Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO<sub>3</sub> perovskite for degradation of organic pollutants

doi:10.1007/s11783-018-1060-9

Front. Environ. Sci. Eng.

2018, Vol. 12

Issue (6) : 10 https://doi.org/10.1007/s11783-018-1060-9

RESEARCH ARTICLE

Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO₃ perovskite for degradation of organic pollutants

Jie Mao, Xie Quan(

), Jing Wang, Cong Gao, Shuo Chen, Hongtao Yu, Yaobin Zhang

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China

Download: PDF(3556 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

OH played a key role in heterogeneous Fenton-like catalytic oxidation of organic pollutants.

Doping Cu into BiFeO₃ promoted the generation of Fe²⁺ and then facilitated the effective formation of •OH.

Cu-doped BiFeO₃ exhibited higher catalytic performance for phenol degradation than non-doped BiFeO₃.

Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO₃ as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H₂O₂ for phenol degradation than un-doped BiFeO₃. BiFe_0.8Cu_0.2O₃ displayed the best performance, which yielded 91% removal of phenol (10 mg L⁻¹) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe_0.8Cu_0.2O₃ catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe₃O₄ and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe_0.8Cu_0.2O₃. The high catalytic activity of BiFe_0.8Cu_0.2O₃ was attributed to the fact that the doping Cu into BiFeO₃ could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H₂O₂ to degrade the organic pollutants.

Keywords Cu doped BiFeO₃ Heterogeneous Fenton-like catalysts Oxidative degradation

Corresponding Author(s): Xie Quan

Issue Date: 19 August 2018

Cite this article:

Jie Mao,Xie Quan,Jing Wang, et al. Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO₃ perovskite for degradation of organic pollutants[J]. Front. Environ. Sci. Eng., 2018, 12(6): 10.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-018-1060-9
https://academic.hep.com.cn/fese/EN/Y2018/V12/I6/10

Fig.1 (a) XRD patterns of BFO and Cu-doped BFO. The enlarged XRD patterns at binding energies near 39° and 56°; (b) Nitrogen adsorption-desorption isotherms

Fig.2 (a) SEM images of BFO, (b) BiFe_0.8Cu_0.2O₃

Fig.3 (a) Phenol removal on different Cu-doped BFO and (b) The pseudo-first-order kinetic constants of phenol degradation by Cu-doped BFO ([phenol] = 10 mg/L, initial pH= 4.0, [catalysts] = 0.5 g/L, [H₂O₂] = 10 mM)

Fig.4 (a) Effect of H₂O₂ on phenol degradation in BiFe_0.8Cu_0.2O₃-H₂O₂ system ([phenol] = 10 mg/L, initial pH= 4.0, [catalysts] = 0.5 g/L), (b) Effect of catalyst load on phenol degradation in BiFe_0.8Cu_0.2O₃-H₂O₂ system ([phenol] = 10 mg/L, initial pH= 4.0, [H₂O₂] = 15 mM) and (c) Effect of initial pH on phenol degradation in BiFe_0.8Cu_0.2O₃-H₂O₂ system ([phenol] = 10 mg/L, [catalysts] = 0.5 g/L, [H₂O₂] = 15 mM)

Fig.5 (a) The phenol removal on different catalysts, (b) the removal of different contaminants in BiFe_0.8Cu_0.2O₃-H₂O₂ system ([pollutants] = 10 mg/L, [catalyst] = 0.5 g/L, [H₂O₂] = 15 mM, pH= 4.0), (c) The kinetic rates of phenol degradation by different catalysts and (d) TOC removal of phenol ([phenol] = 10 mg/L, [BiFe_0.8Cu_0.2O₃] = 0.5 g/L, pH= 4.0, [H₂O₂] = 15 mM)

Fig.6 The phenol degradation over successive cycles ([phenol] = 10 mg/L, [catalyst] = 0.5 g/L, [H₂O₂] = 15 mM, pH= 4.0)

Fig.7 (a) BMPO spin-trapping EPR spectra of •OH radicals in BiFe_0.8Cu_0.2O₃-H₂O₂ system and (b) Radical quenching experiment with TBA in BiFe_0.8Cu_0.2O₃-H₂O₂ system

Fig.8 (a) Fe 2p lines of fresh of BFO, (b) fresh of BiFe_0.8Cu_0.2O₃, (c) used of BFO and (d) used of BiFe_0.8Cu_0.2O₃

Fig.9 (a) Cu 2p lines of fresh of BiFe0.8Cu0.2O3 and 9(b) used of BiFe0.8Cu0.2O3.

