Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles for bisphenol A degradation

doi:10.1007/s11705-023-2327-7

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (10) : 1581-1592 https://doi.org/10.1007/s11705-023-2327-7

RESEARCH ARTICLE

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles for bisphenol A degradation

Fulong Wang, Liang Sun(

), Ziyu Zhang, Fengkai Yang, Jinlong Yang, Weijian Liu(

)

School of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, China

Download: PDF(5558 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al₂O₃, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including $SO 4 •‒$ , OH •, and $O 2 •‒$ ) and singlet oxygen ( $1 O 2$ ) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al₂O₃ promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

Keywords Cu–Al bimetallic oxides mesoporous silica spheres peroxydisulfate bisphenol A

Corresponding Author(s): Liang Sun,Weijian Liu

Just Accepted Date: 26 May 2023 Online First Date: 11 July 2023 Issue Date: 07 October 2023

Cite this article:

Fulong Wang,Liang Sun,Ziyu Zhang, et al. Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles for bisphenol A degradation[J]. Front. Chem. Sci. Eng., 2023, 17(10): 1581-1592.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2327-7
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I10/1581

Fig.1 XRD patterns of Cu–Al and Cu–Al/MSSs.

Tab.1 The characterization data of the prepared materials

Fig.2 (a) Nitrogen sorption isotherms, and (b) the pore size distribution of MSSs, Cu–Al and Cu–Al/MSSs.

Fig.3 Micrographs images and EDS element distribution of (a) Cu–Al, and (b) Cu–Al/MSSs.

Fig.4 (a) The removal performances via different processes, and (b) the comparison of the apparent reaction rate constant between CuO/MSSs + PDS and Cu–Al/MSSs + PDS (conditions: [BPA] = 50 mg·L^?1, [material] = 0.5 g·L^?1, [PDS] = [H₂O₂] = 100 mmol·L^?1, pH = neutral, temperature = 25 °C).

Fig.5 Effect of the initial pH on BPA removal: (a) the removal efficiency, and (b) the pseudo-first-order kinetic model (conditions: [BPA] = 50 mg·L^?1, [Cu–Al/MSSs] = 0.5 g·L^?1, [PDS] = 100 mmol·L^?1, temperature = 25 °C).

Fig.6 The removal performances with (a) different catalyst amount after 30 min and (b) different PDS dosage after 30 min; (c) the effect of the reaction temperature on the BPA removal (inset showing plot of ln(k×10²) versus 10³/T); and (d) the reusability of Cu–Al and Cu–Al/MSSs (conditions: [BPA] = 50 mg·L^?1, [catalyst] = 0.5 g·L^?1 for (b), (c), and (d), [PDS] = 100 mmol·L^?1 for (a), (c), and (d), pH = neutral, temperature = 25 °C for (a), (b), and (d)).

Fig.7 BPA removal in different scavenger systems: (a) the removal efficiency after 30 min, and (b) the apparent reaction rate constant k (conditions: [BPA] = 50 mg·L^?1, [Cu–Al/MSSs] = 0.5 g·L^?1, [PDS] = 100 mmol·L^?1, [scavenger] = 100 mmol·L^?1, pH = neutral, temperature = 25 °C); EPR spectra of the Cu–Al/MSSs + PDS system: (c) DMPO for OH? and

SO 4 ??

and (d) TEMP for

1 O 2

Fig.8 (a) Cu 2p, and (b) O 1s for Cu–Al and Cu–Al/MSSs fresh and used for five cycles.

Fig.9 (a) LSV curves under different conditions, and (b) i–t curve of Cu–Al/MSSs (conditions: [BPA] = 50 mg·L^?1, [Cu–Al/MSSs] = 0.5 g·L^?1, [PDS] = 100 mmol·L^?1, pH = neutral, temperature = 25 °C).

Fig.10 Mechanism scheme of BPA removal in Cu–Al/MSSs + PDS process.

