PREPARATION OF IRON-BASED CELLULOSE MICROSPHERES AND ITS ACTIVATION ON PERSULFATE TO DEGRADE TETRACYCLINE HYDROCHLORIDE

LIU Ruilong; REN Xiaohua; GUO Weilin

doi:10.13205/j.hjgc.202307012

Volume 41 Issue 7

Jul. 2023

Turn off MathJax

Article Contents

Abstract

References

Article Navigation > ENVIRONMENTAL ENGINEERING > 2023 > 41(7): 86-93,101

LIU Ruilong, REN Xiaohua, GUO Weilin. PREPARATION OF IRON-BASED CELLULOSE MICROSPHERES AND ITS ACTIVATION ON PERSULFATE TO DEGRADE TETRACYCLINE HYDROCHLORIDE[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(7): 86-93,101. doi: 10.13205/j.hjgc.202307012

Citation:

LIU Ruilong, REN Xiaohua, GUO Weilin. PREPARATION OF IRON-BASED CELLULOSE MICROSPHERES AND ITS ACTIVATION ON PERSULFATE TO DEGRADE TETRACYCLINE HYDROCHLORIDE[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(7): 86-93,101. doi: 10.13205/j.hjgc.202307012

Citation:

PDF( 5502 KB)

PREPARATION OF IRON-BASED CELLULOSE MICROSPHERES AND ITS ACTIVATION ON PERSULFATE TO DEGRADE TETRACYCLINE HYDROCHLORIDE

doi: 10.13205/j.hjgc.202307012

School of Water Conservancy and Environment, University of Jinan, Jinan 250022, China

Received Date: 2022-04-15

Abstract

Abstract

Iron-based catalysts have excellent performance in activating persulfate (PS) and are readily available, attracting extensive attention from researchers. However, most of the iron-based catalysts studied at the current stage are powder materials, and there are problems such as easy agglomeration and difficulty in recycling, which restrict their practical application. In this study, a microsphere catalyst (CA-Fe microspheres) with high catalytic activity was prepared using cellulose acetate (CA) as a carrier by droplet microfluidic technology. The morphology, structure and composition of the catalysts were characterized by SEM-EDS, FTIR and BET. The high catalytic degradation of tetracycline hydrochloride (TCH) in aqueous solution was tested by catalytic activation of PS. The effects of initial TCH concentration, the dosage of CA-Fe microspheres and the dosage of PS on TCH degradation were also investigated. The results showed that the CA-Fe microspheres had good activation performance for PS, and TCH could be effectively degraded in the CA-Fe/PS system. In the condition of the initial TCH concentration of 20 mg/L, the PS concentration of 2 mmol/L, and the CA-Fe microspheres dosage of 4 g/L, the degradation rate of TCH was about 85%. The electron paramagnetic resonance (EPR) and free radical quenching studies revealed that both SO₄^-· and·OH radicals were found in the CA-Fe microspheres/PS system, and the SO₄^-· radical played a major role in the degradation of TCH. Furthermore, the CA-Fe microspheres exhibited excellent structural stability and recycling performance, and the TCH degradation rate remained 80% above after three cycles. The results can provide a scientific basis for the application of cellulose-based magnetic microspheres/PS catalytic systems in the field of removing antibiotic wastewater.
- iron-based cellulose microspheres,
- microfluidics,
- persulfate,
- tetracycline hydrochloride,
- advanced oxidation process (AOPs)

FullText(HTML)

References(47)

