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

doi:10.19964/j.issn.1006-4990.2022-0579

Abstract

Abstract:

The abuse of antibiotics and disordered discharge of production wastewater cause the pollution of antibiotics in the water.The cubic morphology α-Fe₂O₃ photo-Fenton catalyst was synthesized by solvothermal method，and its microstructure and physical properties were characterized by scanning electron microscopy（SEM），transmission electron microscopy（TEM），and X-ray diffraction（XRD）.The adsorption and photo-Fenton degradation of TC by the new catalysts were investigated using tetracycline hydrochloride（TC） as a model antibiotic pollutant，and the effects of various factors including catalyst concentration，H₂O₂ content，LED light wavelength，and pH on TC degradation removal were investigated.The results showed that the cubic α-Fe₂O₃ with uniform particle size distribution was successfully synthesized and its adsorption on TC could reach equilibrium within 30 min，and the adsorption capacity could reach 7.06 mg/g.When the initial mass concentration of TC was 20 mg/L and the mass concentration of α-Fe₂O₃ catalyst was 0.5 g/L，the removal rate of TC could reach more than 80% by using visible LED light source photo-Fenton degradation for 30 min.

Key words: cubic α-Fe₂O₃, photo-Fenton, degradation, tetracycline hydrochloride

CLC Number:

TQ426

YAN Chaoqun, ZHANG Xianming, WEI Juan, CHENG Zhiliang, XU Qian, ZHANG Xuan. Synthesis of cubic α-Fe₂O₃ catalyst and its photo-Fenton degradation performance of antibiotic under visible light[J]. Inorganic Chemicals Industry, 2023, 55(8): 28-35.