1	V Cleveland, J P Bingham, E Kan. Heterogeneous Fenton degradation of bisphenol A by carbon nanotube-supported Fe3O4. Separation and Purification Technology, 2014, 133: 388–395 https://doi.org/10.1016/j.seppur.2014.06.061
2	P J He, Z Zheng, H Zhang, L M Shao, Q Y Tang. PAEs and BPA removal in landfill leachate with Fenton process and its relationship with leachate DOM composition. Science of the Total Environment, 2009, 407(17): 4928–4933 https://doi.org/10.1016/j.scitotenv.2009.05.036
3	L Sun, H Jiang, Y X Zhao, X Y Deng, K Shen, Y Li, M G Tian. Implementation of fluidized-bed Fenton as tertiary treatment of nitro-aromatic industrial wastewater. Process Safety and Environmental Protection, 2021, 146: 490–498 https://doi.org/10.1016/j.psep.2020.11.046
4	C Calik, D I Cifci. Comparison of kinetics and costs of Fenton and photo-Fenton processes used for the treatment of a textile industry wastewater. Journal of Environmental Management, 2022, 304: 114234 https://doi.org/10.1016/j.jenvman.2021.114234
5	L Sun, Y Li, A M Li. Treatment of actual chemical wastewater by a heterogeneous Fenton process using natural pyrite. International Journal of Environmental Research and Public Health, 2015, 12(11): 13762–13778 https://doi.org/10.3390/ijerph121113762
6	E J Behrman. Peroxydisulfate chemistry in the environmental literature: a brief critique. Journal of Hazardous Materials, 2019, 365: 971 https://doi.org/10.1016/j.jhazmat.2018.11.018
7	L Sun, Z Y Zhang, H Jiang, X X Deng. Facile synthesis of magnetic mesoporous silica spheres for efficient removal of methylene blue via catalytic persulfate activation. Separation and Purification Technology, 2021, 256: 117801 https://doi.org/10.1016/j.seppur.2020.117801
8	L Sun, D H Hu, Z Y Zhang, X Y Deng. Oxidative degradation of methylene blue via PDS-based advanced oxidation process using natural pyrite. International Journal of Environmental Research and Public Health, 2019, 16(23): 4773 https://doi.org/10.3390/ijerph16234773
9	Y Lv, Z Li, X Zhou, S Cheng, L Zheng. Stabilization of source-separated urine by heat-activated peroxydisulfate. Science of the Total Environment, 2020, 749: 142213 https://doi.org/10.1016/j.scitotenv.2020.142213
10	F Lou, Z Qiang, X Zou, J Lv, M Li. Organic pollutant degradation by UV/peroxydisulfate process: impacts of UV light source and phosphate buffer. Chemosphere, 2022, 292: 133387 https://doi.org/10.1016/j.chemosphere.2021.133387
11	D A House. Kinetics and mechanism of oxidations by peroxydisulfate. Chemical Reviews, 1962, 62(3): 185–203 https://doi.org/10.1021/cr60217a001
12	L Sun, Z Y Zhang, F L Wang, M J Bai, X X Deng, L Y Wang. Activation of persulfate by mesoporous silica spheres-doping CuO for bisphenol A removal. Environmental Research, 2022, 205: 112529 https://doi.org/10.1016/j.envres.2021.112529
13	Z Dong, C Jiang, J Yang, X Zhang, W Dai, P Cai. Transformation of iodide by Fe(II) activated peroxydisulfate. Journal of Hazardous Materials, 2019, 373: 519–526 https://doi.org/10.1016/j.jhazmat.2019.03.063
14	J Huang, H Zhang. Mn-based catalysts for sulfate radical-based advanced oxidation processes: a review. Environment International, 2019, 133: 105141 https://doi.org/10.1016/j.envint.2019.105141