References

[1]	ZHANG J J, QIU S, FENG H P, et al.Efficient degradation of tetracycline using core-shell Fe@Fe₂O₃-CeO₂ composite as novel heterogeneous electro-Fenton catalyst[J].Chemical Engineering Journal, 2022, 428:131403.
[2]	WEI Q Q, ZHOU K, CHEN J Y, et al.Insights into the molecular mechanism of tetracycline transport in saturated porous media affected by low-molecular-weight organic acids:role of the functional groups and molecular size[J].Science of the Total Environment, 2021, 799:149361.
[3]	SONG J L, HUANG M H, LIN X H, et al.Novel Fe-based metal-organic framework (MOF) modified carbon nanofiber as a highly selective and sensitive electrochemical sensor for tetracycline detection[J].Chemical Engineering Journal, 2022, 427:130913.
[4]	ALOTHMAN Z A, ALMASOUD N, MBIANDA X Y, et al.Synthesis and characterization of γ-cyclodextrin-graphene oxide nanocomposite:sorption, kinetics, thermodynamics and simulation studies of tetracycline and chlortetracycline antibiotics removal in water[J].Journal of Molecular Liquids, 2022, 345:116993.
[5]	DARVISHI CHESHMEH SOLTANI R, NADERI M, BOCZKAJ G, et al.Hybrid metal and non-metal activation of Oxone by magnetite nanostructures co-immobilized with nano-carbon black to degrade tetracycline:fenton and electrochemical enhancement with bio-assay[J].Separation and Purification Technology, 2021, 274:119055.
[6]	PIMENTEL J A I, DONG C D, GARCIA-SEGURA S, et al.Degradation of tetracycline antibiotics by Fe²⁺-catalyzed percarbonate oxidation[J].Science of The Total Environment, 2021, 781:146411.
[7]	GAO X, CHEN Y Q, KANG Z W, et al.Enhanced degradation of aqueous tetracycline hydrochloride by integrating eggshell-derived CaCO3/CuS nanocomposite with advanced oxidation process[J].Molecular Catalysis, 2021, 501:111380.
[8]	ZHANG J L, JIN X, YANG C H.Efficient removal of organic pollutants in waste sulfuric acid by an advanced oxidation process using coconut shell-derived biochar to produce qualified poly aluminium sulfate[J].Separation and Purification Technology, 2022, 293:121057.
[9]	PARK C M, HEO J, WANG D, et al.Heterogeneous activation of persulfate by reduced graphene oxide-elemental silver/magnetite nanohybrids for the oxidative degradation of pharmaceuticals and endocrine disrupting compounds in water[J].Applied Catalysis B, Environmental, 2018, 225:91-99.
[10]	MASUD M A A, KIM D G, SHIN W S.Highly efficient degradation of phenolic compounds by Fe(Ⅱ)-activated dual oxidant (persulfate/calcium peroxide) system[J].Chemosphere, 2022, 299:134392.
[11]	GAO Y, WANG Q, JI G Z, et al.Degradation of antibiotic pollutants by persulfate activated with various carbon materials[J].Chemical Engineering Journal, 2022, 429:132387.
[12]	ANUSHREE C, NANDA GOPALA KRISHNA D, PHILIP J.Efficient dye degradation via catalytic persulfate activation using iron oxide-manganese oxide core-shell particle doped with transition metal ions[J].Journal of Molecular Liquids, 2021, 337:116429.
[13]	TIAN K, HU L M, LI L T, et al.Recent advances in persulfate-based advanced oxidation processes for organic wastewater treatment[J].Chinese Chemical Letters, 2022, 33(10):4461-4477.
[14]	LIU Q Q, ZHANG L L, CHEN H X, et al.Sulfur and nitrogen co-doped three-dimensional graphene aerogels for high-performance supercapacitors:a head to head vertical bicyclic molecule both as pillaring agent and dopant[J].Applied Surface Science, 2021, 565:150453.
[15]	GE L, SHAO B B, LIANG Q H, et al.Layered double hydroxide based materials applied in persulfate based advanced oxidation processes:property, mechanism, application and perspectives[J].J Hazard Mater, 2022, 424:127612.
