Fe⁃Doped g⁃C3N4 Photocatalytic Activation of Persulfate for Degradation of Azo Dyes

doi:10.3969/j.issn.1672-6952.2022.05.002

Abstract

Abstract:

Ferric nitrate was used to provide iron source, and Fe?C₃N₄ composite material was prepared by impregnation method. FT?IR was used to characterize and analyze the prepared materials. The results show that Fe doping does not change the skeleton structure of g?C₃N₄ and can increase the photocatalytic performance of g?C₃N₄ materials. Taking orange II as the target pollutant, Fe?C₃N₄ catalyzed the activation of persulfate to degrade azo dyes under visible light. The effects of persulfate dosage, Fe?C₃N₄ dosage, pollutant concentration and pH conditions on the degradation effect were examined, and the reaction kinetics was studied to analyze the stability of the prepared catalytic materials. The results show that when the Fe?C₃N₄ concentration is 2.0 g/L, the molar ratio of persulfate to pollutants is 1 200∶1, and pH=3, the degradation effect is best, and the degradation rate is 77.8%; Fe?C₃N₄/persulfate system is dual the degradation of nitrogen dyes satisfies the quasi?second?order kinetic equation; Fe?C₃N₄ material is reusable.

Key words: Iron?doped graphite phase carbon nitride, Persulfate, Photocatalysis, Azo dye

摘要：

以硝酸铁为铁源，通过浸渍法制备Fe?C₃N₄复合材料。采用FT?IR对Fe?C₃N₄材料进行了表征分析。结果表明，Fe掺杂不改变g?C₃N₄的骨架结构，可以增加g?C₃N₄材料的光催化性能。以橙黄II为目标污染物，在可见光下Fe?C₃N₄催化活化过硫酸钠降解偶氮染料，考察了过硫酸钠物质的量、Fe?C₃N₄质量浓度、橙黄II质量浓度及pH对降解效果的影响，并对反应进行了动力学研究，分析了所制备的催化材料的稳定性。结果表明，在Fe?C₃N₄质量浓度为2.0 g/L、过硫酸钠与污染物物质的量比为1 200∶1和pH=3的条件下，降解效果最好，降解率为77.8%；Fe?C₃N₄/过硫酸钠体系对偶氮染料的降解满足准二级动力学方程；Fe?C₃N₄材料具有可重复利用性。

关键词: 铁掺杂石墨相氮化碳, 过硫酸钠, 光催化, 偶氮染料

CLC Number:

X523

Chun Kang, Huiqiang Ma, Shuang Li. Fe⁃Doped g⁃C₃N₄ Photocatalytic Activation of Persulfate for Degradation of Azo Dyes[J]. Journal of Liaoning Petrochemical University, 2022, 42(5): 13-17.

亢春, 马会强, 李爽. Fe掺杂g⁃C₃N₄光催化活化过硫酸钠降解偶氮染料[J]. 辽宁石油化工大学学报, 2022, 42(5): 13-17.