Figures/Tables 10

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References 34

1	YUAN Fang， HU Chun， HU Xuexiang，et al.Photodegradation and toxicity changes of antibiotics in UV and UV/H₂O₂ process［J］.Journal of Hazardous Materials，2011，185（2/3）：1256-1263.
2	AHMED Y， ZHONG Jiexi， YUAN Zhiguo，et al.Roles of reactive oxygen species in antibiotic resistant bacteria inactivation and micropollutant degradation in Fenton and photo-Fenton processes［J］.Journal of Hazardous Materials，2022，430：128408.
3	LIAO Quan， RONG Hongwei， ZHAO Meihua，et al.Interaction between tetracycline and microorganisms during wastewater treatment：A review［J］.Science of the Total Environment，2021，757：143981.
4	TAOUFIK N， BOUMYA W， JANANI F Z，et al.Removal of emerging pharmaceutical pollutants：A systematic mapping study revi-ew［J］.Journal of Environmental Chemical Engineering，2020，8（5）：104251.
5	叶林静.ZnO基磁性光催化材料的制备及其降解四环素类抗生素的研究［D］.西安：长安大学，2014.
	YE Linjing.Synthesis of ZnO based magnetic photocatalysts and study on the photocatalytic degradation on tetracyclines［D］.Xi'an：Changan University，2014.
6	SHI Xiaoqiang， WANG Lina， ZUH A A，et al.Photo-Fenton reaction for the degradation of tetracycline hydrochloride using a FeWO₄/BiOCl nanocomposite［J］.Journal of Alloys and Compo- unds，2022，903：163889.
7	MIAO Yu， HEINTZ M B， BELL C H，et al.Profiling microbial community structures and functions in bioremediation strategies for treating 1，4-dioxane-contaminated groundwater［J］.Journal of Ha- zardous Materials，2021，408：124457.
8	GONZÁLEZ-GARCÍA I， RIAÑO B， CUÉLLAR-FRANCA R M，et al.Environmental sustainability performance of a membrane-based technology for livestock wastewater treatment with nutrient recovery［J］.Journal of Environmental Chemical Engineering，2022，10（2）：107246.
9	FAN Xiulei， ZOU Yefeng， GENG Nan，et al.Investigation on the adsorption and desorption behaviors of antibiotics by degradable MPs with or without UV ageing process［J］.Journal of Hazardous Materials，2021，401：123363.
10	潘涛.混凝法以及混凝-吸附组合法对制药废水的处理［J］.海峡药学，2010，22（2）：20-23.
	PAN Tao.Treatment and test of the pharmaceutical wastewater with coagulation，as well as the combination of coagulation and adsorption［J］.Strait Pharmaceutical Journal，2010，22（2）：20-23.
11	YI Qizhen， ZHANG Yu， GAO Yingxin，et al.Anaerobic treatment of antibiotic production wastewater pretreated with enhanced hydrolysis：Simultaneous reduction of COD and ARGs［J］.Water Research，2017，110：211-217.
12	LI Shizhong， LI Xiaoyan， WANG Dianzuo.Membrane（RO-UF） filtration for antibiotic wastewater treatment and recovery of antibiotics［J］.Separation and Purification Technology，2004，34（1/2/3）：109-114.
13	AKBARI M Z， XU Yifeng， LU Zhikun，et al.Review of antibiotics treatment by advance oxidation processes［J］.Environmental Advances，2021，5：100111.
14	YANG Lu， LI Ling， LIU Zhongtao，et al.Degradation of tetracycline by FeNi-LDH/Ti₃C₂ photo-Fenton system in water：From performance to mechanism［J］.Chemosphere，2022，294：133736.
15	陈娜丽，魏东明，孟雨霏，等.非均相光Fenton催化剂的研究现状［J］.应用化工，2021，50（8）：2269-2274，2279.
	CHEN Nali， WEI Dongming， MENG Yufei，et al.Researches status of heterogeneous photo Fenton catalysts［J］.Applied Chemical Industry，2021，50（8）：2269-2274，2279.
16	GU Lingli， SU Qin， JIANG Wu，et al.How do the unique Au/α-Fe₂O₃ interfacial structures determine activity in CO oxidation？［J］.Catalysis Science & Technology，2018，8（22）：5782-5793.
17	ZHANG Xin， JIA Xueyan， LI Manyuan，et al.Surface modification，adsorption behavior，and optical properties of α-Fe₂O₃@SiO₂/Au core-shell ellipsoids［J］.Colloids and Surfaces A：Physicochemical and Engineering Aspects，2021，625：126888.
18	KHAN J， LIN Shanshan， NIZEYIMANA J C，et al.Removal of copper ions from wastewater via adsorption on modified hematite （α-Fe₂O₃） iron oxide coated sand［J］.Journal of Cleaner Production，2021，319：128687.
19	MILAN-SEGOVIA N， WANG Yujue， CANNON F S，et al.Comparison of hydroxyl radical generation for various advanced oxidation combinations as applied to foundries［J］.Ozone：Science & Engineering，2007，29（6）：461-471.
20	XU Yong， SCHOONEN M A A.The absolute energy positions of conduction and valence bands of selected semiconducting minerals［J］.American Mineralogist，2000，85（3/4）：543-556.
21	LIN Zhirong， MA Xiaohong， ZHAO Ling，et al.Kinetics and products of PCB28 degradation through a goethite-catalyzed Fenton-like reaction［J］.Chemosphere，2014，101：15-20.
22	WU Jie， ZHANG Hui， OTURAN N，et al.Application of response surface methodology to the removal of the antibiotic tetracycline by electrochemical process using carbon-felt cathode and DSA （Ti/RuO₂-IrO₂） anode［J］.Chemosphere，2012，87（6）：614- 620.
23	OUYANG Jing， ZHAO Zai， SUIB S L，et al.Degradation of Congo Red dye by a Fe₂O₃@CeO₂-ZrO₂/Palygorskite composite catalyst：Synergetic effects of Fe₂O₃ ［J］.Journal of Colloid and Interface Science，2019，539：135-145.
24	XIANG Hengli， REN Genkuan， YANG Xiushan，et al.A low-cost solvent-free method to synthesize α-Fe₂O₃ nanoparticles with applications to degrade methyl orange in photo-Fenton system［J］.Ecotoxicology and Environmental Safety，2020，200：110744.
25	QIAO Disi， LI Zehao， DUAN Jinyou，et al.Adsorption and photocatalytic degradation mechanism of magnetic graphene oxide/ZnO nanocomposites for tetracycline contaminants［J］.Chemical Engineering Journal，2020，400：125952.
26	LIU Ying， KONG Jijie， YUAN Julong，et al.Enhanced photocatalytic activity over flower-like sphere Ag/Ag₂CO₃/BiVO₄ plasmonic heterojunction photocatalyst for tetracycline degradation［J］.Che- mical Engineering Journal，2018，331：242-254.
27	NASSEH N， HOSSEIN PANAHI A， ESMATI M，et al.Enhanced photocatalytic degradation of tetracycline from aqueous solution by a novel magnetically separable FeNi₃/SiO₂/ZnO nano-composite under simulated sunlight：Efficiency，stability，and kinetic studies［J］.Journal of Molecular Liquids，2020，301：112434.
28	GAO Bo， SAFAEI Z， BABU I，et al.Modification of ZnIn₂S₄ by anthraquinone-2-sulfonate doped polypyrrole as acceptor-donor system for enhanced photocatalytic degradation of tetracycline［J］.Journal of Photochemistry and Photobiology A：Chemistry，2017，348：150-160.
29	MA Yuhan， LI Mingyu， JIANG Jingjing，et al. In-situ prepared MIL-53（Fe）/BiOI photocatalyst for efficient degradation of tetracycline under visible-light driven photo-Fenton system：Investigation of performance and mechanism［J］.Journal of Alloys and Compounds，2021，870：159524.
30	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，2020，263：118282.
31	LIU Fang， YAO Hong， SUN Shaobin，et al.Photo-Fenton activation mechanism and antifouling performance of an FeOCl-coated ceramic membrane［J］.Chemical Engineering Journal，2020，402：125477.
32	ZHENG Mengting， XING Chao， ZHANG Weiping，et al.Hydrogenated hematite nanoplates for enhanced photocatalytic and photo-
	Fenton oxidation of organic compounds［J］.Inorganic Chemistry Communications，2020，119：108040.
33	LI Jialong， MENG Fanming， WU Hao，et al.Construction of Ag：ZnIn₂S₄/Bi₂S₃ Z-scheme heterojunctions for boosting interfacial charge separation and photocatalytic degradation of TC［J］.Applied Surface Science，2022，605：154763.
34	LIU Lei， HAN Chunjiang， DING Guofang，et al.Oxygen vacancies-enriched Cu/Co bimetallic oxides catalysts for high-efficiency peroxymonosulfate activation to degrade TC：Insight into the increase of Cu⁺ triggered by Co doping［J］.Chemical Engineering Journal，2022，450：138302.

