Magnetic Nitrogen-Doped Fe₃C@ c Catalysts for Efficient Activation of Peroxymonosulfate for Degradation of Organic Pollutants

Abstract:

Recoverable and stable nanocatalysts are essential for peroxymonosulfate - based advanced oxidation processes (AOPs) in wastewater purification treatment. In this paper, Fe₃C nanorods @ nitrogen-doped carbon composites (N-Fe₃C@C) with core-shell architecture were fabricated by the co-precipitation and calcination methods, and characterized and analyzed in terms of their crystal structure, microscopic morphology, and surface chemical elements. In addition, N-Fe₃C@C-4 degraded 85.36% of tetracycline in 10 min under PMS, which was much higher than the catalytic ability of Fe₃O₄ (42.03% in 10 min). Both the active radical trapping and EPR experiments verified that ¹O₂ played a key role for degradation of organic dyes in PMS system. The investigation on the degradation mechanism revealed that the presence of the carbon layer facilitated to adsorb TC, accelerate free radical generation and promote the redox cycle of Fe²⁺/Fe³⁺ in the nanocatalyst. This study offers novel ideas for multifunctional catalysts for advanced wastewater purification treatment.

• Periodical: Journal of Nano Research (Volume 83)
• Pages: 17-32
• DOI: https://doi.org/10.4028/p-cAjZK4
• Online since: July 2024
• Authors: Hong Wu Zhu, Yu Song Pan*, Yuan Qing Wang, Yan Lei Xiang, Rong Han, Run Huang
• Keywords: Catalytic Activity, Nitrogen-Doped Carbon, Peroxymonosulfate, Tetracycline

References

[1] S. Zhang, J. Wang, Y. Zhang, J. Ma, L. Huang, S. Yu, L. Chen, G. Song, M. Qiu, X. Wang, Applications of water-stable metal-organic frameworks in the removal of water pollutants: A review, Environ. Pollut, 291 (2021) 118076.

DOI: 10.1016/j.envpol.2021.118076

[2] A.O. Adeola, B.A. Abiodun, D.O. Adenuga, P.N. Nomngongo, Adsorptive and photocatalytic remediation of hazardous organic chemical pollutants in aqueous medium: A review, J. Contam. Hydrol. 248 (2022) 104019.

DOI: 10.1016/j.jconhyd.2022.104019

[3] D. Li, S. Zhang, S. Li, J. Tang, T. Hua, F. Li, Mechanism of the application of single-atom catalyst-activated PMS/PDS to the degradation of organic pollutants in water environment: A review, J. Clean. Prod. 397 (2023) 136468.

DOI: 10.1016/j.jclepro.2023.136468

[4] J. Li, W. Zhu, Y. Gao, P. Lin, J. Liu, J. Zhang, T. Huang, The catalyst derived from the sulfurized Co-doped metal-organic framework (MOF) for peroxymonosulfate (PMS) activation and its application to pollutant removal, Sep. Purif. 285 (2022) 120362.

DOI: 10.1016/j.seppur.2021.120362

[5] Y. Yao, Y. Hu, H. Hu, L. Chen, M. Yu, M. Gao, S. Wang, Metal-free catalysts of graphitic carbon nitride-covalent organic frameworks for efficient pollutant destruction in water, J. Colloid Interface Sci. 554 (2019) 376-387.

DOI: 10.1016/j.jcis.2019.07.002

[6] X. Hong, Y. Zhao, R. Zhuang, J. Liu, G. Guo, J. Chen, Y. Yao, Bioremediation of tetracycline antibiotics-contaminated soil by bioaugmentation, RSC Adv. 10 (2020) 33086.

DOI: 10.1039/d0ra04705h

[7] M. Atif, H.Z. Haider, R. Bongiovanni, M. Fayyaz, T. Razzaq, S. Gul, Physisorption and chemisorption trends in surface modification of carbon black, Surf. Interfaces, 31 (2022) 102030.

DOI: 10.1016/j.surfin.2022.102080

[8] M. Zhang, Z. Zhang, S. Liu, Y. Peng, J. Chen, S.Y. Ki, Ultrasound-assisted electrochemical treatment for phenolic wastewater, Ultrason Sonochem, 65 (2020) 105058.

DOI: 10.1016/j.ultsonch.2020.105058

[9] P. Wu, L. Xie, W. Mo, B. Wang, H. Ge, X. Sun, Y. Tian, R. Zhao, F. Zhu, Y. Zhang, Y. Wang, The biodegradation of carbaryl in soil with Rhodopseudomonas capsulata in wastewater treatment effluent, J. Environ. Manage. 249 (2019) 109226.

