Enhanced photocatalysis using metal-organic framework MIL-101(Fe) for crude oil degradation in oil-polluted water
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摘要: 利用溶剂热法合成了一种稳定的金属有机框架（MOF）MIL-101（Fe），并作为一种新型光催化剂提高了油田废水中原油的降解性能。通过对反应条件的优化，确定了以下最佳参数：暗反应时间为30 min，光反应时间为30 min，pH值为5.5，催化剂量为150 mg/L，反应温度为303.15 K。在这些反应条件下，去除率达到了94.73%。本研究是铁基MOFs在油田废水光催化降解中的应用。MIL-101（Fe）在温和的酸性条件下表现出良好的稳定性，并且可以有效地循环利用。这些发现为利用MIL-101（Fe）作为一种很有前途的工业应用材料，通过光催化降解从受油污染的水中去除原油提供了有价值的见解。Abstract: A stable metal-organic framework (MOF), MIL-101(Fe), was successfully synthesised using a solvothermal method and employed as a novel photocatalyst for degrading crude oil in oilfield wastewater. Through optimisation of reaction conditions, the following optimal parameters were determined: a dark reaction time of 30 min, a light reaction time of 30 min, a pH of 5.5, a catalyst amount of 150 mg/L, and a reaction temperature of 303.15 K. Under these reaction conditions, an impressive removal of 94.73% was achieved. This study represents the first application of Fe-based MOFs in the photocatalytic degradation of oilfield wastewater. MIL-101(Fe) notably demonstrated excellent stability under mild acid conditions and can be efficiently recycled. These findings offer valuable insights into using MIL-101(Fe) as a promising material for industrial applications in removing crude oil from oil-polluted water through photocatalytic degradation.
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Key words:
- MIL-101(Fe) /
- MOF /
- photocatalysis /
- solvothermal /
- oilfield wastewater /
- degradation
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Figure 8 Degradation of crude oil using MIL-101(Fe) under different conditions (catalyst+light, only catalyst, and only light)
Figure 9 Photocatalytic degradation of crude oil using MIL-101(Fe) in the initial state
Figure 10 Removal rate of crude oil in the MOF-photo-Fenton system under different conditions ((a) effect of reaction time, (b) and (c) effect of pH, (d) effect of catalyst dosage, (e) effect of temperature)
Figure 11 Experimental kinetic analysis of photocatalytic degradation of crude oil using MIL-101(Fe) under optimum conditions
Figure 12 (a) Recyclability and stability of MIL-101(Fe), (b) XRD of MIL-101(Fe) before and after reaction, (c) SEM of MIL-101(Fe) after reaction
Figure 13 Capture experiments to investigate the generation of active species behind MIL-101(Fe) in the photocatalytic degradation of crude oil
Figure 14 (a) EIS spectra of MIL-101(Fe), (b) Plots of Intensity versus Binding Energy using MIL-101(Fe)
Table 1 Summary of research on photocatalytic degradation of oily wastewater by various catalysts
Photocatalyst Activator
amount/gPollutant Concentration Dose of
pollutant/mLSource of
irradiationTime/
minMaximum
degradation/
adsorptionRef. MIL-101(Fe) 0.015 OPW 5.0×10−4 60 UV 30 94.73 this paper TiO2-SiO2 0.16 OPW 1.0×10−4 400 UV 30 95 [19] Ce/Bi2O3 10.51 OPW 5.0×10−5 2000 Visible 30 90 [20] Fe- TiO2 0.10 OPW 2.05×10−4 100 UV 60 98.1 [21] Go/ZnIn2S4 0.10 OPW 1.0×10−4
（COD）100 Visible 60 72 [22] MoS2/ZIS 0.10 OPW 1.2×10−4 100 Visible 80 92 [23] TiO2
(Aerogel)0.16 OPW 1.0×10−4 400 UV 90 91 [24] MoS2/P-C3N4 0.10 OPW 1.6×10−4
(COD)100 Visible 100 94 [25] γ-Fe2O3 1 toluene 5.0×10−2 100 Visible 120 90 [26] γ-Fe2O3 1 toluene 1.0×10−1 100 Visible 120 86 [26] γ-Fe2O3 1 toluene 1.5×10−1 100 Visible 120 78 [26] Ag@ZnO/
Zn2Ti3O80.10 OPW 1.5×10−4 100 UV 300 89 [27] AgTiZn
(MW)0.10 OPW 1.5×10−4 100 UV 300 90.15 [28] CuTiZn 0.10 OPW 1.5×10−4 100 UV 300 87.02 [28] AgMgZn
(MW)0.10 OPW 1.5×10−4 100 UV 300 93.35 [28] AgMnZn