催化剂	反应条件	TC处理量/mL	反应时间	降解率/%	速率常数/ min^-1
磁性氧化石墨烯/氧化锌纳米复合材料^［25］	TC质量浓度为50 mg/L，光照强度为1 kW/m²，催化剂质量浓度为1 g/L	50	吸附时间为40 h，光反应时间为100 min	74.0	14.0×10^-3
花球状Ag/Ag₂CO₃/BiVO₄^［26］	TC质量浓度为20 mg/L，催化剂质量浓度为 0.4 g/L，500 W氙灯	50	吸附时间为60 min，光反应时间为150 min	94.9	18.6×10^-3
FeNi₃/SiO₂/ZnO^［27］	TC质量浓度为10 mg/L，催化剂质量浓度为 0.02 g/L，500 W氙灯，pH为9	50	吸附时间为30 min，光反应时间为200 min	100.0	25.0×10^-3
ZnIn₂S₄^［28］	TC质量浓度为10 mg/L，催化剂质量浓度为 0.3 g/L，光照强度为380 kW/m²	100	吸附时间为30 min，光反应时间为180 min	98.0	—
MIL-53（Fe）/BiOI^［29］	TC质量浓度为25 mg/L，催化剂质量浓度为 0.5 g/L，300 W氙灯	50	吸附时间为30 min，光反应时间为14 min	86.2	90.6×10^-3
Fe-MOF^［30］	TC质量浓度为50 mg/L，催化剂质量浓度为 0.1g/L，300 W氙灯，pH为4.1	200	吸附时间为30 min，光反应时间为20 min	82.5	70.0×10^-3
立方体形α-Fe₂O₃（本研究）	TC质量浓度为20 mg/L，催化剂质量浓度为 0.5 g/L，405 nm-45 W LED，pH为5	100	吸附时间为30 min，光反应时间为30 min	80.0	67.5×10^-3

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Synthesis of cubic α-Fe₂O₃ catalyst and its photo-Fenton degradation performance of antibiotic under visible light

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Synthesis of cubic α-Fe2O3 catalyst and its photo-Fenton degradation performance of antibiotic under visible light