[16]	DING X Y, SONG X, CHEN X, et al.Degradation and mechanism of hexafluoropropylene oxide dimer acid by thermally activated persulfate in aqueous solutions[J].Chemosphere, 2021, 286:131720.
[17]	REN T L, MA X W, WU X Q, et al.Degradation of imidazolium ionic liquids in a thermally activated persulfate system[J].Chemical Engineering Journal, 2021, 412:128624.
[18]	ZHANG Y L, CHU W.Bisphenol S degradation via persulfate activation under UV-LED using mixed catalysts:synergistic effect of Cu-TiO₂ and Zn-TiO₂ for catalysis[J].Chemosphere, 2021, 286:131797.
[19]	CHEN T S, MA J S, ZHANG Q X, et al.Degradation of propranolol by UV-activated persulfate oxidation:reaction kinetics, mechanisms, reactive sites, transformation pathways and Gaussian calculation[J].The Science of the Total Environment, 2019, 690:878-890.
[20]	KAN H S, WANG T C, YU J X, et al.Remediation of organophosphorus pesticide polluted soil using persulfate oxidation activated by microwave[J].J Hazard Mater, 2021, 401:123361.
[21]	GARCIA-CERVILLA R, SANTOS A, ROMERO A, et al.Compatibility of nonionic and anionic surfactants with persulfate activated by alkali in the abatement of chlorinated organic compounds in aqueous phase[J].The Science of the Total Environment, 2021, 751:141782.
[22]	SHAN A, IDREES A, ZAMAN W Q, et al.Synthesis of nZVI-Ni@BC composite as a stable catalyst to activate persulfate:trichloroethylene degradation and insight mechanism[J].Journal of Environmental Chemical Engineering, 2021, 9(1):104808.
[23]	MIAO W, LIU Y, WANG D D, et al.The role of Fe-Nx single-atom catalytic sites in peroxymonosulfate activation:formation of surface-activated complex and non-radical pathways[J].Chemical Engineering Journal, 2021, 423:130250.
[24]	DUAN P T, PAN J W, DU W Y, et al.Activation of peroxymonosulfate via mediated electron transfer mechanism on single-atom Fe catalyst for effective organic pollutants removal[J].Applied Catalysis B:Environmental, 2021, 299:120714.
[25]	GAO Y, CONG S B, YU H Y, et al.Investigation on microwave absorbing properties of 3D C@ZnCo₂O₄ as a highly active heterogenous catalyst and the degradation of ciprofloxacin by activated persulfate process[J].Separation and Purification Technology, 2021, 262:118330.
[26]	RAO L J, YANG Y F, LIU X D, et al.Heterogeneous activation of persulfate by supporting ferric oxalate onto activated carbon fibers for organic contaminants removal[J].Materials Research Bulletin, 2020, 130:110919.
[27]	LI T, CHEN C, BROZENA A H, et al.Developing fibrillated cellulose as a sustainable technological material[J].Nature, 2021, 590(7844):47-56.
[28]	FAHIM A M, ABOUZEID R E, KIEY S A A, et al.Development of semiconductive foams based on cellulose- benzenesulfonate/CuFe₂O₄-nanoparticles and theoretical studies with DFT/B3PW91/LANDZ2 basis set[J].Journal of Molecular Structure, 2022, 1247:131390.
[29]	MIAO F, LIU Z H, KANG X C, et al.Electro-enhanced heterogeneous activation of peroxymonosulfate via acceleration of Fe(Ⅲ)/Fe(Ⅱ) redox cycle on Fe-B catalyst[J].Electrochimica Acta, 2021, 377:138073.
[30]	YANG Z, LUO M S, LIU Q L, et al.In situ XRD and raman investigation of the activation process over K-Cu-Fe/SiO₂ catalyst for fischer-tropsch synthesis reaction[J].Catalysis Letters, 2020, 150(8):2437-2445.
[31]	SÁNCHEZ-VELANDIA J E, AGUDELO-CIFUENTES A, VILLA A L.Kinetics of the isomerization of α-pinene epoxide over Fe supported MCM-41 and SBA-15 materials[J].Reaction Kinetics, Mechanisms and Catalysis, 2019, 128(2):1005-1028.