15	J Wang, B Li, Y Li, X Fan, F Zhang, G Zhang, Y Zhu, W Peng. Easily regenerated CuO/γ-Al2O3 for persulfate-based catalytic oxidation: insights into the deactivation and regeneration mechanism. ACS Applied Materials & Interfaces, 2021, 13(2): 2630–2641 https://doi.org/10.1021/acsami.0c19013
16	W Peng, J Liu, C Li, F Zong, W Xu, X Zhang, Z Fang. A multipath peroxymonosulfate activation process over supported by magnetic CuO-Fe3O4 nanoparticles for efficient degradation of 4-chlorophenol. Korean Journal of Chemical Engineering, 2018, 35(8): 1662–1672 https://doi.org/10.1007/s11814-018-0074-0
17	P Sathishkumar, R Sweena, J J Wu, S Anandan. Synthesis of CuO-ZnO nanophotocatalyst for visible light assisted degradation of a textile dye in aqueous solution. Chemical Engineering Journal, 2011, 171(1): 136–140 https://doi.org/10.1016/j.cej.2011.03.074
18	L Sun, H Jiang, Y X Zhao, J Wan, L L Li, L Y Wang, Y Zhang. Facile synthesis of copper-based bimetallic oxides for efficient removal of bisphenol a via Fenton-like degradation. Separation and Purification Technology, 2022, 205: 112529
19	K Kim, D K Yi, U Paik. CuO embedded silica nanoparticles for tungsten oxidation via a heterogeneous Fenton-like reaction. Microelectronic Engineering, 2017, 183: 58–63 https://doi.org/10.1016/j.mee.2017.10.004
20	H Song, Z Guan, D Xia, H Xu, F Yang, D Li, X Li. Copper-oxygen synergistic electronic reconstruction on g-C3N4 for efficient non-radical catalysis for peroxydisulfate and peroxymonosulfate. Separation and Purification Technology, 2021, 257: 117957 https://doi.org/10.1016/j.seppur.2020.117957
21	G Wang, Y Zhang, L Ge, Z Liu, X Zhu, S Yang, P Jin, X Zeng, X Zhang. Monodispersed CuO nanoparticles supported on mineral substrates for groundwater remediation via a nonradical pathway. Journal of Hazardous Materials, 2022, 429: 128282 https://doi.org/10.1016/j.jhazmat.2022.128282
22	R Yin, W Guo, H Wang, J Du, X Zhou, Q Wu, H Zheng, J Chang, N Ren. Selective degradation of sulfonamide antibiotics by peroxymonosulfate alone: direct oxidation and nonradical mechanisms. Chemical Engineering Journal, 2018, 334: 2539–2546 https://doi.org/10.1016/j.cej.2017.11.174
23	R Luo, M Li, C Wang, M Zhang, M A N Khan, X Sun, J Shen, W Han, L Wang, J Li. Singlet oxygen-dominated non-radical oxidation process for efficient degradation of bisphenol A under high salinity condition. Water Research, 2019, 148: 416–424 https://doi.org/10.1016/j.watres.2018.10.087
24	G Wang, L Ge, Z Liu, X Zhu, S Yang, K Wu, P Jin, X Zeng, X Zhang. Activation of peroxydisulfate by defect-rich CuO nanoparticles supported on layered MgO for organic pollutants degradation: an electron transfer mechanism. Chemical Engineering Journal, 2022, 431: 134026 https://doi.org/10.1016/j.cej.2021.134026
25	A Khalida, U H Ikram, M Khan. Gas sensing properties of semiconducting copper oxide nanospheroids. Powder Technology, 2015, 283: 505–511 https://doi.org/10.1016/j.powtec.2015.06.023
