硅藻土负载MnFe<sub>2</sub>O<sub>4</sub>纳米颗粒活化PMS降解金橙Ⅱ

张理军; 严群; 周子琳; 陈燕; 陈锦富

doi:10.13205/j.hjgc.202211009

硅藻土负载MnFe₂O₄纳米颗粒活化PMS降解金橙Ⅱ

doi: 10.13205/j.hjgc.202211009

张理军^1,3,
严群^2, ,,
周子琳²,
陈燕¹,
陈锦富²

1. 江西理工大学资源与环境工程学院, 江西赣州 341000;
2. 江西理工大学土木与测绘工程学院, 江西赣州 341000;
3. 江西理工大学赣江流域水质安全保障工程技术研究中心, 江西赣州 341000

详细信息

作者简介:
张理军(1997-),男,硕士,主要研究方向为水污染控制理论与污水资源化利用。995758417@qq.com

通讯作者:
严群(1973-),女,博士,副教授,主要研究方向为水污染控制理论与资源化。1068630@qq.com

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出版历程
- 收稿日期: 2022-03-08
- 网络出版日期: 2023-03-24

NANOPARTICLES SUPPORTED BY DIATOMITE FOR REMOVAL OF ORANGE Ⅱ THROUGH ACTIVATING PMS

1. School of Resources and Environmental Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China;
2. School of Civil and Surveying&Mapping Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China;
3. Research Center for Water Quality Security Technology at Ganjiang River Basin, Jiangxi University of Science and Technology, Ganzhou 341000, China

摘要

摘要: 采用溶胶-凝胶法制备硅藻土/MnFe₂O₄复合型催化剂（DMF），以金橙Ⅱ为目标污染物，分析DMF活化过一硫酸盐（PMS）的性能和作用机制。结果表明：1） MnFe₂O₄颗粒均匀负载于硅藻土上，使DMF具有更好的分散性和活化性；2） DMF对PMS的活化能力优于单一MnFe₂O₄，DMF （1：1）/PMS体系降解金橙Ⅱ符合准一级动力学模型，且降解速率是MnFe₂O₄/PMS体系的2.16倍，0.5 g/L DMF和0.5 mmol/L PMS在40 min内对50 mg/L金橙Ⅱ降解率达到93.1%；3）反应体系中存在·OH、SO₄^-·、¹O₂、·O₂^- 4种活性物种，其中·OH和SO₄^-·起主导作用；4） DMF复合材料具有更好的结构稳定性，金属离子溶出量远低于MnFe₂O₄。研究结果可为新型高效PMS催化剂在处理工业废水的实际应用提供参考。
- 高级氧化 /
- MnFe₂O₄ /
- 硅藻土 /
- 过一硫酸盐 /
- 金橙Ⅱ MnFe₂O₄
Abstract: Diatomite/MnFe₂O₄ composite catalyst (DMF) was rationally synthesized by sol-gel method. The performance and reaction mechanism of DMF activated peroxymonosulfate (PMS) were degraded with orange Ⅱ as the target pollutant. The results showed that:1) MnFe₂O₄ particles were uniformly loaded on diatomite and DMF had better dispersion and stability; 2) DMF had a better catalytic activity to PMS than MnFe₂O₄ so that the degradation rate of DMF/PMS system for orange Ⅱ removal was 2.16 times that of MnFe₂O₄ system, the reaction process could be fitted by the pseudo-first-order kinetic pattern. A degradation rate of 93.1% could be achieved within 40 min for 50 mg/L AO₂ by 0.5 g/L DMF and 0.5 mmol/L PMS; 3) there were four active radicals ·OH、SO₄^-·、¹O₂ and ·O₂^- in the reaction system, and OH and SO₄^- play the main role; 4) DMF had better structural stability and its metal ion dissolution was much lower than MnFe₂O₄. This study paved a way for the practical application of the new PMS activators in industrial wastewater treatment.
- advanced oxidation /
- MnFe₂O₄ /
- diatomite /
- peroxymonosulphate /
- orange Ⅱ