1	Afzal S, Quan X, Zhang J L (2017). High surface area mesoporous nanocast LaMO3 (M= Mn, Fe) perovskites for efficient catalytic ozonation and an insight into probable catalytic mechanism. Applied Catalysis B: Environmental, 206: 692–703 https://doi.org/10.1016/j.apcatb.2017.01.072
2	An J J, Zhu L, Wang N, Song Z, Yang Z, Du D, Tang H (2013). Photo-Fenton like degradation of tetrabromobisphenol A with graphene-BiFeO3 composite as a catalyst. Chemical Engineering Journal, 219(3): 225–237 https://doi.org/10.1016/j.cej.2013.01.013
3	Bobu M, Yediler A, Siminiceanu I, Schulte-Hostede S (2008). Degradation studies of ciprofloxacin on a pillared iron catalyst. Applied Catalysis B: Environmental, 83(1): 15–23 https://doi.org/10.1016/j.apcatb.2008.01.029
4	Eberhardt M K, Ramirez G, Ayala E (1989). Does the reaction of Cu+ with H2O2 give OH radicals? A study of aromatic hydroxylation. Journal of Organic Chemistry, 54(25) https://doi.org/10.1021/jo00286a024
5	El-Desoky M M, Mostafa M M, Ayoub M S, Ahmed M A (2015). Transport properties of Ba-doped BiFeO3 multiferroic nanoparticles. Journal of Materials Science Materials in Electronics, 26(9): 6793–6800 https://doi.org/10.1007/s10854-015-3291-x
6	Gao C, Chen S, Quan X, Yu H T, Zhang Y B (2017). Enhanced Fenton-like catalysis by iron-based metal organic frameworks for degradation of organic pollutants. Journal of Catalysis, 356: 125–132 https://doi.org/10.1016/j.jcat.2017.09.015
7	Gao F, Chen X Y, Yin K B, Dong S, Ren Z F, Yuan F, Yu T, Zou Z G, Liu J M (2007). Visible-light photocatalytic properties of weak magnetic BiFeO3 nanoparticles. Advanced Materials, 19(19): 2889–2892 https://doi.org/10.1002/adma.200602377
8	Ghodselahi T, Vesaghi M A, Shafiekhani A, Baghizadeh A, Lameii M (2008). XPS study of the Cu@Cu2O core-shell nanoparticles. Applied Surface Science, 255(5): 2730–2734 https://doi.org/10.1016/j.apsusc.2008.08.110
9	Guo R Q, Fang L, Dong W, Zheng F G, Shen M R (2010). Enhanced photocatalytic activity and ferromagnetism in Gd doped BiFeO3 nanoparticles. Journal of Physical Chemistry C, 114(49): 21390–21396 https://doi.org/10.1021/jp104660a
10	Han Z B, Dong Y C, Dong S M (2011). Copper-iron bimetal modified PAN fiber complexes as novel heterogeneous Fenton catalysts for degradation of organic dye under visible light irradiation. Journal of Hazardous Materials, 189(1–2): 241–248 https://doi.org/10.1016/j.jhazmat.2011.02.026
11	Jin H, Tian X K, Nie Y L, Zhou Z X, Yang C, Li Y, Lu L Q (2017). Oxygen vacancy promoted heterogeneous Fenton-like degradation of ofloxacin at pH 3.2–9.0 by Cu substituted magnetic Fe3O4@FeOOH nanocomposite. Environmental Science & Technology, 51(21): 12699–12706 https://doi.org/10.1021/acs.est.7b04503
12	Li H, Shang J, Yang Z P, Shen W J, Ai Z H, Zhang L Z (2017). Oxygen vacancy associated surface Fenton chemistry: surface structure dependent hydroxyl radicals generation and substrate dependent reactivity. Environmental Science & Technology, 51(10): 5685–5694 https://doi.org/10.1021/acs.est.7b00040
13	Liao Q, Sun J, Gao L (2009). Degradation of phenol by heterogeneous Fenton reaction using multi-walled carbon nanotube supported Fe2O3 catalysts. Colloids and Surfaces. A, Physicochemical and Engineering Aspects, 345(1–3): 95–100 https://doi.org/10.1016/j.colsurfa.2009.04.037
14	Luo W, Zhu L H, Wang N, Tang H Q, Cao M J, She Y B (2010). Efficient removal of organic pollutants with magnetic nanoscaled BiFeO3 as a reusable heterogeneous Fenton-like catalyst. Environmental Science & Technology, 44(5): 1786–1791 https://doi.org/10.1021/es903390g
15	Matta R, Hanna K, Kone T, Chiron S (2008). Oxidation of 2,4,6-trinitrotoluene in the presence of different iron-bearing minerals at neutral pH. Chemical Engineering Journal, 144(3): 453–458 https://doi.org/10.1016/j.cej.2008.07.013
16	Nie Y L, Hu C, Qu J H, Zhao X (2009). Photoassisted degradation of endocrine disruptors over CuOx-FeOOH with H2O2 at neutral pH. Applied Catalysis B: Environmental, 87(1–2): 30–36 https://doi.org/10.1016/j.apcatb.2008.08.022
17	Patel K B, Willson R L (1973). Semiquinone free radicals and oxygen. Pulse radiolysis study of one electron transfer equilibria. Journal of the Chemical Society, Faraday Transactions, 69(4): 814–825 https://doi.org/10.1039/f19736900814