Figures/Tables 8

References 21

1	王佳莹，孙德栋，孙义才，等.g⁃C₃N₄负载铁钴双金属催化过硫酸氢盐降解亚甲基橙［J］.工业水处理，2018，38（11）：66⁃69.
2	赵妍.高级氧化技术处理难降解有机污染物研究进展［J］.广东化工，2019，46（4）：93⁃94.
3	Lemaire J， Bues M， Kabeche T， et al. Oxidant selection to treat an aged PAH contaminated soil by in situ chemical oxidation［J］. Journal of Environmental Chemical Engineering， 2013， 1： 1261⁃1268.
4	吴丽颖，王炳煌，张圆春，等. 凝胶球负载零价铁活化过硫酸钠降解偶氮染料废水［J］. 化工进展， 2017， 36（6）： 2318⁃2324.
5	李强，李晴，吕扬，等. 碱金属改性g⁃C₃N₄及其对氮气吸附影响的理论研究［J］. 辽宁石油化工大学学报， 2018，38（6）：37⁃42.
6	张宏玲，李森，张杨，等. 过渡金属离子活化过硫酸盐去除土壤中的芘［J］. 环境工程学报， 2016， 10（10）： 6009⁃6014.
7	Yukselen A Y， Reddy K R. Effect of soil composition on electrokinetically enhanced persulfate oxidation of polychlorobiphenyls［J］. Electrochimica Acta， 2012， 86： 164⁃169.
8	李炳智，朱江. 超声活化过硫酸钠氧化降解水溶液中的全氟辛烷磺酸盐［J］. 农业环境科学学报， 2019， 38（4）：912⁃920.
9	Roshani B， Leitner N K V. Effect of persulfate on the oxidation of benzotriazole and humic acid by e⁃beam irradiation［J］. Journal of Hazardous Materials， 2011， 190（1⁃3）： 403⁃408.
10	侯先宇，陈炜鸣，李启彬，等. 微波活化过硫酸钠耦合混凝处理二硝基重氮酚工业废水［J］. 中国环境科学， 2018，38（12）：5⁃12.
11	史宸菲，薛瑞杰，李雨濛，等. 不同活性炭活化过硫酸钠的效能及机理的规律研究［J］. 环境科学学报， 2018， 38（4）：1501⁃1508.
12	金瑞瑞，游继光，张倩，等.Fe掺杂g⁃C₃N₄的制备及其可见光催化性能［J］.物理化学学报，2014，30（9）：1706⁃1712.
13	Tonda S， Kumar S， Kandula S， et al. Fe⁃doped and ⁃mediated graphitic carbon nitride nanosheets for enhanced photocatalytic performance under natural sunlight［J］. Journal of Materials Chemistry A， 2014， 2（19）：6772⁃6780.
14	吴文倩，邓德明. 铁掺杂氮化碳的制备及其可见光催化性能［J］. 武汉大学学报（理学版），2017，63（3）：227⁃233.
15	李昱慧，张静，张昱屾，等. 石墨相氮化碳光催化剂改性的研究进展［J］. 石油化工高等学校学报，2019，32（2）：1⁃7.
16	吝美霞，李法云，王艳杰，等. 改性石墨相氮化碳光催化降解有机污染物［J］. 辽宁石油化工大学学报， 2019， 39（2）：1⁃9.
17	Gao J T， Wang Y， Zhou S J， et al. A facile one⁃step synthesis of fe⁃doped g⁃C₃N₄nanosheets and their improved visible⁃light photocatalytic performance［J］. ChemCatChem， 2017， 9（9）： 1708⁃1715.
18	Dai B， Li X Y， Zhang J L， et al. Application of mesoporous carbon nitride as a support for an au atalyst for acetylene hydrochlorination［J］. Chemical Engineering Science， 2015， 135： 472⁃478.
19	Oh W D， Chang V W C， Hu Z T， et al. Enhancing the catalytic activity of g⁃C₃N₄ through Me doping （Me=Cu， Co and Fe） for selective sulfathiazole degradation via redox⁃based advanced oxidation process［J］. Chemical Engineering Journal， 2017， 323： 260⁃269.
20	Hu J S， Zhang P F， An W J， et al. In⁃situ Fe⁃doped g⁃C₃N₄ heterogeneous catalyst via photocatalysis⁃fenton reaction with enriched photocatalytic performance for removal of complex wastewater ［J］. Applied Catalysis B： Environmental， 2019， 245： 130⁃142.
21	Ansari R， Seyghali B， Mohammad⁃khah A， et al. Highly efficient adsorption of anionic dyes from aqueous solutions using sawdust modified by cationic surfactant of cetyltrimethylammonium bromide［J］. Journal of Surfactants & Detergents， 2012， 15（5）：557⁃565.

ρ（橙黄II）/ (mg·L^-1)	一级动力学方程			二级动力学方程
ρ（橙黄II）/ (mg·L^-1)	k₁/min^-1	Q_e/（mg·g^-1）	R²	k₂/[g·（mg·min）^-1]	Q_e/（mg·g^-1）	R²
50	0.017	0.18	0.896 4	0.16	0.36	0.992 0
20	0.011	0.15	0.969 7	0.18	0.41	0.996 7
10	0.016	0.20	0.867 0	0.14	0.42	0.992 2

ρ（橙黄II）/ (mg·L^-1)	一级动力学方程			二级动力学方程
ρ（橙黄II）/ (mg·L^-1)	k₁/min^-1	Q_e/（mg·g^-1）	R²	k₂/[g·（mg·min）^-1]	Q_e/（mg·g^-1）	R²
50	0.017	0.18	0.896 4	0.16	0.36	0.992 0
20	0.011	0.15	0.969 7	0.18	0.41	0.996 7
10	0.016	0.20	0.867 0	0.14	0.42	0.992 2