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参考文献(29)

[1]	MERCYRAN B, HERNANDEZ-MAYA R, SOLÍS-LÓPEZ1 M, et al. Photocatalytic degradation of Orange G using TiO₂/Fe₃O₄ nanocomposites[J]. Journal of Materials Science:Materials in Electronics, 2018, 29(8):15436-15444.
[2]	HU L X, DENG G H, LU W C, et al. Peroxymonosulfate activation by Mn₃O₄/metal-organic framework for degradation of refractory aqueous organic pollutant rhodamine B[J]. Chinese Journal of Catalysis, 2017, 38(8):1360-1372.
[3]	OLMEZ-HANCI T, ARSLAN-ALATON I. Comparison of sulfate and hydroxyl radical based advanced oxidation of phenol[J].Chemical Engineering Journal, 2013, 224(1):10-16.
[4]	XU Y, AI J, ZHANG H. The mechanism of degradation of bisphenol A using the magnetically separable CuFe₂O₄/peroxymonosulfate heterogeneous oxidation process[J]. Journal of Hazardous Materials, 2016, 309:87-96.
[5]	SHAO S, QIAN L, ZHAN X, et al. Transformation and toxicity evolution of amlodipine mediated by cobalt ferrite activated peroxymonosulfate:effect of oxidant concentration[J]. Chemical Engineering Journal, 2020, 382:123005.
[6]	XIONG C Y, REN Q F, CHEN S H, et al. A multifunctional Ag₃PO₄/Fe₃O₄/Diatomite composites:photocatalysis, adsorption and sterilization[J]. Materials Today Communications, 2021, 28:102695.
[7]	KHRAISHEH M A, AL-GHOUTI M A, ALLEN S J. Effect of OH and silanol groups in the removal of dyes from aqueous solution using diatomite[J]. Water Research, 2005, 39(5):922-932.
[8]	DONG X D, SUN Z M, ZHANG X W, et al. Synthesis and enhanced solar light photocatalytic activity of a C/N Co-doped TiO₂/diatomite composite with exposed (001) facets[J]. Australian Journal of Chemistry, 2018, 71:315-324.
[9]	WANG B, ZHANG G X, LENG X, et al, Characterization and improved solar light activity of vanadium doped TiO₂/diatomite hybrid catalysts[J]. Journal of Hazardous Materials, 2015, 285:212-220.
[10]	TAN C Q, GAO N Y, FU D F, et al. Efficient degradation of paracetamol with nanoscaled magnetic CoFe₂O₄ and MnFe₂O₄ as a heterogeneous catalyst of peroxymonosulfate[J]. Separation and Purification Technology, 2017, 175:47-57.
[11]	石清清,蒲生彦,杨犀.纳米Cu₀@Fe₃O₄活化PMS降解对-硝基苯酚的协同反应机制[J]. 环境科学, 2020, 41(10):4616-4625.
[12]	ZHANG Z L, WANG Y, TAN Q Q, et al. Facile solvothermal synthesis of mesoporous manganese ferrite (MnFe₂O₄) microspheres as anode materials for lithium-ion batteries[J]. Journal of Colloid and Interface Science, 2013, 398:185-192.
[13]	TAN C Q, GAO N Y, DENG Y, et al. Radical induced degradation of acetaminophen with Fe₃O₄ magnetic nanoparticles as heterogeneous activator of peroxymonosulfate[J]. Journal of Hazardous Materials, 2014, 276:442-460.
[14]	DATSKO T Y, ZELENTSOV V I, DATSKO E E, et al. Physicochemical and adsorption-structural properties of diatomite modified with aluminum compounds[J]. Surface Engineering and Applied Electrochemistry, 2011, 47(6):530-539.
[15]	HU Z B, ZHENG S L, JIA M Z, et al. Preparation and characterization of novel diatomite/ground calcium carbonate composite humidity control material[J]. Separation and Purification Technology. Advanced Powder Technology, 2017, 28(5):1372-1381.