18	Pham L T, Lee C, Doyle F M, Sedlak D L (2009). A silica-supported iron oxide catalyst capable of activating hydrogen peroxide at neutral pH values. Environmental Science & Technology, 43(23): 8930–8935 https://doi.org/10.1021/es902296k
19	Ramadan W, Parves A, Shaikh , Ebrahim S, Ramadan A, Hannoyer B, Jouen S, Sauvage X, Ogale S (2013). Highly efficient photocatalysis by BiFeO3/a(g)-Fe2O3 ferromagnetic nano P/N junctions formed by dopant-induced phase separation. Journal of Nanoparticle Research, 15(15): 1–10
20	Sedlak D L, Hoigne J (1994). Oxidation of S(IV) in atmospheric water by photooxidants and iron in the presence of copper. Environmental Science & Technology, 28(11): 1898–1906 https://doi.org/10.1021/es00060a021
21	Soltani T, Lee B K (2016). Novel and facile synthesis of Ba-doped BiFeO3 nanoparticles and enhancement of their magnetic and photocatalytic activities for complete degradation of benzene in aqueous solution. Journal of Hazardous Materials, 316: 122–133 https://doi.org/10.1016/j.jhazmat.2016.03.052
22	Soltani T, Lee B K (2017a). Comparison of benzene and toluene photodegradation under visible light irradiation by Ba-doped BiFeO3 magnetic nanoparticles with fast sonochemical synthesis. Photochemical & Photobiological Sciences, 16(1): 86–95 https://doi.org/10.1039/C6PP00212A
23	Soltani T, Lee B K (2017b). Enhanced formation of sulfate radicals by metal-doped BiFeO3 under visible light for improving photo-Fenton catalytic degradation of 2-chlorophenol. Chemical Engineering Journal, 313: 1258–1268 https://doi.org/10.1016/j.cej.2016.11.016
24	Xia M, Long M C, Yang Y D, Chen C, Cai W M, Zhou B X (2011). A highly active bimetallic oxides catalyst supported on Al-containing MCM-41 for Fenton oxidation of phenol solution. Applied Catalysis B: Environmental, 110: 118–125 https://doi.org/10.1016/j.apcatb.2011.08.033
25	Xu L J, Wang J L (2012). Magnetic nanoscaled Fe3O4/CeO2 composite as an efficient Fenton-like heterogeneous catalyst for degradation of 4-chlorophenol. Environmental Science & Technology, 46(18): 10145–10153 https://doi.org/10.1021/es300303f
26	Yin Y H, Liu W F, Huo N N, Yang S T (2017). High rate capability and long cycle stability of Fe2O3/MgFe2O4 anode material synthesized by gel-cast processing. Chemical Engineering Journal, 307: 999–1007 https://doi.org/10.1016/j.cej.2016.09.025
27	Zaki M I, Ramadan W, Katrib A, Rabee A I M (2014). Surface chemical and photocatalytic consequences of Ca-doping of BiFeO3 as probed by XPS and H2O2 decomposition studies. Applied Surface Science, 317: 929–934 https://doi.org/10.1016/j.apsusc.2014.09.007
28	Zhang C Y, Sun H J, Chen W, Zhou J, Li B, Wang Y B (2009). Hydrothermal synthesis and photo-catalytic property of Bi25FeO40 powders: Applications of Ferroelectrics. IEEE International Symposium on the IEEE,1–3
29	Zhang J B, Zhuang J, Gao L Z, Zhang Y, Gu N, Feng J, Yang D L, Zhu J D, Yan X Y (2008). Decomposing phenol by the hidden talent of ferromagnetic nanoparticles. Chemosphere, 73(9): 1524–1528 https://doi.org/10.1016/j.chemosphere.2008.05.050
30	Zhang X Y, Ding Y B, Tang H Q, Han X Y, Zhu L H, Wang N (2014). Degradation of bisphenol A by hydrogen peroxide activated with CuFeO2 microparticles as a heterogeneous Fenton-like catalyst: Efficiency, stability and mechanism. Chemical Engineering Journal, 236: 251–262 https://doi.org/10.1016/j.cej.2013.09.051
31	Zhu J J, Li H L, Zhong L Y, Xiao P, Xu X L, Yang X G, Zhao Z, Li J L (2014). Perovskite oxides: Preparation, characterizations, and applications in heterogeneous catalysis. ACS Catalysis, 4(9): 2917–2940 https://doi.org/10.1021/cs500606g
32	Zhu J J, Thomas (2009). A Perovskite-type mixed oxides as catalytic material for NO removal. Applied Catalysis B: Environmental, 92(3–4): 225–233

[1]

FSE-18028-OF-MJ_suppl_1

Download

[1]	Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan. Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of organic pollutants[J]. Front. Environ. Sci. Eng., 2019, 13(2): 18-.

Viewed

Full text

Abstract

Cited

Shared

Discussed