|
|
|
| Degradation of sulfadiazine by hydroxylamine hydrochloride/Fe-MOFs/persulfate system |
| WU Cheng-zi1,2,3, ZHANG Wei1,2,3, WAN Yan-tao1,2,3, XIU Guang-li1,2,3 |
1. State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237;
2. Shanghai Key Laboratory of Environmental Standards and Risk Management of Chemical Pollutants, Shanghai 200237;
3. Shanghai Institute of Pollution Control and Ecological Safety, Shanghai 200092, China |
|
|
|
|
Abstract Hydroxylamine hydrochloride was used to promote Fe(Ⅲ)/Fe(Ⅱ) cycle in iron-based metal organic framework (Fe-MOFs)/persulfate(PS) system to degrade sulfadiazine (SDZ) in water. The structure and morphology of Fe-MOFs were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The influence of initial pH, PS, Fe-MOFs, HA, SDZ, co-existing ions and humic acid on the removal of SDZ were investigated and the prospect for practical application of this system was also evaluated. The results showed that Fe-MOFs/PS/HA system had a good removal performance of SDZ in a wide initial pH range (3~6), and the removal of SDZ at 180min reached above 90.1%. The appropriate amount of HA could promote the degradation of SDZ in Fe-MOFs/PS system. The results of the free radical scavenging and electron paramagnetic resonance experiments showed that the SO4-·、·OH、O2-· and 1O2 were produced in the Fe-MOFs/PS/HA system during the degradation process of SDZ. Within the experiment scope of this study, the degradation performance of SDZ by Fe-MOFs/PS/HA system decreased gradually with the increase of pH value in the range of (pH=3~6). With the increase of the concentration of PS, HA and Fe-MOFs, the removal of SDZ exhibited the rising-then-falling pattern. Chlorine ion, humic acid and other factors had the negative effects on the removal of SDZ in the system in actual surface water, however HA could enhance the degradation of SDZ in the natural environment. The result of recycle experiment revealed that Fe-MOFs system had a good reusability and exhibited a great application potential.
|
|
Received: 17 October 2020
|
|
|
|
|
|
| [1] |
秦丽婷,童蕾,刘慧,等.环境中磺胺类抗生素的生物降解及其抗性基因污染现状[J].环境化学, 2016,35(5):875-883. Qin L T, Tong L, Liu H, et al. Biodegradation of sulfonamides and the pollution characteristics of sulfonamide resistance genes in the environment[J]. Environmental Chemistry, 2016,35(5):875-883.
|
| [2] |
Zhang Q, Ying G, Pan G, et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science & Technology, 2015,49(11):6772-6782.
|
| [3] |
Xiao S, Cheng M, Zhong H, et al. Iron-mediated activation of persulfate and peroxymonosulfate in both homogeneous and heterogeneous ways:A review[J]. Chemical Engineering Journal, 2020,384:123265.
|
| [4] |
Haldar D, Duarah P, Purkait M K. MOFs for the treatment of arsenic, fluoride and iron contaminated drinking water:A review[J]. Chemosphere, 2020,251:126388.
|
| [5] |
Pu M J, Guan Z Y, Ma Y W, et al. Synthesis of iron-based metal-organic framework MIL-53 as an efficient catalyst to activate persulfate for the degradation of Orange G in aqueous solution[J]. Applied Catalysis A:General, 2018,549:82-92.
|
| [6] |
Li X H, Guo W L, Liu Z H, et al. Quinone-modified NH2-MIL-101(Fe) composite as a redox mediator for improved degradation of bisphenol A[J]. Journal of Hazardous Materials, 2017,324:665-672.
|
| [7] |
Li J, Wan Y J, Li Y J, et al. Surface Fe(III)/Fe(II) cycle promoted the degradation of atrazine by peroxymonosulfate activation in the presence of hydroxylamine[J]. Applied Catalysis B:Environmental, 2019,256:117782.
|
| [8] |
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, 2019,377:62-69.
