Abstract：The magnetic sandwich composite Fe3O4@MXene was prepared to activate peroxymonosulfate (PMS) for removing Bisphenol A(BPA) from water. The effects of PMS dosage, Fe3O4@MXene dosage, initial solution pH value and initial BPA concentration on BPA degradation were investigated. The results show that the degradation of BPA conformed to the quasi-first order reaction kinetics. At 25℃, the combination of Fe3O4@MXene dosage of 0.3g/L, PMS dosage of 1.01g/L and initial pH of 6.0could degrade 97.4% of BPA (25mg/L) after 90-minute, in which hydroxyl radical and sulfate radical were the dominant reactive oxygen species for BPA degradation despite having singlet oxygen involved. The MXene-supported Fe3O4 particles showed a uniform size distribution with obviously improved activity and stability. The Ti atoms on the surface of MXene helped accelerate the Fe(II)/Fe(III) redox cycle, which thus improved PMS activation. Evidently, the Fe3O4@MXene can be used as an ideal heterogeneous catalyst for the advanced oxidation process of persulfate.
周宇辉, 林洋仟, 王御豪, 杨盈, 徐西蒙. 磁性复合材料活化过硫酸盐去除水中双酚A[J]. 中国环境科学, 2024, 44(2): 832-840.
ZHOU Yu-hui, LIN Yang-qian, WANG Yu-hao, YANG Ying, XU Xi-meng. Removing bisphenol A with magnetic sandwich composite activated peroxymonosulfate. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(2): 832-840.
Lee J, Gunten U V, Kim J H. Persulfate-based Advanced Oxidation:Critical Assessment of Opportunities and Roadblocks [J]. Environmental Science and Technology, 2020,54:3064−3081.
[2]
Gao Y, Zhu Y, Chen Z, et al. Nitrogen-coordinated cobalt embedded in a hollow carbon polyhedron for superior catalytic oxidation of organic contaminants with peroxymonosulfate [J]. Environmental Science and Technology, 2021,1,1:76−85.
[3]
Liu L, Liu Q, Wang Y, et al. Nonradical activation of peroxydisulfate promoted by oxygen vacancy-laden NiO for catalytic phenol oxidative polymerization [J]. Applied Catalysis B:Environmental, 2019,254:166−173.
[4]
Hu J, Zeng X, Wang G, et al. Modulating mesoporous Co3O4 hollow nanospheres with oxygen vacancies for highly efficient peroxymono-sulfate activation [J]. Chemical Engineering Journal, 2020,400:125869.
[5]
Oh W D, Dong Z L, Lim T T. Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal:Current development, challenges and prospects [J]. Applied Catalysis B:Environmental, 2016,194:169−201.
[6]
Huang G X, Wang C Y, Yang C W, et al. Degradation of Bisphenol A by Peroxymonosulfate Catalytically Activated with Mn1.8Fe1.2O4 Nanospheres:Synergism between Mn and Fe [J]. Environmental Science & Technology, 2017,51(21):12611-12618.
[7]
Zou J, Ma J, Chen L W. Rapid Acceleration of Ferrous Iron/PeroxymonosuSfate Oxidation of Organic Pollutants by Promoting Fe(lll)/Fe(ll) Cycle with Hydroxylamine [J]. Environmental Science and Technology, 2013,47(20):11685-11691.
[8]
Oh W D, Lua S K, Dong Z L, et al. High surface area DPA-hematite for efficient detoxification of bisphenol A via peroxymonosulfate activation [J]. Journal of Materials Chemistry A, 2014,32:15836.
[9]
Liu J, Zhou J, Ding Z, et al. Ultrasound irritation enhanced heterogeneous activation of peroxymonosulfate with Fe3O4 for degradation of azo dye [J]. Ultrasonics Sonochemistry, 2017,34:953-959.
[10]
Kwan W P, Voelker B M. Rates of hydroxyl radical generation and organic compound oxidation in mineral-catalyzed fenton-like systems [J]. Environmental Science & Technology, 2003,37(6):1150-1158.
[11]
Munoz M, Pedro Z D, Casas J A, et al. Preparation of magnetite-based catalysts and their application in heterogeneous Fenton oxidation-A review [J]. Applied Catalysis B Environmental, 2015,176-177:249-265.
[12]
Matta R, Hanna K, Chiron S. Fenton-like oxidation of 2, 4, 6-trinitrotoluene using different iron minerals [J]. Science of the Total Environment, 2007,385:242-251.
[13]
Hanna K, Kone T, Medjahdi G. Synthesis of the mixed oxides of iron and quartz and their catalytic activities for the Fenton-like oxidation [J]. Catalysis Communications, 2008,9:955-959.
[14]
Yin J J, Ge B C, Jiao T F, et al. Self-Assembled sandwich-like MXene-Derived composites as highly efficient and sustainable catalysts for wastewater treatment [J]. Langmuir, 2021,37:1267-1278.
