架材料的研究进展[J]. 无机盐工业, 2023, 55(6): 8-17.
[12]	陈彰旭, 傅明连, 朱丹琛, 郑炳云. 碳/石墨相氮化碳复合材料制备及其去除亚甲基蓝性能[J]. 无机盐工业, 2023, 55(3): 134-139.
[13]	王君良, 赵爱明, 敖先权, 李松鸿, 曹阳. 白酒酒糟与污水污泥共气化制氢反应特性及协同性分析[J]. 无机盐工业, 2023, 55(3): 118-125.
[14]	李松鸿,周松华,赵爱明,董文燕,姜春燕,曹阳,敖先权. 水/二氧化碳气氛下酒糟催化气化反应特性的研究[J]. 无机盐工业, 2023, 55(2): 132-140.
[15]	马炳香,申云霞,李娜,李敏,韦尧意,赵宇. 硫酸根对聚合氮化碳光催化活性的影响[J]. 无机盐工业, 2022, 54(9): 150-157.

首页

全国无机盐信息中心

中国化工学会

无机酸碱盐专业委员会