DOI: 10.1016/j.jenvman.2019.06.127

[10] Y. Deng, R. Zhao, Advanced Oxidation Processes (AOPs) in Wastewater Treatment, Curr. Pollut. Rep. 1 (2015) 167-176.

DOI: 10.1007/s40726-015-0015-z

[11] M.P. Rayaroth, C.T. Aravindakumar, N.S. Shah, G. Boczkaj, Advanced oxidation processes (AOPs) based wastewater treatment-unexpected nitration side reactions - a serious environmental issue: A review, Chem. Eng. J. 430 (2022) 133002.

DOI: 10.1016/j.cej.2021.133002

[12] X. Yi, T. Wang, H. Chu, Y. Gao, C. Wang, Y. Li, L. Chen, P. Wang, H. Fu, C. Zhao, W. Liu, Effective elimination of tetracycline antibiotics via photoactivated SR-AOP over vivianite: A new application approach of phosphorus recovery product from WWTP, Chem. Eng. J. 449 (2022) 137784.

DOI: 10.1016/j.cej.2022.137784

[13] Y. Wu, Y. Li, T. Zhao, X. Wang, V.I. Isaeva, L.M. Kustov, J. Yao, J. Gao, Bimetal-organic framework-derived nanotube@cellulose aerogels for peroxymonosulfate (PMS) activation, Carbohydr. Polym. 296 (2022) 119969.

DOI: 10.1016/j.carbpol.2022.119969

[14] C. Wang, J. Zhao, C. Chen, P. Na, Catalytic activation of PS/PMS over Fe-Co bimetallic oxides for phenol oxidation under alkaline conditions, Appl. Surf. Sci. 562 (2021) 150134.

DOI: 10.1016/j.apsusc.2021.150134

[15] X. Huang, C. Liu, Z. Zhang, V. Vasanthakumar, H. Ai, L. Xu, M. Fu, B. Yuan, Stable Cu-Co/C carbon-based composites for efficiency catalytic degradation of Orange II by PMS: Effect factors, application potential analysis, and mechanism, J Ind Eng Chem, 126 (2023) 307-316.

DOI: 10.1016/j.jiec.2023.06.021

[16] L. Yang, X. Shan, Y. Zhao, Z. Xiao, Q. An, S. Zhai, Efficient phosphate capture of Fe3O4/UiO-66-NH2/CeO2 in wide pH spectrum, Microporous Mesoporous Mater. 331 (2022) 111653.

DOI: 10.1016/j.micromeso.2021.111653

[17] X. Yang, C. Li, J. Huang, Y. Liu, W. Chen, J. Shen, Y. Zhu, C. Li, Nitrogen-doped Fe3C@C particles as an efficient heterogeneous photo-assisted Fenton catalyst, RSC Adv. 7 (2017) 15168.

DOI: 10.1039/c7ra00486a

[18] J. Shen, Y. Zhu, K. Zhou, X. Yang, C. Li, Tailored anisotropic magnetic conductive film assembled from graphene-encapsulated multifunctional magnetic composite microspheres, J. Mater. Chem. 22 (2012) 545.

DOI: 10.1039/c1jm13216d

[19] M. Lo Faro, R.M. Reis, G.G.A. Saglietti, V.L. Oliveira, S.C. Zignani, S. Trocino, S. Maisano, E.A. Ticianelli, N. Hodnik, F. Ruiz-Zepeda, A.S. Aricò, Solid oxide fuel cells fed with dry ethanol: The effect of a perovskite protective anodic layer containing dispersed Ni-alloy @ FeOx core-shell nanoparticles, Appl. Catal. B, 220 (2018) 98-110.

DOI: 10.1016/j.apcatb.2017.08.010

[20] C. Han, Y. Wang, Y. Lei, B. Wang, N. Wu, Q. Shi, Q. Li, In situ synthesis of graphitic-C3N4 nanosheet hybridized N-doped TiO2 nanofibers for efficient photocatalytic H2 production and degradation, Nano Res. 8 (2015) 1199-1209.

DOI: 10.1007/s12274-014-0600-2

[21] X. Du, H. Liu, Y. Mai, Ultrafast Synthesis of Multifunctional N‑DopedGraphene Foam in an Ethanol Flame, ACS Nano, 10 (2016) 453-462.