[15]
刘超,李茜,郝丽芬,等.MXene的功能化改性及其应用研究进展[J]. 复合材料学报, 2021,38(4):1020-1028. Liu C, Li X, Hao L F, et al. Research progress of functional modification of MXene and its applications [J]. Acta Materiae Compositae Sinica, 2021,38(4):1020-1028.
[16]
Zhang W, Ma J, Zhang W J. A multidimensional nano-structural design towards electrochemically stable and mechanically strong hydrogel electrodes [J]. Nanoscale, 2020,12(12):6637-6643.
[17]
Qi Q, Zhang H, Zhang P, et al. Self-assembled sandwich hollow porous carbon sphere@MXene composites as superior Li-S battery cathode hosts [J]. 2D Materials, 2020,7(2):25-49.
[18]
Karthikeyan P, Ramkumar K, Pandi K, Effective removal of Cr(VI) and methyl orange from the aqueous environment using two-dimensional (2D) Ti3C2Tx MXene nanosheets [J]. Ceramics International, 2021,47:3692-3698.
[19]
Zhang Z H, Xu J Y, Yang X L. MXene/sodium alginate gel beads for adsorption of methylene blue [J]. Materials Chemistry and Physics, 2021,260:124123.
[20]
Zhang Q R, Teng J, Zou G D, et al. Efficient phosphate sequestration for water purification by unique sandwich-like MXene/magnetic iron oxide nanocomposites [J]. Nanoscale, 2016,8:7085-7093.
[21]
Song H R, Zu D Y, Li C P, et al. Ultrafast activation of peroxymonosulfate by reduction of trace Fe3+ with Ti3C2MXene under neutral and alkaline conditions:Reducibility and confinement effect [J]. Chemical Engineering Journal, 2021,423:130012.
[22]
Wang L, Song H, Yuan L Y, et al. Effective removal of anionic Re(VII) by surface-modified Ti2CTx MXene nanocomposites:implications for Tc(VII) sequestration [J]. Environmental Science & Technology, 2019, 53:3739-3747.
[23]
Yang Z C, Shan C, Pan B C, et al. The Fenton reaction in water assisted by picolinic acid:accelerated iron cycling and co-generation of a selective Fe-based oxidant [J]. Environmental Science & Technologyl, 2021,55(12):8299-8308.
[24]
Wang Y S, Li Y Y, Qiu Z P, et al. Fe3O4@Ti3C2MXene hybrids with ultrahigh volumetric capacity as an anode material for lithium-ion batteries [J]. Journal of Materials Chemistry A, 2018,6:11189-11197.
[25]
Song H R, Zu D Y, Li C P, et al. Ultrafast activation of peroxymonosulfate by reduction of trace Fe3+ with Ti3C2MXene under neutral and alkaline conditions:Reducibility and confinement effect [J]. Chemical Engineering Journal, 2021,423:130012.
[26]
Wang L, Song H, Yuan L Y, et al. Effective removal of anionic Re(VII) by surface-modified Ti2CTx MXene nanocomposites:implications for Tc(VII) sequestration [J]. Environmental Science & Technology, 2019,53:3739-3747.
[27]
Xu X M, Chen W M, Zong S Y, et al. Atrazine degradation using Fe3O4-sepiolite catalyzed persulfate:Reactivity, mechanism and stability [J]. Journal of Hazardous Materials, 2019,377(5):62-69.
[28]
Xu X M, Zong S Y, Chen W M, et al. Heterogeneously catalyzed binary oxidants system with magnetic fly ash for the degradation of bisphenol A [J]. Chemical Engineering Journal, 2019,360:1363-1370.
[29]
Xu X M, Zong S Y, Chen W M, et al. Comparative study of Bisphenol A degradation via heterogeneously catalyzed H2O2 and persulfate:Reactivity, products, stability and mechanism [J]. Chemical Engineering Journal, 2019,360:470-479.
[30]
Xu X M, Chen W M, Zong S Y, et al. Magnetic clay as catalyst applied to organics degradation in a combined adsorption and Fenton-like process [J]. Chemical Engineering Journal, 2019,373:140-149.
[31]
Xu X M, Zhou Y H, Li S S, et al. Activation of sodium percarbonate with Fe3O4@MXene composite for the efficient removal of bisphenol A [J]. Journal of Environmental Chemical Engineering, 2022,10:108702.
[32]
Qi C, Liu X, Ma J, et al. Activation of peroxymonosulfate by base:Implications for the degradation of organic pollutants [J]. Chemosphere, 2016,151:280-288.
[33]
Lei Y, Yu Y F, Lei X, et al. Assessing the use of probes and quenchers for understanding the reactive species in advanced oxidation processes [J]. Environmental Science & Technology, 2023,57:5433-5444.
[34]
Zhang Q H, He D, Li X R, et al. Mechanism and performance of singlet oxygen dominated peroxymonosulfate activation on CoOOH nanoparticles for 2,4-dichlorophenol degradation in water [J]. Journal of Hazardous Materials, 2020,384:12135.