|
| [9] |
Pu M J, Ma Y W, Wan J Q, et al. Activation performance and mechanism of a novel heterogeneous persulfate catalyst:metal-organic framework MIL-53(Fe) with FeII/FeIII mixed-valence coordinatively unsaturated iron center[J]. Catalysis Science & Technology, 2017,7(5):1129-1140.
|
| [10] |
Wan Y J, Wan J Q, Ma Y W,et al. Sustainable synthesis of modulated Fe-MOFs with enhanced catalyst performance for persulfate to degrade organic pollutants[J]. Science of the Total Environment, 2020,701:134806.
|
| [11] |
Luo LS, Yao Y Y, Gong F, et al. Drastic enhancement on Fenton oxidation oforganic contaminants by accelerating Fe(III)/Fe(II)cycle with L-cysteine[J]. Royal Society of Chemistry Advance, 2016,6:47661-47668.
|
| [12] |
Hou X J, Huang X P, Ai Z H, et al. Ascorbic acid/Fe@Fe2O3:A highly efficient combined Fenton reagent to remove organic contaminants.[J]. Journal of Hazardous Materials, 2016,310:170-178.
|
| [13] |
Bloch E D, Murray L J, Queen W L, et al. Selective binding of O2 over N2 in a redox-active metal-organic framework with open iron(II) coordination sites[J]. Journal of the American Chemical Society, 2011,133(37):14814-14822.
|
| [14] |
Tamura H, Goto K, Yotsuyanagi T, et al. Spectrophotometric determination of iron(II) with 1,10-phenanthroline in the presence of large amounts of iron(II)[J]. Talanta, 1974,21(4):314-318.
|
| [15] |
Chi H Y, Wan J Q, Ma Y W, et al. Ferrous metal-organic frameworks with stronger coordinatively unsaturated metal sites for persulfate activation to effectively degrade dibutyl phthalate in wastewater[J]. Journal of Hazardous Materials, 2019,377:163-171.
|
| [16] |
Huang S, Yang K L, Liu X F, et al. MIL-100(Fe)-catalyzed efficient conversion of hexoses to lactic acid[J]. Royal Society of Chemistry Advance, 2017,7:5621-5627.
|
| [17] |
Guo W Q, Zhao Q, Du J S, et al. Enhanced removal of sulfadiazine by sulfidated ZVI activated persulfate process:Performance, mechanisms and degradation pathways[J]. Chemical Engineering Journal, 2020, 388:124303.
|
| [18] |
Miao Z W, Gu X G, Lu S G, et al. Enhancement effects of reducing agents on the degradation of tetrachloroethene in the Fe(II)/Fe(III) catalyzed percarbonate system[J]. Journal of Hazardous Materials, 2015,300:530-537.
|
| [19] |
Guo Y, Zhang Y X, Yu G, et al. Revisiting the role of reactive oxygen species for pollutant abatement duringcatalytic ozonation:The probe approach versus the scavenger approach[J]. Applied Catalysis B:Environmental, 2020,280:119418.
|
| [20] |
Chen X, Guo H G, Li W, et al. Metal-free carbocatalysis for persulfate activation toward nonradical oxidation:Enhanced singlet oxygen generation based on active sites and electronic property[J]. Chemical Engineering Journal, 2020,396:125107.
|
| [21] |
Kamagatea M, Assadi A A, Kone T, et al. Activation of persulfate by irradiated laterite for removal of fluoroquinolones in multi-component systems[J]. Journal of Hazardous Materials, 2018,346:159-166.
|
| [22] |
Keith P M, Hitoshi T. The role of the DMPO-hydrated electron spin adduct in DMPO-·OH spin trapping[J]. Free Radical Biology and Medicine, 2001,30(12):1374-1380.
|
| [23] |
Xu Y Y, Wang Y, Wan J Q, et al. Reduced graphene oxide-supported metal organic framework as a synergistic catalyst for enhanced performance on persulfate induced degradation of trichlorophenol[J]. Chemosphere, 2020,240:124849.
|
| [24] |
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.
|
| [25] |
Lin C C, Chen Y H. Feasibility of using nanoscale zero-valent iron and persulfate to degrade sulfamethazine in aqueous solutions[J]. Separation and Purification Technology, 2018,194:388-395.