[16]	FENG Y, WU D L, DENG Y, et al. Sulfate radical-mediated degradation of sulfadiazine by CuFeO₂ rhombohedral crystal-catalyzed peroxymonosulfate:synergistic effects and mechanisms[J]. Environmental Science & Technology, 2016, 50(6):3119-3127.
[17]	LIN C H, SHI D J, WU Z T, et al. CoMn₂O₄ catalyst prepared using the sol-gel method for the activation of peroxymonosulfate and degradation of UV filter 2-phenylbenzimidazole-5-sulfonic acid(PBSA)[J]. Nanomaterials, 2019, 9(5):774.
[18]	TAN Y, LI C Q, SUN Z M, et al. Natural diatomite mediated spherically monodispersed CoFe₂O₄ nanoparticles for efficient catalytic oxidation of bisphenol A through activating peroxymonosulfate[J]. Chemical Engineering Journal, 2020, 388:124386.
[19]	GUAN Y H, MA J, REN Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Reseach, 2013, 47(14):5431-5438.
[20]	HUANG G X, WANG C Y, YANG C W, et al. Degradation of bisphenol a by peroxymonosulfate catalytically activated with Mn_1.8Fe_1.2O₄ nanospheres:synergism between Mn and Fe[J]. Environmental Science & Technology, 2017, 51(21):12611-12618.
[21]	PAN Y, SU H R, ZHU Y T, et al. CaO₂ based Fenton-like reaction at neutral pH:accelerated reduction of ferric species and production of superoxide radicals[J]. Water Research, 2018, 145:731-740.
[22]	DUAN P J, MA T F, YUE Y. Fe/Mn nanoparticles encapsulated in nitrogen-doped carbon nanotubes as a peroxymonosulfate activator for acetamiprid degradation[J]. Environmental Science:Nano, 2019, 6(6):1799-1811.
[23]	YANG S S, WUA P X, LIU J Q, et al. Efficient removal of bisphenol A by superoxide radical and singlet oxygen generated from peroxymonosulfate activated with Fe⁰-montmorillonite[J]. Chemical Engineering Journal, 2018, 350:484-495.
[24]	DONG X B, REN B X, SUN Z M, et al. Monodispersed CuFe₂O₄ nanoparticles anchored on natural kaolinite as highly efficient peroxymonosulfate catalyst for bisphenol A degradation[J]. Applied Catalysis B:Environmental, 2019, 253:206-217.
[25]	DENG J, FENG S F, MA X Y, et al. Heterogeneous degradation of Orange Ⅱ with peroxymonosulfate activated by ordered mesoporous MnFe₂O₄[J]. Separation and Purification Technology, 2016, 167:181-189.
[26]	GUAN Y H, MA J, LI X C, et al. Influence of pH on the Formation of Sulfate and Hydroxyl Radicals in the UV/Peroxymonosulfate System[J]. Environmental Science & Technology, 2011, 45(21):9308-9314.
[27]	FU H C, MA S L, ZHAO P, et al. Activation of peroxymonosulfate by graphitized hierarchical porous biochar and MnFe₂O₄ magnetic nanoarchitecture for organic pollutants degradation:structure dependence and mechanism[J]. Chemical Engineering Journal, 2019, 360:157-170.
[28]	MA W J, WANG N, DU Y C, et al. One-step synthesis of novel Fe₃C@nitrogen-doped carbon nanotubes/graphene nanosheets for catalytic degradation of Bisphenol A in the presence of peroxymonosulfate[J]. Chemical Engineering Journal, 2019, 356:1022-1031.
[29]	ANIPSITAKIS G P, DIONYSIOU D D, GONZALEZ M A. Cobalt-mediated activation of peroxymonosulfate and sulfate radical attack on phenolic compounds:implications of chloride ions[J]. Environmental Science & Technology, 2006, 40(3):1000-1007.