[32]	JI Y F, FERRONATO C, SALVADOR A, et al.Degradation of ciprofloxacin and sulfamethoxazole by ferrous-activated persulfate:implications for remediation of groundwater contaminated by antibiotics[J].The Science of the Total Environment, 2014, 472:800-808.
[33]	WU J X, WANG B, BLANEY L, et al.Degradation of sulfamethazine by persulfate activated with organo-montmorillonite supported nano-zero valent iron[J].Chemical Engineering Journal, 2019, 361:99-108.
[34]	NIU L, ZHANG G M, XIAN G, et al.Tetracycline degradation by persulfate activated with magnetic γ-Fe₂O₃/CeO₂ catalyst:performance, activation mechanism and degradation pathway[J].Separation and Purification Technology, 2021, 259:118156.
[35]	RUAN Y, KONG L J, ZHONG Y W, et al.Review on the synthesis and activity of iron-based catalyst in catalytic oxidation of refractory organic pollutants in wastewater[J].Journal of Cleaner Production, 2021, 321:128924.
[36]	ZHAO G Q, ZOU J C, CHEN X Q, et al.Iron-based catalysts for persulfate-based advanced oxidation process:microstructure, property and tailoring[J].Chemical Engineering Journal, 2021, 421:127845.
[37]	GUO Y X, YAN L G, LI X G, et al.Goethite/biochar-activated peroxymonosulfate enhances tetracycline degradation:inherent roles of radical and non-radical processes[J].Science Total Environment, 2021, 783:147102.
[38]	SU S S, CAO C J, ZHAO Y P, et al.Efficient transformation and elimination of roxarsone and its metabolites by a new α-FeOOH@GCA activating persulfate system under UV irradiation with subsequent As(Ⅴ) recovery[J].Applied Catalysis B:Environmental, 2019, 245:207-219.
[39]	WANG L, MA X L, HUANG G F, et al.Construction of ternary CuO/CuFe₂O₄/g-C₃N₄ composite and its enhanced photocatalytic degradation of tetracycline hydrochloride with persulfate under simulated sunlight[J].J Environ Sci (China), 2022, 112:59-70.
[40]	FENG Q Q, ZHOU J B, LUO W J, et al.Photo-Fenton removal of tetracycline hydrochloride using LaFeO₃ as a persulfate activator under visible light[J].Ecotoxicology and Environmental Safety, 2020, 198:110661.
[41]	ZHANG Y F, WEI J, XING L Y, et al.Superoxide radical mediated persulfate activation by nitrogen doped bimetallic MOF (FeCo/N-MOF) for efficient tetracycline degradation[J].Separation and Purification Technology, 2022, 282:120124.
[42]	ELBENBERGER H, STEENKEN S, O'NEILL P, et al.Pulse radiolysis and electron spin resonance studies concerning the reaction of SO₄.cntdot.- with alcohols and ethers in aqueous solution[J].Journal of Physical Chemistry, 1978, 82:749-750.
[43]	BUXTON G V, GREENSTOCK C L, HELMAN W P, et al.Critical review of rate constants for reactions of hydrated electrons chemical kinetic data base for combustion chemistry[J].Journal of Physical & Chemical Reference Data, 1988, 17:513-886.
[44]	ANIPSITAKIS P G, DIONYSIOU D D.Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science & Technology, 2004, 38:3705-3712.
[45]	WANG R Y, YU Y J, ZHANG R J, et al.Vacancy-rich structure inducing efficient persulfate activation for tetracycline degradation over Ni-Fe layered double hydroxide nanosheets[J].Separation and Purification Technology, 2022, 289:120663.
[46]	DENG J, XIAO L W, YUAN S J, et al.Activation of peroxymonosulfate by CoFeNi layered double hydroxide/graphene oxide (LDH/GO) for the degradation of gatifloxacin[J].Separation and Purification Technology, 2021, 255:117685.
[47]	HOU L H, LI X M, YANG Q, et al.Heterogeneous activation of peroxymonosulfate using Mn-Fe layered double hydroxide:performance and mechanism for organic pollutant degradation[J].Science of the Total Environment, 2019, 663:453-464.

