Journal of Guangxi Normal University(Natural Science Edition) ›› 2023, Vol. 41 ›› Issue (3): 210-220.doi: 10.16088/j.issn.1001-6600.2022050903

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Preparation of CuO/MIL(Cr, Cu) Composite and Its Performance in Fenton-like Catalytic Degradation of Phenol

YANG Wen1, SU Yingjie1, HOU Dongrui2, LUO Jing1, SUN Qinggong1, ZHANG Mengyang2, YANG Hao2, WANG Jianfeng2*   

  1. 1. School of Chemical Engineering, Zhengzhou University, Zhengzhou Henan 450007, China;
    2. School of Ecology and Environment, Zhengzhou University, Zhengzhou Henan, 450007, China
  • Received:2022-05-09 Revised:2022-05-17 Online:2023-05-25 Published:2023-06-01

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Abstract: CuO/MIL(Cr, Cu) heterogeneous Fenton-like catalysts were synthesized by hydrothermal calcination. The CuO/MIL(Cr, Cu) composite was characterized by XRD, FT-IR, SEM, XPS, BET, etc. The results showed that CuO was uniformly dispersed on the surface of the metal-organic framework MIL(Cr, Cu). In addition, the performance of different catalysts for the catalytic degradation of phenol were compared. The results of degradation experiments showed that when the catalyst dosage was 0.3 g/L, the H2O2 concentration was 50 mmol/L, pH=6, and the initial substrate concentration was 30 mg/L, the CuO/MIL(Cr, Cu) composite had the best degradation efficiency as high as almost 100%, better than that of CuO and MIL-101(Cr). Finally, the radical quenching experimentand EPR test proved that ·OH was the main active radical in the catalytic system, and the possible catalytic mechanism was proposed. CuO/MIL(Cr, Cu) composite can degrade phenolic pollutants in the near-neutral range and have good application prospects.

Key words: heterogeneous catalyst, Fenton-like, metal organic framework, copper oxide, phenol wastewater