26	S Xu, H Zhu, W Cao, Z Wen, J Wang, C P François-Xavier, T Wintgens. Cu–Al2O3-g-C3N4 and Cu–Al2O3-C-dots with dual-reaction centres for simultaneous enhancement of Fenton-like catalytic activity and selective H2O2 conversion to hydroxyl radicals. Applied Catalysis B: Environmental, 2018, 234: 223–233 https://doi.org/10.1016/j.apcatb.2018.04.029
27	J A Botas, J A Melero, F Martínez, M I Pariente. Assessment of Fe2O3/SiO2 catalysts for the continuous treatment of phenol aqueous solutions in a fixed bed reactor. Catalysis Today, 2010, 149(3–4): 334–340 https://doi.org/10.1016/j.cattod.2009.06.014
28	J Zong, Y Zhu, X Yang, C Li. Confined growth of CuO, NiO, and Co3O4 nanocrystals in mesoporous silica (MS) spheres. Journal of Alloys and Compounds, 2011, 509(6): 2970–2975 https://doi.org/10.1016/j.jallcom.2010.11.175
29	G P Anipsitakis, D D Dionysiou. Radical generation by the interaction of transition metals with common oxidants. Environmental Science & Technology, 2004, 38(13): 3705–3712 https://doi.org/10.1021/es035121o
30	R O C NormanP M StoreyP R West. Electron spin resonance studies. Part XXV. Reactions of the sulphate radical anion with organic compounds. Journal of the Chemical Society B: Physical Organic, 1970, 1087–1095
31	H Cai, X Li, D Ma, Q Feng, D Wang, Z Liu, X Wei, K Chen, H Lin, S Qin, F Lu. Stable Fe3O4 submicrospheres with SiO2 coating for heterogeneous Fenton-like reaction at alkaline condition. Science of the Total Environment, 2021, 764: 144200 https://doi.org/10.1016/j.scitotenv.2020.144200
32	J Yan, L Zhu, Z Luo, Y Huang, H Tang, M Chen. Oxidative decomposition of organic pollutants by using persulfate with ferrous hydroxide colloids as efficient heterogeneous activator. Separation and Purification Technology, 2013, 106: 8–14 https://doi.org/10.1016/j.seppur.2012.12.012
33	Y Guo, H Liang, L Bai, K Huang, B Xie, D Xu, J Wang, G Li, X Tang. Application of heat-activated peroxydisulfate pre-oxidation for degrading contaminants and mitigating ultrafiltration membrane fouling in the natural surface water treatment. Water Research, 2020, 179: 115905 https://doi.org/10.1016/j.watres.2020.115905
34	X Zhang, Y Ding, H Tang, X Han, L Zhu, N Wang. Degradation of bisphenol A by hydrogen peroxide activated with CuFeO2 microparticles as a heterogeneous Fenton-like catalyst: efficiency, stability and mechanism. Chemical Engineering Journal, 2014, 236: 251–262 https://doi.org/10.1016/j.cej.2013.09.051
35	Y Liu, R Luo, Y Li, J Qi, C Wang, J Li, X Sun, L Wang. Sandwich-like Co3O4/MXene composite with enhanced catalytic performance for bisphenol A degradation. Chemical Engineering Journal, 2018, 347: 731–740 https://doi.org/10.1016/j.cej.2018.04.155
36	X Li, Y Zhang, Y Xie, Y Zeng, P Li, T Xie, Y Wang. Ultrasonic enhanced Fenton-like degradation of bisphenol A using a bio-synthesized schwertmannite catalyst. Journal of Hazardous Materials, 2018, 344: 689–697 https://doi.org/10.1016/j.jhazmat.2017.11.019
37	L Lyu, L Zhang, Q Wang, Y Nie, C Hu. Enhanced Fenton catalytic efficiency of γ-Cu–Al2O3 by σ-Cu2+–ligand complexes from aromatic pollutant degradation. Environmental Science & Technology, 2015, 49(14): 8639–8647 https://doi.org/10.1021/acs.est.5b00445
