金属有机框架MIL-101（Fe）用于增强光催化降解含油污水中的原油

Liang Yuning; Wang Baohui; Li Shuohui; Chi Weimeng; Bi Mingchun; Liu Yuxuan; Wang Yiran; Yao Ming; Zhang Tianying; Chen Ying

doi:10.1016/S1872-5813(23)60396-2

金属有机框架MIL-101（Fe）用于增强光催化降解含油污水中的原油

doi: 10.1016/S1872-5813(23)60396-2

梁宇宁^1,,
王宝辉^1,,
李硕辉^1,,
迟伟蒙¹,
毕明春^1,,
刘雨萱^1,,
王一然^1,,
姚明^1,,
张天赢^2,,
陈颖^1, ,

1.
东北石油大学化学与化学工程学院石油与天然气加工重点实验室, 大庆, 中国黑龙江省, 163318
2.
大庆油田生产测试分公司, 黑龙江, 163318

详细信息

中图分类号: X74
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- 被引次数: 0
出版历程
- 收稿日期: 2023-07-04
- 修回日期: 2023-10-12
- 录用日期: 2023-10-18
- 网络出版日期: 2023-11-10

Enhanced photocatalysis using metal–organic framework MIL-101(Fe) for crude oil degradation in oil-polluted water

1.
Key Laboratory of Oil and Natural Gas Processing, School of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing, Heilongjiang, China, 163318
2.
Operation Team 3 of Daqing Oil Field Production Testing Branch, Daqing, Heilongjiang, China, 163318

More Information

Corresponding author: Tel:18345996681, E-mail:chenying648617@163.com

摘要

摘要: 利用溶剂热法成功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为5.5，催化剂量为0.15 g/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首次应用。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。
- MIL-101(Fe) /
- MOF /
- 光催化 /
- 溶剂热 /
- 油田废水 /
- 降解.
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 0.15 g/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.
- MIL-101(Fe) /
- MOF /
- photocatalysis /
- Solvothermal /
- oilfield wastewater /
- degradation.

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Figure 1 XRD spectrum of MIL-101(Fe)

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Figure 2 (a)-(c) SEM images of MIL-101(Fe). (d) TEM image of MIL-101(Fe)

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Figure 3 FT-IR spectrum of MIL-101(Fe)

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Figure 4 (a) UV-Vis DRS of MIL-101(Fe), (b) plots of (αhv)² versus energy (hv) of MIL-101(Fe)

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Figure 5 N₂ adsorption-desorption isotherms of MIL-101(Fe)

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Figure 6 XPS spectra of MIL-101(Fe)

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Figure 7 Wettability of MIL-101(Fe)

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Figure 8 Degradation of crude oil using MIL-101(Fe) under different conditions (catalyst + light, only catalyst, and only light)

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Figure 9 Photocatalytic degradation of crude oil using MIL-101(Fe) in the initial state

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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

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Figure 11 Experimental kinetic analysis of photocatalytic degradation of crude oil using MIL-101(Fe) under optimum conditions

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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

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Figure 13 Capture experiments to investigate the generation of active species behind MIL-101(Fe) in the photocatalytic degradation of crude oil

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Figure 14 (a) EIS spectra of MIL-101(Fe), (b) Plots of Intensity versus Binding Energy using MIL-101(Fe)

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Figure 15 Proposed mechanistic pathway under visible light irradiation

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Table 1 Summary of research on photocatalytic degradation of oily wastewater by various catalysts

Photocatalyst	Activator amount /g	Pollutant	Concentration	Dose of pollutant /ml	Source of irradiation	Time / min	Maximum degradation/ adsorption	Reference
MIL-101(Fe)	0.015	OPW	500 ppm	60	UV	30	94.73	This paper
TiO₂-SiO₂	0.16	OPW	100 ppm	400	UV	30	95	19
Ce/Bi₂O₃	10.51	OPW	50 ppm	2000	Visible	30	90	20
Fe- TiO₂	0.10	OPW	205 ppm	100	UV	60	98.1	21
Go/ZnIn₂S₄	0.10	OPW	100 ppm （COD）	100	Visible	60	72	22
MoS₂/ZIS	0.10	OPW	120 ppm	100	Visible	80	92	23
TiO₂ (Aerogel)	0.16	OPW	100 ppm	400	UV	90	91	24
MoS₂/P-C₃N₄	0.10	OPW	160 ppm (COD)	100	Visible	100	94	25
γ-Fe₂O₃	1	toluene	50000 ppm	100	Visible	120	90	26
γ-Fe₂O₃	1	toluene	100000 ppm	100	Visible	120	86	26
γ-Fe₂O₃	1	toluene	150000 ppm	100	Visible	120	78	26
Ag@ZnO/ Zn₂Ti₃O₈	0.10	OPW	150 ppm	100	UV	300	89	27
AgTiZn (MW)	0.10	OPW	150 ppm	100	UV	300	90.15	28
CuTiZn	0.10	OPW	150 ppm	100	UV	300	87.02	28
AgMgZn (MW)	0.10	OPW	150 ppm	100	UV	300	93.35	28
AgMnZn (MW)	0.10	OPW	150 ppm	100	UV	300	88.95	28
Pt/TiO₂	0.30	POME (COD)	40000−100000 ppm	300	UV& Visible	480	90	29
Ag/TiO₂	0.30	POME (COD)	40000−100000 ppm	300	UV& Visible	480	90	30
PVDF/TiO₂	15 cm² membrane	OIL	1000 ppm	100	UV	480	60 +	31
g-C₃N₄-2AC	0.025	OPW	1000 ppm	50	Visible	480	97.2	32
GCN	0.20	OPW	1000 ppm	200	UV	540	96.6	33
GCN	0.20	OPW	1000 ppm	200	Visible	540	85.4	33
EG-ZnO	0.10	OPW	1000 ppm	100	UV	4320	35	34
N/TiO₂/rGO	0.025	OPW	500000 ppm	200	UV	40320	54.80	35

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参考文献(35)

[1]	HASSANI S S, DARAEE M, SOBAT Z. Advanced development in upstream of petroleum industry using nanotechnology[J]. CHINESE 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]. Journal of University of Science and Technology 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]. Industrial 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 Chemical Industry,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]. Contemporary Chemical Industry,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.
[32]	RAN L T. Study on Modification of g-C3N4 Photocatalyst and its Degradation of Oily Wastewater[D]. 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]. Environmental Protection and of Chemical Industry,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.