[1]	Lin ZHANG, Xiaojie GONG, Lihua LI. Photocatalytic Degradation of Tetracycline Hydrochloride by CeO₂@UiO⁃66 [J]. Journal of Liaoning Petrochemical University, 2024, 44(5): 8-14.
[2]	Xiangyu Ren, Baokuan Chen, Jing Sun, Yanfeng Bi. Double Polyoxometalates⁃Based Metal⁃Organic Framework with Photocatalytic Degradation Properties [J]. Journal of Liaoning Petrochemical University, 2023, 43(4): 51-58.
[3]	Changdong Chen, Zhe Li, Ke Li, Jinying Cong, Yuhang Yang, Fangfang Wang. Topological Transition Synthesis and Properties of TiO₂ Homogeneous Materials [J]. Journal of Liaoning Petrochemical University, 2022, 42(3): 37-41.
[4]	Jie Li, Kexin Fang, Lizhu Yao. Preparation and Photocatalytic Degradation Rhodamine B Properties of CNTs/Bi₁₂O₁₇Cl₂ Photocatalyst [J]. Journal of Liaoning Petrochemical University, 2021, 41(6): 42-47.
[5]	Huaichuan Shi, Lei Shi. Preparation and Photocatalytic Properties of Nanocarbon Particles/Carbon Nitride [J]. Journal of Liaoning Petrochemical University, 2021, 41(4): 41-45.
[6]	Wang Xiaodi， Li Lihua， Zhang Jinsheng， Wu Xian， Ma Cheng. Preparation of MnFe₂O₄/TiO₂and Its Fenton⁃Like Photocatalytic Properties [J]. Journal of Liaoning Petrochemical University, 2021, 41(2): 32-36.
[7]	Zhan Qi， Li Shuang， Zong Fang， Yang Changsheng， Ma Huiqiang. Bimetallic Catalyzed Persulfate Degradation of Azo Dyes [J]. Journal of Liaoning Petrochemical University, 2021, 41(1): 8-12.
[8]	Zhou Wenli， Hu Jiaqiao， Qu Yongkang， Kong Xingang. Photocatalytic Property of CsLaTa₂O₇/Na₂Ta₂O₆ Hetero⁃Architecture [J]. Journal of Liaoning Petrochemical University, 2020, 40(6): 1-5.
[9]	Qian Zhongwen, Lai Xiaochen, Lai Junling, Luo Genxiang. Synthesis of CuS by Elemental-Direct-Reaction in Deep Eutectic Solvents and Test on Photocatalytic Performance [J]. Journal of Liaoning Petrochemical University, 2016, 36(6): 10-13.
[10]	Wu Zhenyu, Liu Ningning. Photocatalytic Degradation of Rhodamine B by Metal Coordination Compounds [J]. Journal of Liaoning Petrochemical University, 2016, 36(2): 5-8.
[11]	Li Xiuping, Yuan Zhe, Gong Xiaojie, Xia Baosen, Zhang Xuanrui, Zhao Rongxiang. Preparation of Nickel Ferrite Composite Oxide with Combustion and Its Photocatalytic Application [J]. Journal of Liaoning Petrochemical University, 2016, 36(2): 9-12.
[12]	Lu Yuanyuan, Zhang Dan, Zhang Jing，Gong Xiaojie, Song Jia. Research on Synthesis and the Photocatalytic Degradation of Rhodanmine B of MIL53(Fe) [J]. Journal of Liaoning Petrochemical University, 2015, 35(5): 1-4.
[13]	Su Tingting, You Chunling, Zang Litao, Fan Chunyu, Jiang Heng, Gong Hong. LowTemperature Synthesis of Potassium Niobate by Improved SolidState Method and Its Photocatalytic Properties [J]. Journal of Liaoning Petrochemical University, 2014, 34(4): 18-21.
[14]	LI Xiuping, LI Xiurong, ZHAO Rongxiang, HU Yanan. Preparation of Nano ZnO with Homogeneous Precipitation  and Its Photocatalytic Properity [J]. Journal of Liaoning Petrochemical University, 2014, 34(1): 39-42.

Fe⁃Doped g⁃C₃N₄ Photocatalytic Activation of Persulfate for Degradation of Azo Dyes

Fe掺杂g⁃C₃N₄光催化活化过硫酸钠降解偶氮染料

HTML

PDF

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 8

References 21

Related Articles 14

Recommended Articles

Metrics