Relative Articles

[1]	WU Yan, RONG Nai, HAN Long, LIU Kaiwei, WANG Jiuheng, MU Zhengyong, WANG Shanshan, SHI Xiuliang. STEAM HYDRATION ACTIVATION OF CELLULOSE TEMPLATE MODIFIED Ca-BASED CO₂ SORBENT[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(5): 163-171. doi: 10.13205/j.hjgc.202405021
[2]	HUANG Jiming, LIU Runqing, WU Sizhan, QIN Hangdao, CHEN Jing. PREPARATION AND CHARACTERIZATION OF DEFECTIVE Zr-BASED METAL-ORGANIC FRAMEWORKS AND THEIR ADSORPTION PROPERTIES FOR TETRACYCLINE[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(3): 33-40. doi: 10.13205/j.hjgc.202403004
[3]	LENG Jiewen, SHI Ke, WANG Xuejing, KOU Wei, FU Xiaowei, SUN Zhaonan. ADSORPTION OF TETRACYCLINE ON BIOCHAR PREPARED FROM MUNICIPAL SLUDGE[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(5): 75-82. doi: 10.13205/j.hjgc.202405010
[4]	HE Xi, LIU Chen, LI Jinglu, CHEN Ming, B. Larry LI. PERFORMANCE AND MECHANISM OF CSB-BOC ACTIVATED PMS FOR REMOVAL OF TETRACYCLINE HYDROCHLORIDE IN WATER IN SLOW-GATHERING AREAS OF RIVER[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(2): 82-96. doi: 10.13205/j.hjgc.202402010
[5]	CONG Xin, SUN Meizhen, YUAN Xuehong, LI Taolue, XUE Nandong. IRON-BASED NANOMATERIALS MEDIATED BY LEAF EXTRACTS FROM SYCAMORE ACTIVATE PERSULFATES TO CATALYZE TBBPA DEGRADATION IN SOIL[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(5): 107-114. doi: 10.13205/j.hjgc.202305015
[6]	LI Wei, NING Yuyang, LIU Ning, GAO Mingjie. ADSORPTION PERFORMANCE OF PEO-BASED MOFs HYBRID FOAM MATERIALS ON TETRACYCLINE AND Cu²⁺[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(7): 76-85. doi: 10.13205/j.hjgc.202307011
[7]	YAN Yuan, WANG Yajun, CHEN Tianjing, AN Fangjiao. RESPONSE OF THREE PLANTS TO TETRACYCLINE POLLUTION STRESS IN BIORETENTION CELL[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(8): 65-74. doi: 10.13205/j.hjgc.202308009
[8]	YANG Jiani, ZHAO Baowei, YANG Maoying, SUO Jinmiao, ZHU Zhengyu, DENG Aiqin. PREPARATION OF Fe/C CATALYST BASED ON FERRIC CITRATE AND ITS ACTIVATION PERFORMANCE ON PEROXYDISULFATE TO DEGRADE SULFADIAZINE[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(7): 116-123,251. doi: 10.13205/j.hjgc.202307016
[9]	ZHANG Shicheng, LI Simin, ZHU Jia. DEGRADATION OF METHYL ORANGE BY CuO/g-C₃N₄ ACTIVATED PEROXODISULFATE[J]. ENVIRONMENTAL ENGINEERING , 2022, 40(10): 40-48. doi: 10.13205/j.hjgc.202210006
[10]	SUN Li-hua, MEI Xiao-yu, GAO Cheng, FENG Cui-min. MECHANISMS AND EFFICIENCY OF REMOVAL OF ORGANIC MATTER AND ANTIBIOTIC RESISTANCE GENES IN SECONDARY EFFLUENT OF WATARPLANTS BY DIFFERENT PERSULFATE ACTIVATION METHODS[J]. ENVIRONMENTAL ENGINEERING , 2022, 40(9): 74-80,134. doi: 10.13205/j.hjgc.202209010
[11]	GUO Zhi-wei, ZHAO Bao-long, ZHENG Zhi-hong, HONG Fei-yu, XIN Si-yuan, WANG Xiao-wei, WANG Xing-xiao, ZHANG Zhen-zhen, NIU Fang, LI Guo-ting. PREPARATION OF MODIFIED DIATOMITE VIA CARBONIZATION AND ITS ADSORPTION PERFORMANCE ON TETRACYCLINE[J]. ENVIRONMENTAL ENGINEERING , 2022, 40(5): 44-52. doi: 10.13205/j.hjgc.202205007
[12]	LIAO Quan, LUO Hua-yong, RONG Hong-wei, CHEN Bing-wei, LIANG Ying. ADSORPTION PERFORMANCE OF TETRACYCLINE ONTO NANO-ALUMINA MODIFIED GEL BEADS[J]. ENVIRONMENTAL ENGINEERING , 2020, 38(9): 36-42. doi: 10.13205/j.hjgc.202009006
[13]	XU Rui, YANG Wei, YANG Zhe, CHENG Qian-lan, GU Li-ting, GUO Sheng. HIGH-EFFICIENT REMOVAL OF TETRACYCLINE HYDROCHLORIDE BASED ON PEROXYMONOSULFATE ACTIVATED BY CuO/EXPANDED GRAPHITE COMPOSITE[J]. ENVIRONMENTAL ENGINEERING , 2020, 38(2): 48-54,47. doi: 10.13205/j.hjgc.202002006

Supplements(0)

Cited By

Cited by

Periodical cited type(2)

1.	赵凯，孟宪荣，余浪，武冕，许伟，滕振兴，刘阳，施维林. Fe-MCM-41改性及其催化过硫酸盐对地下水中恩诺沙星去除效果. 环境科学学报. 2025(02): 59-68 .
2.	闫兴雨，王艳，王善虎，莫原野，许伟，刘阳，孟宪荣，施维林. 金属-硅核壳结构诱导强化nZVI@SiO_2/PDS体系降解地下水氯苯. 环境科学学报. 2024(02): 125-135 .

Other cited types(1)

Proportional views

Proportional views

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Get Citation

PDF

XML

Article Metrics

Article views (117) PDF downloads(3)