(MW)0.10 OPW 1.5×10−4 100 UV 300 88.95 [28] Pt/TiO2 0.30 POME (COD) 4.0×10−2−1.0×10−1 300 UV& Visible 480 90 [29] Ag/TiO2 0.30 POME (COD) 4.0×10−2−1.0×10−1 300 UV& Visible 480 90 [30] PVDF/TiO2 15 cm2 membrane OIL 1.0×10−3 100 UV 480 60+ [31] g-C3N4-2AC 0.025 OPW 1.0×10−3 50 Visible 480 97.2 [32] GCN 0.20 OPW 1.0×10−3 200 UV 540 96.6 [33] GCN 0.20 OPW 1.0×10−3 200 Visible 540 85.4 [33] EG-ZnO 0.10 OPW 1.0×10−3 100 UV 4320 35 [34] N/TiO2/rGO 0.025 OPW 5.0×10−1 200 UV 40320 54.80 [35] 
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[1] HASSANI S S, DARAEE M, SOBAT Z. Advanced development in upstream of petroleum industry using nanotechnology[J]. Chin J Chem Eng,2020,28(6):1483−1491. doi: 10.1016/j.cjche.2020.02.030 [2] SHEN Y, LI D W, WANG L L, et al. Superelastic polyimide nanofiber-based aerogels modified with silicone nano filaments for ultrafast oil/water separation[J]. ACS Appl Mater Interfaces,2021,13(17):20489−20500. doi: 10.1021/acsami.1c01136 [3] LIU B C, LI H S, LIU N, et al. Experimental study on filtration effect of oilfield sewage based on new polyurethane modified materials[J]. Water Sci Technol,2020,82(10):2039−2050. doi: 10.2166/wst.2020.462 [4] ZHU X L, RAN Y L, GUO W J, et al. Optimization of reinjection treatment technology for oilfield wastewater in Longdong area[J]. E3S Web of Conferences,2020,194:04046. doi: 10.1051/e3sconf/202019404046 [5] HOFFMANN M R, MARTIN S T, CHOI W. Environmental applications of semiconductor photocatalysis[J]. Chem Rev,1995,95(1):69−96. doi: 10.1021/cr00033a004 [6] SINGH M, PAKSHIRAJAN K, TRIVEDI V. A study on combined effect of methylene blue and sodium anthraquinone-2-sulphonate on inactivation efficiency of escherichia coli and enterococcus hirae[J]. Appl Catal B: Environ,2019,88(3):283−291. [7] SIEDL N, BAUMANN S O, ELSER M J, et al. Particle networks from powder mixtures: generation of Tio2-Sno2 heterojunctions via surface charge-induced heteroaggregation[J]. J Phys Chem C,2019,116(43):22967−22973. [8] MA S L, ZHAN S H, XIA Y G, et al. Enhanced photocatalytic bactericidal performance and mechanism with novel Ag/ZnO/g-C3N4 composite under visible light[J]. Catal Today,2019,330:179−188. doi: 10.1016/j.cattod.2018.04.014 [9] ZHU T T, Ye X J, ZHANG Q Q, et al. Efficient utilisation of photogenerated electrons and holes for photocatalytic redox reactions using visible light-driven Au/ZnIn2S4 hybrid[J]. J Hazard Mater,2019,367:277−285. doi: 10.1016/j.jhazmat.2018.12.093 [10] XIA Q, WANG H, HUANG B B, et al. State‐of‐the‐art advances and challenges of iron-based metal organic frameworks from attractive features, synthesis to multifunctional applications[J]. Small,2019,15(2):1803088. doi: 10.1002/smll.201803088 [11] RUI K, ZHAO G, CHEN Y, et al. Hybrid 2D dual-metal-organic frameworks for enhanced water oxidation catalysis[J]. Adv Funct Mater,2018,28(26):1801554. doi: 10.1002/adfm.201801554 [12] ZHAO F, LIU Y, HAMMOUDA S B, et al. MIL-101(Fe)/g-C3N4 for enhanced visible-light-driven photocatalysis toward simultaneous reduction of Cr(VI) and oxidation of bisphenol A in aqueous media[J]. Appl Catal B: Environ,2020,272:119033. doi: 10.1016/j.apcatb.2020.119033 [13] HAN H, ZHANG H X, CHEN Y, et al. Enhanced photocatalysis degradation of organophosphorus flame retardant using MIL-101(Fe)/persulfate: effect of irradiation wavelength and real water matrixes[J]. Chem Eng J,2019,368:273−284. doi: 10.1016/j.cej.2019.02.190 [14] ZHANG Y, XIONG M Y, SUN A R, et al. MIL-101(Fe) nanodot-induced improvement of adsorption and photocatalytic activity of carbon fiber/TiO2-based weavable photocatalyst for removing pharmaceutical pollutants[J]. J Clean Prod,2021,290:125782. doi: 10.1016/j.jclepro.2021.125782 [15] MILLANGE F, GUILLOU N, MEDINA M E. Selective sorption of organic molecules by the flexible porous hybrid metal-organic framework MIL-53(Fe) controlled by various host-guest interactions[J]. J Mater Chem A , 2010, 