DOI: 10.1021/acsnano.5b05373

[22] G. Zhang, Y. Ding, W. Nie, H. Tang, Efficient degradation of drug ibuprofen through catalytic activation of peroxymonosulfate by Fe3C embedded on carbon, J Environ Sci (China), 78 (2019) 1-12.

DOI: 10.1016/j.jes.2018.10.002

[23] Y. Liu, Q. You, X. Yang, G. Liao, D. Wang, Nitrogen rich hollow carbon spheres with well-developed mesoporous: An efficient adsorbent for tetracycline removal. Chem. Eng. J. 10 (2022) 107043.

DOI: 10.1016/j.jece.2021.107043

[24] Y. Long, S. Bu, Y. Huang, Y. Shao, L. Xiao, X. Shi, N-doped hierarchically porous carbon for highly efficient metal-free catalytic activation of peroxymonosulfate in water: A non-radical mechanism, Chemosphere, 216 (2019) 545-555.

DOI: 10.1016/j.chemosphere.2018.10.175

[25] X. Wang, Y. Qin, L. Zhu, H. Tang, Nitrogen-Doped Reduced Graphene Oxide as a Bifunctional Materialfor Removing Bisphenols: Synergistic Effect between Adsorption andCatalysis, Environ. Sci. Technol. 49 (2015) 6855-6864.

DOI: 10.1021/acs.est.5b01059

[26] J. Zhou, X. Li, J. Yuan, Z. Wang, Efficient degradation and toxicity reduction of tetracycline by recyclable ferroferric oxide doped powdered activated charcoal via peroxymonosulfate (PMS) activation, Chem. Eng. J. 441 (2022) 136061.

DOI: 10.1016/j.cej.2022.136061

[27] S. Xue, Z. Xie, X. Ma, Y. Xu, S. Zhang, Q. Jia, R. Wan, H. Tao, Insights into the singlet oxygen mechanism of Fe-doped activated carbon for Rhodamine B advanced oxidation, Microporous Mesoporous Mater. 337 (2022) 111948.

DOI: 10.1016/j.micromeso.2022.111948

[28] Y. Li, T. Yang, S. Qiu, W. Lin, J. Yan, S. Fan, Q. Zhou, Uniform N-coordinated single-atomic iron sites dispersed in porous carbon framework to activate PMS for efficient BPA degradation via high-valent iron-oxo species, Chem. Eng. J. 389 (2020) 124382.

DOI: 10.1016/j.cej.2020.124382

[29] H. Yan, Y. Pan, X. Liao, Y. Zhu, R. Huan, C. Pa, Metal organic framework derived CuSx/C with plentiful S-vacancies for efficient heterogenous activation of peroxymonosulfate, Appl. Surf. Sci. 607 (2023) 155009.

DOI: 10.1016/j.apsusc.2022.155009

[30] S. Han, P. Xiao, L. An, D. Wu, Oxidative degradation of tetracycline using peroxymonosulfate activated by cobalt doped pomelo peel carbon composite, Environ. Sci. Pollut. Res. 29 (2022) 21656-21669.

DOI: 10.1007/s11356-021-17391-9

[31] Y. Wang, C. Liu, Y. Zhang, W. Meng, B. Yu, S. Pu, D. Yuan, F. Qi, B. Xue, W. Chu, Sulfate radical-based photo-Fenton reaction derived by CuBi2O4 and its composites with α-Bi2O3 under visible light irradiation: Catalyst fabrication, performance and reaction mechanism, Appl. Catal. B, 235 (2018) 264-273.

DOI: 10.1016/j.apcatb.2018.04.058

[32] X. Zhou, C. Luo, M. Luo, Q. Wang, J. Wang, Z. Liao, Z. Chen, Z. Chen, Understanding the synergetic effect from foreign metals in bimetallic oxides for PMS activation: A common strategy to increase the stoichiometric efficiency of oxidants, Chem. Eng. J. 381 (2020) 122587.

DOI: 10.1016/j.cej.2019.122587

[33] R. Yuan, L. Hu, P. Yu, H. Wang, Z. Wang, J. Fang, Nanostructured Co3O4 grown on nickel foam: An efficient and readily recyclable 3D catalyst for heterogeneous peroxymonosulfate activation, Chemosphere, 198 (2018) 204-215.

DOI: 10.1016/j.chemosphere.2018.01.135

[34] Y. Long, S. Li, Y. Su, S. Wang, S. Zhao, S. Wang, Z. Zhang, W. Huang, Y. Liu, Z. Zhang, Sulfur-containing iron nanocomposites confined in S/N co-doped carbon for catalytic peroxymonosulfate oxidation of organic pollutants: Low iron leaching, degradation mechanism and intermediates, Chem. Eng. J. 404 (2021) 126499.