38	Y G Bu, H C Li, W J Yu, Y F Pan, L J Li, Y F Wang, L T Pu, J Ding, G D Gao, B C Pan. Peroxydisulfate activation and singlet oxygen generation by oxygen vacancy for degradation of contaminants. Environmental Science & Technology, 2021, 55(3): 2110–2120 https://doi.org/10.1021/acs.est.0c07274
39	L J Fu, X Y Li, M Z Liu, H M Yang. Insights into the nature of Cu doping in amorphous mesoporous alumina. Journal of Materials Chemistry A, 2013, 1(46): 14592–14605 https://doi.org/10.1039/c3ta13273k
40	Y C Cho, R Y Lin, Y P Lin. Degradation of 2,4-dichlorophenol by CuO-activated peroxydisulfate: importance of surface-bound radicals and reaction kinetics. Science of the Total Environment, 2020, 699: 134379 https://doi.org/10.1016/j.scitotenv.2019.134379
41	X Zhou, M K Ke, G X Huang, C Chen, W X Chen, K Liang, Y T Qu, J Yang, Y Wang, F T Li, H Q Yu, Y Wu. Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density. Proceedings of the National Academy of Sciences of the United States of America, 2022, 119(8): e2119492119 https://doi.org/10.1073/pnas.2119492119
42	B W Li, L Ma, Q H Wu, L Cheng, S Q Zhao, A Khan, X X Li, A H Xu. Mixed nanocomposites of Cu2O and Mn3O4 to activate peroxydisulfate for efficient degradation of tetracycline via Cu(III) species. ACS Applied Nano Materials, 2023, 6(1): 598–606 https://doi.org/10.1021/acsanm.2c04724
43	F E López-Suárez, S Parres-Esclapez, A Bueno-López, M J Illán-Gómez, B Ura, J Trawczynski. Role of surface and lattice copper species in copper-containing (Mg/Sr) TiO3 perovskite catalysts for soot combustion. Applied Catalysis B: Environmental, 2009, 93(1-2): 82–89 https://doi.org/10.1016/j.apcatb.2009.09.015
44	X Duan, H Sun, Z Shao, S Wang. Nonradical reactions in environmental remediation processes: uncertainty and challenges. Applied Catalysis B: Environmental, 2018, 224: 973–982 https://doi.org/10.1016/j.apcatb.2017.11.051
45	K Y Zhao, X H Wang, T Chen, H Wu, J G Li, B X Yang, D Y Li, J F Wei. Bisphenol A adsorption properties of mesoporous CaSiO3@SiO2 grafted nonwoven polypropylene fiber. Industrial & Engineering Chemistry Research, 2017, 56(9): 2549–2556 https://doi.org/10.1021/acs.iecr.6b03015
46	S Bucur, A Diacon, I Mangalagiu, A Mocanu, F Rizea, A Dinescu, A Ghebaur, A C Boscornea, G Voicu, E Rusen. Bisphenol A adsorption on silica particles modified with beta-cyclodextrins. Nanomaterials, 2021, 12(1): 39 https://doi.org/10.3390/nano12010039
47	J Ali, K Zhan, H Wang, A Shahzad, Z Zeng, J Wang, X Zhou, H Ullah, Z Chen, Z Chen. Tuning of persulfate activation from a free radical to a nonradical pathway through the incorporation of non-redox magnesium oxide. Environmental Science & Technology, 2020, 54(4): 2476–2488 https://doi.org/10.1021/acs.est.9b04696
48	H Wang, W Guo, B Liu, Q Wu, H Luo, Q Zhao, Q Si, F Sseguya, N Ren. Edge-nitrogenated biochar for efficient peroxydisulfate activation: an electron transfer mechanism. Water Research, 2019, 160: 405–414 https://doi.org/10.1016/j.watres.2019.05.059

[1]

FCE-23007-OF-FW_suppl_1

Download

[1]	Baohe WANG, Lili WANG, Jing ZHU, Shuang CHEN, Hao SUN. Condensation of phenol and acetone on a modified macroreticular ion exchange resin catalyst[J]. Front Chem Sci Eng, 2013, 7(2): 218-225.

Viewed

Full text

Abstract

Cited

Shared

Discussed