Simultaneous removal of total oxidizable carbon, phosphate and various metallic ions from H<sub>2</sub>O<sub>2</sub> solution with amino-functionalized zirconia as adsorbents

doi:10.1007/s11705-022-2231-6

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (4) : 470-482 https://doi.org/10.1007/s11705-022-2231-6

RESEARCH ARTICLE

Simultaneous removal of total oxidizable carbon, phosphate and various metallic ions from H₂O₂ solution with amino-functionalized zirconia as adsorbents

Yitong Wang¹, Yue Zhang¹, Li Wang^1,²(

)

¹. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
². Zhejiang Institute of Tianjin University, Ningbo 315201, China

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Abstract

Amino-functionalized zirconia was synthesized by the co-condensation method using zirconium butanol and 3-aminopropyltriethoxy silane for the simultaneous removal of various impurities from aqueous 30% H₂O₂ solution. The results of Fourier transform infrared (FTIR) and Zeta potential showed that the content of N in amino-functionalized zirconia increased with the added amount of 3-aminopropyltriethoxy silane. Accordingly, the removal efficiency of total oxidizable carbon, phosphate and metallic ions from the H₂O₂ solution increased. The adsorbent with an N content of 1.62% exhibited superior adsorption performance. The removal efficiency of 82.7% for total oxidizable carbon, 34.2% for phosphate, 87.1% for Fe³⁺, 83.2% for Al³⁺, 55.1% for Ca²⁺ and 66.6% for Mg²⁺, with a total adsorption capacity of 119.6 mg·g^–1, could be achieved. The studies conducted using simulated solutions showed that the adsorption process of phosphate on amino-functionalized zirconia is endothermic and spontaneous, and the behaviors could be well described by the pseudo-second-order model and Langmuir model with a maximum adsorption capacity of 186.7 mg·g^–1. The characterizations of the spent adsorbents by Zeta potential, FTIR and X-ray photoelectron spectroscopy revealed that the adsorption mechanism of phosphate is predominantly electrostatic attraction by the protonated functional groups and complementary ligand exchange with zirconium hydroxyl groups.

Keywords adsorption zirconia total oxidizable carbon phosphate metallic ions hydrogen peroxide

Corresponding Author(s): Li Wang

Online First Date: 10 January 2023 Issue Date: 24 March 2023

Cite this article:

Yitong Wang,Yue Zhang,Li Wang. Simultaneous removal of total oxidizable carbon, phosphate and various metallic ions from H₂O₂ solution with amino-functionalized zirconia as adsorbents[J]. Front. Chem. Sci. Eng., 2023, 17(4): 470-482.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2231-6
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I4/470

Tab.1 Physicochemical properties of Zr-N-2 and ZrO₂-UN

Fig.1 XRD patterns of Zr-N-Xs and ZrO₂-UN.

Fig.2 FTIR spectra of Zr-N-Xs and ZrO₂-UN.

Fig.3 TGA curves of Zr-N-Xs and ZrO₂-UN (inset: DTG curves).

Fig.4 Zeta potential of Zr-N-Xs and ZrO₂-UN.

Fig.5 Removal efficiency of (a) TOC and phosphate and (b) metallic ions from real H₂O₂ solution.

Tab.2 Adsorption results in the real H₂O₂ solution

Fig.6 Adsorption kinetics of phosphate at 30 °C and initial concentration of 200 mg·L^–1. (a) PFOM and (b) PSOM.

Fig.7 Adsorption equilibrium isotherm of phosphate in simulated solution at pH 3 and 30 °C. (a) Langmuir model and (b) Freundlich model.

Tab.3 Thermodynamic properties for phosphate adsorption process on ZrO₂-UN and Zr-N-2

Fig.8 Zeta potential of spent adsorbents (S-ZrO₂-UN and S-Zr-N-2 mean used ZrO₂-UN and Zr-N-2 in simulated phosphate solution of 200 mg·L^–1 at pH = 3).

Fig.9 FTIR spectra of spent adsorbents.

Fig.10 XPS spectra of fresh and spent adsorbents. (a) O 1s spectra; (b) Zr 3d spectra; (c) N 1s spectra; (d) P 2p spectra.

Scheme1 Adsorption mechanisms of phosphate on amino-functionalized zirconia.