CLC Number:  X703;TQ426.94
[1] FORTUNY A, FONT J, FABREGAT A. Wet air oxidation of phenol using active carbon as catalyst[J]. Applied Catalysis B: Environmental, 1998, 19(3/4): 165-173. DOI: 10.1016/S0926-3373(98)00072-1.
[2] VILLEGAS L G C, MASHHADI N, CHEN M, et al. A short review of techniques for phenol removal from wastewater[J]. Current Pollution Reports, 2016, 2(3): 157-167. DOI: 10.1007/s40726-016-0035-3.
[3] SUN X F, WANG C W, LI Y B, et al. Treatment of phenolic wastewater by combined UF and NF/RO processes[J]. Desalination, 2015, 355: 68-74. DOI: 10.1016/j.desal.2014.10.018.
[4] KULKARNI S J, KAWARE J P. Review on research for removal of phenol from wastewater[J]. International Journal of Scientific and Research Publications, 2013, 3(4): 1-5.
[5] ALSHABIB M, ONAIZI S A. A review on phenolic wastewater remediation using homogeneous and heterogeneous enzymatic processes: current status and potential challenges[J]. Separation and Purification Technology, 2019, 219: 186-207. DOI: 10.1016/j.seppur.2019.03.028.
[6] FAN X L, CAO Q Q, MENG F Y, et al. A Fenton-like system of biochar loading Fe-Al layered double hydroxides (FeAl-LDH@BC)/H2O2 for phenol removal[J]. Chemosphere, 2021, 266: 128992. DOI: 10.1016/j.chemosphere.2020.128992.
[7] PI Y H, LI X Y, XIA Q B, et al. Adsorptive and photocatalytic removal of persistent organic pollutants (POPs) in water by metal-organic frameworks (MOFs)[J]. Chemical Engineering Journal, 2018, 337: 351-371. DOI: 10.1016/j.cej.2017.12.092.
[8] ZANCHETTIN G, DA SILVA FALK G, GÓMEZ GONZÁLEZ S Y, et al. High performance magnetically recoverable Fe3O4 nanocatalysts: fast microwave synthesis and photo-Fenton catalysis under visible-light[J]. Chemical Engineering and Processing-Process Intensification, 2021, 166: 108438. DOI: 10.1016/j.cep.2021.108438.
[9] 邵禹萌,崔宝臣,刘淑芝,等.MIL-101(Cr)催化单过硫酸氢钾降解罗丹明B[J].净水技术,2019,38(10):88-93. DOI:10.15890/j.cnki.jsjs.2019.10.016.
[10] DE VOORDE B V, BUEKEN B, DENAYER J, et al. Adsorptive separation on metal-organic frameworks in the liquid phase[J]. Chemical Society Reviews, 2014, 43(16): 5766-5788. DOI: 10.1039/C4CS00006D.
[11] WU C D, ZHAO M. Incorporation of molecular catalysts in metal-organic frameworks for highly efficient heterogeneous catalysis[J]. Advanced Materials, 2017, 29(14): 1605446. DOI: 10.1002/adma.201605446.
[12] KHAN M S, KHALID M, SHAHID M. What triggers dye adsorption by metal organic frameworks? The current perspectives[J]. Materials Advances, 2020, 1(6): 1575-1601. DOI: 10.1039/D0MA00291G.
[13] 任逸,施梦琦,尹越,等.Fe2O3/MIL-53(Al)催化类芬顿氧化性能及其作用机制研究[J].环境科学学报,2019,39(8):2508-2516. DOI:10.13671/j.hjkxxb.2019.0103.
[14] REN Y, SHI M Q, ZHANG W M, et al. Enhancing the Fenton-like catalytic activity of nFe2O3 by MIL-53(Cu) support: a mechanistic investigation[J]. Environmental Science & Technology, 2020, 54(8): 5258-5267. DOI: 10.1021/acs.est.0c00203.
[15] 张宗伟,李酽,初飞雪.稀土、Fe3+掺杂TiO2光催化降解水中氨氮研究[J].广西师范大学学报(自然科学版),2014,32(2):117-121. DOI:10.3969/j.issn.1001-6600.2014.02.020.
[16] MA R, LIU G M, FENG S H, et al. Optimization and effects of catalytic ozonation of actual phenolic wastewater by CuO/Al2O3[J]. China Petroleum Processing and Petrochemical Technology, 2019, 21(3): 74-80.
[17] 刘剑,王彩瑜,彭钢,等.5A分子筛载CuO对甲基橙的催化湿式过氧化氢氧化[J].材料导报,2018,32(S2):218-222.
[18] ZHONG Z, LI M, FU J H, et al. Construction of Cu-bridged Cu2O/MIL(Fe/Cu) catalyst with enhanced interfacial contact for the synergistic photo-Fenton degradation of thiacloprid[J]. Chemical Engineering Journal, 2020, 395: 125184. DOI: 10.1016/j.cej.2020.125184.
[19] 焦华,王君龙.CuO微/纳米结构的可控合成与红外性质[J].粉末冶金材料科学与工程,2013,18(5):700-705. DOI:10.3969/j.issn.1673-0224.2013.05.013.
[20] 蔡培新,陈建民,顾为芳.YBa2Cu3O7-δ中Cu—O伸缩振动的红外吸收峰[J].低温物理学报,1993,10(5):345-349.
[21] GEORGE A, MAGIMAI ANTONI RAJ D, DHAYAL RAJ A, et al. Morphologically tailored CuO nanostructures toward visible-light-driven photocatalysis[J]. Materials Letters, 2020, 281: 128603. DOI: 10.1016/j.matlet.2020.128603.
[22] BIESINGER M C, PAYNE B P, GROSVENOR A P, et al. Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni[J]. Applied Surface Science, 2011, 257(7): 2717-2730. DOI: 10.1016/j.apsusc.2010.10.051.
[23] ARONNIEMI M, SAINIO J, LAHTINEN J. Chemical state quantification of iron and chromium oxides using XPS: the effect of the background subtraction method[J]. Surface Science, 2005, 578(1/3): 108-123. DOI: 10.1016/j.susc.2005.01.019.
[24] YAO Y J, LU F, ZHU Y P, et al. Magnetic core-shell CuFe2O4@C3N4 hybrids for visible light photocatalysis of Orange II[J]. Journal of Hazardous Materials, 2015, 297: 224-233. DOI: 10.1016/j.jhazmat.2015.04.046.
[25] WANG J, FAN D Q, YU T, et al. Improvement of low-temperature hydrothermal stability of Cu/SAPO-34 catalysts by Cu2+ species[J]. Journal of Catalysis, 2015, 322: 84-90. DOI: 10.1016/j.jcat.2014.11.010.
[26] LIU J, CUI J N, ZHAO T Y, et al. Fe3O4-CeO2 loaded on modified activated carbon as efficient heterogeneous catalyst[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2019, 565: 59-69. DOI: 10.1016/j.colsurfa.2018.12.052.
[27] 张丹薇.铜铈二元混合氧化物催化过硫酸氢钾降解苯酚研究[D].哈尔滨:哈尔滨工业大学,2013. DOI:10.7666/d.D594691.
[28] NIU H Y, ZHENG Y, WANG S H, et al. Continuous generation of hydroxyl radicals for highly efficient elimination of chlorophenols and phenols catalyzed by heterogeneous Fenton-like catalysts yolk/shell Pd@Fe3O4@metal organic frameworks[J]. Journal of Hazardous Materials, 2018, 346: 174-183. DOI: 10.1016/j.jhazmat.2017.12.027.
[29] LUO M Y, LI M F, JIANG S, et al. Supported growth of inorganic-organic nanoflowers on 3D hierarchically porous nanofibrous membrane for enhanced enzymatic water treatment[J]. Journal of Hazardous Materials, 2020, 381: 120947. DOI: 10.1016/j.jhazmat.2019.120947.
[30] 方嘉声,于光认,陈晓春,等.石墨烯掺杂分子筛负载氧化铁芬顿催化降解苯酚影响因素的研究[J].环境科学学报,2015,35(11):3529-3537. DOI:10.13671/j.hjkxxb.2014.1069.
[31] 封立伟.Fe/AC非均相Fenton体系降解废水中苯酚研究[J].工业用水与废水,2019,50(3):26-29. DOI:10.3969/j.issn.1009-2455.2019.03.006.
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