22, 14: 4237–4245. [16] KIM P J, YOU Y W, PARK H, et al. Separation of SF6 from SF6/N2 mixture using metal–organic framework MIL-100(Fe) granule[J]. Chem Eng J,2015,262:683−690. doi: 10.1016/j.cej.2014.09.123 [17] KIM B C, HONG W G, LEE S M, et al. Enhancement of hydrogen storage capacity in polyaniline-vanadium pentoxide nanocomposites[J]. Int J Hydrogen Energ,2010,35:1300−1304. [18] AI L H, ZHANG C H, LI L L, et al. Iron terephthalate metal–organic framework: Revealing the effective activation of hydrogen peroxide for the degradation of organic dye under visible light irradiation[J]. Appl Catal B: Environ, 2014, 148–149: 191−200. [19] LI X W, ZHAO H L, LU P P, et al. Photocatalytic activity of monolithic TiO2-SiO2 composite aerogels obtained by ambient drying for degrading oily wastewater[J]. J Univ Sci Technol Beijing,2013,35(5):651−658. [20] ZHOU G H. Degradation of oily wastewater by coated photocatalyst with visible light response[D]. Dalian: Dalian Maritime University, 2014. [21] GAO Y H, CHEN Y, WANG Z X, et al. Treatment of oily wastewater by photocatalytic degradation using nano Fe-TiO2[J]. Adv Mater Res,2013,781−784(2606):2241−2244. [22] ZHANG Y, ZHAO L. Ozone-assisted photocatalytic degradation of oil-polluted water on graphene/ZnIn2S4 composites[J]. Chem Res Appl,2022,34(8):1719−1726. [23] XIA D G, DU Y L. Preparation of MoS2/ZnIn2S4 and photocatalytic degradation of oily wastewater[J]. Ind Water Wastewater,2022,53(5):51−56. [24] LI X W, LÜ P P, YAO K F, et al. Preparation of monolithic TiO2 aerogel via ambient drying and photocatalytic degradation of oily wastewater[J]. J Inorg Mater,2012,27(11):1153−1158. [25] RUAN Y. Study on the performance of P-C3N4 coated with MoS2 for the degradation of oily wastewater[J]. Energy Chem Ind,2022,43(5):64−68. [26] ROUSHERNAS P, YUSOP Z, MAJIDNIA Z. Photocatalytic degradation of spilled oil in sea water using maghemite nanoparticles[J]. Desalin Water Treat,2016,57(13):5837−5841. doi: 10.1080/19443994.2015.1005149 [27] CHU Y H, WU X, LU D Q, et al. Preparation of nano-Ag@ZnO/Zn2Ti3O8 and its application in photocatalytic degradation of oilfield wastewater[J]. Contemp Chem Ind,2022,51(2):350−353. [28] SUN B. Study on microwave synthesis, characterisation and properties of nanocomposites[D]. Fushun: Liaoning Petrochemical University, 2020. [29] CHENG C K, DERAHMAN M R, KHAN M R. Evaluation of the photocatalytic degradation of pre-treated palm oil mill effluent (POME) over Pt-loaded titania[J]. J Environ Chem Eng,2015,1(3):261−270. [30] CHENG C K, DERAHMAN M R, NG K H, et al. Preparation of titania doped argentum photocatalyst and its photoactivity towards palm oil mill effluent degradation[J]. J Clean Prod,2016,112(1):1128−1135. [31] RUSLI U N, ALIAS N H, SHAHRUDDIN M Z, et al. Photocatalytic Degradation of Oil using Polyvinylidene Fluoride/Titanium Dioxide Composite Membrane for Oily Wastewater Treatment. Munich: MATEC Web of Conferences, 2016, 69: 05003. [32] RAN L T. Study on modification of g-C3N4 photocatalyst and its degradation of oily wastewater[D]. Xi'an: Xi'an Shiyou University, 2022. [33] ALIAS N H, JAAFAR J, SAMITSU S, et al. Photocatalytic degradation of oilfield produced water using graphitic carbon nitride embedded in electrospun polyacrylonitrile nanofibers[J]. Chemosphere,2018,204(AUG.):79−86. [34] WANG W Y, WANG L Q, ZHANG R J. Preparation of expanded graphite-ZnO composite and its photocatalytic degradation of crude oil[J]. Environ Prot Chem Ind,2007,27(4):367−370. [35] LI Y H, ZHANG Q Q, JIANG J X, et al. Long-acting photocatalytic degradation of crude oil in seawater via combination of TiO2 and N-doped TiO2/ reduced graphene oxide[J]. Environ Technol,2021,42(5/8):860−870. -
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