|
| [26] |
Chen L W, Ma J, Li X C, et al. Strong enhancement on fenton oxidation by addition of hydroxylamine to accelerate the ferric and ferrous iron cycles[J]. Environmental Science & Technology. 2011,45:3925-3930.
|
| [27] |
Jin Y Y, Sun S P, Yang X Y, et al. Degradation of ibuprofen in water by Fe(II) -NTA complex-activated persulfate with hydroxylamine at neutral pH[J]. Chemical Engineering Journal, 2018,337:152-160.
|
| [28] |
Zhuo Y L, Lu W, Yu L L, et al. Unraveling the interaction of hydroxylamine and Fe(III) in Fe(II)/Persulfate system:A kinetic and simulating study[J]. Water Research, 2020,168:115093.
|
| [29] |
Zhou L, Zhang Y, Ying R, et al. Thermoactivated persulfate oxidation of pesticide chlorpyrifos in aquatic system:kinetic and mechanistic investigations[J]. Environmental Science and Pollution Research, 2017,24(12):11549-11558.
|
| [30] |
Yang Y, Pignatello J J, Ma J, et al. Comparison of halide impacts on the efficiency ofcontaminant degradation by sulfate and hydroxyl radical-based advanced oxidationprocesses (aops)[J]. Environmental Science & Technology, 2014,48(4):2344-2351.
|
| [31] |
Zuo Z, Cai Z, Katsumura Y, et al. Reinvestigation of the acid-base equilibrium of the (bi) carbonate radical and ph dependence of its reactivity with inorganic reactants[J]. Radiation Physics and Chemistry, 1999,55(1):15-23.
|
| [32] |
Valentine R L, Wang H A. Iron oxide surface catalyzed oxidation of quinoline by hydrogen peroxide[J]. Journal of Environmental Engineering, 1998,124(1):31-38.
|
| [33] |
Hou X J, Huang X P, Li M L,et al. Fenton oxidation of organic contaminants with aquifer sediment activatedby ascorbic acid[J]. Chemical Engineering Journal, 2018,348:255-262.
|
| [34] |
Zhou Y X, Shi J Q,Li Y P, et al. Degradation kinetics and mechanism of bis(2-chloroethyl) ether by electromagnetic induction electrodeless lamp activated persulfate[J]. Chemosphere, 2020,261:127709.
|
| [35] |
Liu H, Chen J, Wu N, et al. Oxidative degradation of chlorpyrifos using ferrate(VI):Kinetics and reaction mechanism[J]. Ecotoxicology and Environmental Safety, 2019,170:259-266.
|
| [36] |
Li X J, Liao F Z, Ye L M, et al. Controlled pyrolysis of MIL-88A to prepare iron/carbon composites for synergistic persulfate oxidation of phenol:Catalytic performance and mechanism[J]. Journal of Hazardous Materials, 2020,398:122938.
|
| [37] |
Liu T, Wu K, Wang M, et al. Performance and mechanisms of sulfadiazine removal using persulfate activated by Fe3O4@CuOX hollow spheres[J]. Chemosphere, 2021,262:127845.
|
| [38] |
Zou X L, Zhou T, Mao J, et al.Synergistic degradation of antibiotic sulfadiazine in a heterogeneousultrasound-enhanced Fe0/persulfate Fenton-like system[J]. Chemical Engineering Journal, 2014,257:36-44.
|
| [39] |
Feng Y, Wu D L, Liao C Z, et al. Red mud powders as low-cost and efficient catalysts for persulfateactivation:Pathways and reusability of mineralizing sulfadiazine[J]. Separation and Purification Technology, 2016,167:136-145.
|
| [40] |
王楠楠, 张巍, 修光利. MIL-88B(Fe)非均相芬顿催化降解磺胺甲恶唑[J]. 环境污染与防治, 2020,42(6):682-689.Wang N N, Zhang W, Xiu G L. Heterogeneous Fenton catalyzed degradation of sulfamethoxazole by MIL-88B(Fe)[J]. Environmental Pollution & Control, 2020,42(6):682-689.
|
|
|
|