1	H Li, B Zheng, Z Pan, B Zong, M Qiao. Advances in the slurry reactor technology of the anthraquinone process for H2O2 production. Frontiers of Chemical Science and Engineering, 2018, 12(1): 124–131 https://doi.org/10.1007/s11705-017-1676-5
2	Y Bu, Y Wang, G Han, Y Zhao, X Ge, F Li, Z Zhang, Q Zhong, J B Baek. Carbon-based electrocatalysts for efficient hydrogen peroxide production. Advanced Materials, 2021, 33(49): 2103266 https://doi.org/10.1002/adma.202103266
3	J Liang, F Wang, W Li, J Zhang, C Guo. Highly dispersed and stabilized Pd species on H2 pre-treated Al2O3 for anthraquinone hydrogenation and H2O2 production. Molecular Catalysis, 2022, 524: 112264 https://doi.org/10.1016/j.mcat.2022.112264
4	E Yuan, X Ren, L Wang, W Zhao. A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a Pd/Al2O3 catalyst. Frontiers of Chemical Science and Engineering, 2017, 11(2): 177–184 https://doi.org/10.1007/s11705-016-1604-0
5	G Luan, W Gao, P Yao. Progress on the preparation of ultra-pure hydrogen peroxide. Journal of Industrial and Engineering Chemistry, 2007, 13(7): 1047–1053
6	F Zhang, M Chen, X Jia, W Xu, N Shi. Research on the effect of resin on the thermal stability of hydrogen peroxide. Process Safety and Environmental Protection, 2019, 126: 1–6 https://doi.org/10.1016/j.psep.2019.03.040
7	R Abejon, A Garea, A Irabien. Integrated countercurrent reverse osmosis cascades for hydrogen peroxide ultrapurification. Computers & Chemical Engineering, 2012, 41: 67–76 https://doi.org/10.1016/j.compchemeng.2012.02.017
8	R Abejon, A Garea, A Irabien. Ultrapurification of hydrogen peroxide solution from ionic metals impurities to semiconductor grade by reverse osmosis. Separation and Purification Technology, 2010, 76(1): 44–51 https://doi.org/10.1016/j.seppur.2010.09.018
9	R Abejon, A Garea, A Irabien. Effective lifetime study of commercial reverse osmosis membranes for optimal hydrogen peroxide ultrapurification processes. Industrial & Engineering Chemistry Research, 2013, 52(48): 17270–17284 https://doi.org/10.1021/ie402895p
10	Q Lin, Y Jiang, J Geng, Y Qian. Removal of organic impurities with activated carbons for ultra-pure hydrogen peroxide preparation. Chemical Engineering Journal, 2008, 139(2): 264–271 https://doi.org/10.1016/j.cej.2007.07.091
11	Y Zhao, X Shan, Q An, Z Xiao, S Zhai. Interfacial integration of zirconium components with amino-modified lignin for selective and efficient phosphate capture. Chemical Engineering Journal, 2020, 398: 125561 https://doi.org/10.1016/j.cej.2020.125561
12	L Ouni, A Ramazani, S T Fardood. An overview of carbon nanotubes role in heavy metals removal from wastewater. Frontiers of Chemical Science and Engineering, 2019, 13(2): 274–295 https://doi.org/10.1007/s11705-018-1765-0
13	L Wang, C Shi, L Wang, L Pan, X Zhang, J Zou. Rational design, synthesis, adsorption principles and applications of metal oxide adsorbents: a review. Nanoscale, 2020, 12(8): 4790–4815 https://doi.org/10.1039/C9NR09274A
14	P Xu, G Zeng, D Huang, C Feng, S Hu, M Zhao, C Lai, Z Wei, C Huang, G Xie, Z F Liu. Use of iron oxide nanomaterials in wastewater treatment: a review. Science of the Total Environment, 2012, 424: 1–10 https://doi.org/10.1016/j.scitotenv.2012.02.023
15	M Hua, S Zhang, B Pan, W Zhang, L Lv, Q Zhang. Heavy metal removal from water/wastewater by nanosized metal oxides: a review. Journal of Hazardous Materials, 2012, 211-212: 317–331 https://doi.org/10.1016/j.jhazmat.2011.10.016
16	V B Cashin, D S Eldridge, A Yu, D Zhao. Surface functionalization and manipulation of mesoporous silica adsorbents for improved removal of pollutants: a review. Environmental Science. Water Research & Technology, 2018, 4(2): 110–128 https://doi.org/10.1039/C7EW00322F
17	S Sonal, B K Mishra. A comprehensive review on the synthesis and performance of different zirconium-based adsorbents for the removal of various water contaminants. Chemical Engineering Journal, 2021, 424: 130509 https://doi.org/10.1016/j.cej.2021.130509
18	J Lin, Y Zhan, H Wang, M Chu, C Wang, Y He, X Wang. Effect of calcium ion on phosphate adsorption onto hydrous zirconium oxide. Chemical Engineering Journal, 2017, 309: 118–129 https://doi.org/10.1016/j.cej.2016.10.001
19	K Shehzad, M Ahmad, C Xie, D Zhan, W Wang, Z Li, W Xu, J Liu. Mesoporous zirconia nanostructures (MZN) for adsorption of As(III) and As(V) from aqueous solutions. Journal of Hazardous Materials, 2019, 373: 75–84 https://doi.org/10.1016/j.jhazmat.2019.01.021
20	L Song, J Li, H Zong, Y Lin, H Ding, L Huang, P Zhang, X Lai, G Liu, Y Fan. Zirconia nano-powders with controllable polymorphs synthesized by a wet chemical method and their phosphate adsorption characteristics & mechanism. Ceramics International, 2022, 48(5): 6591–6599 https://doi.org/10.1016/j.ceramint.2021.11.208
21	Y Ma, D Zhu, C Wang, Y Zhang, Y Shang, F Liu, T Ye, X Chen, Z Wei. Simultaneous and fast separation of three chlorogenic acids and two flavonoids from bamboo leaves extracts using zirconia. Food and Chemical Toxicology, 2018, 119: 375–379 https://doi.org/10.1016/j.fct.2018.02.008
22	L Treccani, T Y Klein, F Meder, K Pardun, K Rezwan. Functionalized ceramics for biomedical, biotechnological and environmental applications. Acta Biomaterialia, 2013, 9(7): 7115–7150 https://doi.org/10.1016/j.actbio.2013.03.036
23	B Wu, J Wan, Y Zhang, B Pan, I M C Lo. Selective phosphate removal from water and wastewater using sorption: process fundamentals and removal mechanisms. Environmental Science & Technology, 2020, 54(1): 50–66 https://doi.org/10.1021/acs.est.9b05569
24	A Majedi, F Davar, A Abbasi. Citric acid-silane modified zirconia nanoparticles: preparation, characterization and adsorbent efficiency. Journal of Environmental Chemical Engineering, 2018, 6(1): 701–709 https://doi.org/10.1016/j.jece.2017.12.059
25	T Mahmood, A Ullah, R Ali, A Naeem, M Farooq, M Aslam. Amino functionalized zirconia as novel adsorbent for removal of Cr(VI) from aqueous solutions: kinetics, equilibrium, and thermodynamics studies. Desalination and Water Treatment, 2021, 210: 377–392 https://doi.org/10.5004/dwt.2021.26567
26	G Liu, C Wu, X Zhang, Y Liu, H Meng, J Xu, Y Han, X Xu, Y Xu. Surface functionalization of zirconium dioxide nano-adsorbents with 3-aminopropyl triethoxysilane and promoted adsorption activity for bovine serum albumin. Materials Chemistry and Physics, 2016, 176: 129–135 https://doi.org/10.1016/j.matchemphys.2016.03.042
27	X Wang, K Li, G Liang, Y Zhao, R Su, Z Luan, L Li, H Xi. Amino-modified zirconia aerogels for the efficient filtration of NO2: effects of water on the removal mechanisms. Environmental Science. Nano, 2021, 8(12): 3722–3734 https://doi.org/10.1039/D1EN00829C
28	S Rana, S Mallick, K M Parida. Facile method for synthesis of polyamine-functionalized mesoporous zirconia and its catalytic evaluation toward henry reaction. Industrial & Engineering Chemistry Research, 2011, 50(4): 2055–2064 https://doi.org/10.1021/ie101777a
29	Y Su, H Cui, Q Li, S Gao, J Shang. Strong adsorption of phosphate by amorphous zirconium oxide nanoparticles. Water Research, 2013, 47(14): 5018–5026 https://doi.org/10.1016/j.watres.2013.05.044
30	Y He, A Jawad, X Li, M Atanga, F Rezaei, A A Rownaghi. Direct aldol and nitroaldol condensation in an aminosilane-grafted Si/Zr/Ti composite hollow fiber as a heterogeneous catalyst and continuous-flow reactor. Journal of Catalysis, 2016, 341: 149–159 https://doi.org/10.1016/j.jcat.2016.07.001
31	Q Ma, N Wang, G Liu, L Wang. Enhanced performance of Pd nanoparticles on SBA-15 grafted with alkyltrialkoxysilane in 2-ethyl-anthraquinone hydrogenation. Microporous and Mesoporous Materials, 2019, 279: 245–251 https://doi.org/10.1016/j.micromeso.2018.12.037
32	L Wang, Y Zhang, Q Ma, Z Pan, B Zong. Hydrogenation of alkyl-anthraquinone over hydrophobically functionalized Pd/SBA-15 catalysts. RSC Advances, 2019, 9(59): 34581–34588 https://doi.org/10.1039/C9RA07351E
33	T Mongkol, P Phuwadej, W Anyarat, S Nagahiro. Liquid-phase plasma-assisted in situ synthesis of amino-rich nanocarbon for transition metal ion adsorption. ACS Applied Nano Materials, 2020, 3(1): 218–228 https://doi.org/10.1021/acsanm.9b01915
34	H Bacelo, A M A Pintor, S C R Santos, R A R Boaventura, C M S Botelho. Performance and prospects of different adsorbents for phosphorus uptake and recovery from water. Chemical Engineering Journal, 2020, 381: 122566 https://doi.org/10.1016/j.cej.2019.122566
35	K F Lam, K L Yeung, G Mckay. Selective mesoporous adsorbents for Cr2O72– and Cu2+ separation. Microporous and Mesoporous Materials, 2007, 100(1-3): 191–201 https://doi.org/10.1016/j.micromeso.2006.10.037
36	T Yokoi, T Tatsumi, H Yoshitake. Fe3+ coordinated to amino-functionalized MCM-41: an adsorbent for the toxic oxyanions with high capacity, resistibility to inhibiting anions, and reusability after a simple treatment. Journal of Colloid and Interface Science, 2004, 274(2): 451–457 https://doi.org/10.1016/j.jcis.2004.02.037
37	B Liu, Z Liu, H Wu, S Pan, Y Sun, Y Xu. Insight into simultaneous selective removal of nitrogen and phosphorus species by lanthanum-modified porous polymer: performance, mechanism and application. Chemical Engineering Journal, 2021, 415: 129026 https://doi.org/10.1016/j.cej.2021.129026
38	E Salehi, F Soroush, M Momeni, A Barati, A Khakpour. Chitosan/polyethylene glycol impregnated activated carbons: synthesis, characterization and adsorption performance. Frontiers of Chemical Science and Engineering, 2017, 11(4): 575–585 https://doi.org/10.1007/s11705-017-1650-2
39	F Li, C Chen, Y Wang, W Li, G Zhou, H Zhang, J Zhang, J Wang. Activated carbon-hybridized and amine-modified polyacrylonitrile nanofibers toward ultrahigh and recyclable metal ion and dye adsorption from wastewater. Frontiers of Chemical Science and Engineering, 2021, 15(4): 984–997 https://doi.org/10.1007/s11705-020-2000-3
40	E Zong, X Liu, J Jiang, S Fu, F Chu. Preparation and characterization of zirconia-loaded lignocellulosic butanol residue as a biosorbent for phosphate removal from aqueous solution. Applied Surface Science, 2016, 387: 419–430 https://doi.org/10.1016/j.apsusc.2016.06.107
41	B Wu, I M C Lo. Surface functional group engineering of CeO2 particles for enhanced phosphate adsorption. Environmental Science & Technology, 2020, 54(7): 4601–4608 https://doi.org/10.1021/acs.est.9b06812
42	H Fu, Y Yang, R Zhu, J Liu, M Usman, Q Chen, H He. Superior adsorption of phosphate by ferrihydrite-coated and lanthanum decorated magnetite. Journal of Colloid and Interface Science, 2018, 530: 704–713 https://doi.org/10.1016/j.jcis.2018.07.025
43	Z Yan, L Fu, H Yang, J Ouyang. Amino-functionalized hierarchical porous SiO2-AlOOH composite nanosheets with enhanced adsorption performance. Journal of Hazardous Materials, 2018, 344: 1090–1100 https://doi.org/10.1016/j.jhazmat.2017.11.058
44	Y Shang, X Xu, S Qi, Y Zhao, Z Ren, B Gao. Preferable uptake of phosphate by hydrous zirconium oxide nanoparticles embedded in quaternary-ammonium Chinese reed. Journal of Colloid and Interface Science, 2017, 496: 118–129 https://doi.org/10.1016/j.jcis.2017.02.019
45	K Yang, L Yan, Y Yang, S Yu, R Shan, H Yu, B Zhu, B Du. Adsorptive removal of phosphate by Mg−Al and Zn−Al layered double hydroxides: kinetics, isotherms and mechanisms. Separation and Purification Technology, 2014, 124: 36–42 https://doi.org/10.1016/j.seppur.2013.12.042

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