DOI: 10.1016/j.cej.2020.126499

[35] Y. Huang, C. Han, Y. Liu, M.N. Nadagouda, L. Machala, K.E. O'Shea, V.K. Sharma, D.D. Dionysiou, Degradation of atrazine by ZnxCu1−xFe2O4 nanomaterial-catalyzed sulfite under UV–vis light irradiation: Green strategy to generate SO●- 4, Appl. Catal. B, 221 (2018) 380-392.

DOI: 10.1016/j.apcatb.2017.09.001

[36] M. Nie, C. Yan, M. Li, X. Wang, W. Bi, W. Dong, Degradation of chloramphenicol by persulfate activated by Fe2+ and zerovalent iron, Chem. Eng. J. 279 (2015) 507-515.

DOI: 10.1016/j.cej.2015.05.055

[37] M. Nie, Y. Yang, Z. Zhang, C. Yan, X. Wang, H. Li, W. Dong, Degradation of chloramphenicol by thermally activated persulfate in aqueous solution, Chem. Eng. J. 246 (2014) 373-382.

DOI: 10.1016/j.cej.2014.02.047

[38] A.M. Dugandžić, A.V. Tomašević, M.M. Radišić, N.Ž. Šekuljica, D.Ž. Mijin, S.D. Petrović, Effect of inorganic ions, photosensitisers and scavengers on the photocatalytic degradation of nicosulfuron, J. Photochem. Photobiol. A, 336 (2017) 146-155.

DOI: 10.1016/j.jphotochem.2016.12.031

[39] J. Wei, D. Han, J. Bi, J. Gong, Fe-doped ilmenite CoTiO3 for antibiotic removal: Electronic modulation and enhanced activation of peroxymonosulfate, Chem. Eng. J. 423 (2021) 130165.

DOI: 10.1016/j.cej.2021.130165

[40] X. Li, Z. Wang, B. Zhang, A.I. Rykova, M.A. Ahmed, J. Wang, FexCo3−xO4 nanocages derived from nanoscale metal–organic frameworks for removal of bisphenol A by activation of peroxymonosulfate, Appl. Catal. B, 181 (2016) 788-799.

DOI: 10.1016/j.apcatb.2015.08.050

[41] H. Yan, Y. Pan, X. Liao, Y. Zhu, R. Huang, C. Pan, Significantly enhanced Fenton-based oxidation processes with CuS-Cu9S8 as co-catalyst by accelerating the Fe3+/Fe2+cycles, Appl. Surf. Sci. 559 (2021) 149952.

DOI: 10.1016/j.apsusc.2021.149952

[42] F. Wang, M. Xiao, X. Ma, S. Wu, M. Ge, X. Yu, Insights into the transformations of Mn species for peroxymonosulfate activation by tuning the Mn3O4 shapes, Chem. Eng. J. 404 (2021) 127097.

DOI: 10.1016/j.cej.2020.127097

[43] S. Ding, J. Wan, Y. Ma, Y. Wang, M. Pu, X. Li, J. Sun, Water stable SiO2-coated Fe-MOF-74 for aqueous dimethyl phthalate degradation in PS activated medium, J. Hazard. Mater. 411 (2021) 125194.

DOI: 10.1016/j.jhazmat.2021.125194

[44] H. Li, Z. Yang, S. Lu, L. Su, C. Wang, J. Huang, J. Zhou, J. Tang, M. Huang, Nano-porous bimetallic CuCo-MOF-74 with coordinatively unsaturated metal sites for peroxymonosulfate activation to eliminate organic pollutants: Performance and mechanism, Chemosphere, 273 (2021) 129643.

DOI: 10.1016/j.chemosphere.2021.129643

[45] S. Gao, H. Zhou, Y. Xia, X. Liu, Y. Yao, W. Wang, H. Chen, Carbon fiber-assisted iron carbide nanoparticles as an efficient catalyst via peroxymonosulfate activation for organic contaminant removal, Catal. Sci. Technol. 9 (2019) 4365-4373.

DOI: 10.1039/c9cy00756c

[46] Z. Wang, Z. Zhu, G. Wang, X. Ma, W. Lu, Iron (II) phthalocyanine loaded tourmaline efficiently activates PMS to degrade pharmaceutical contaminants under solar light, Environ. Technol. 44(2023) 3491-3503.

DOI: 10.1080/09593330.2022.2064236

[47] C. Tan, X. Cheng, T. Xu, K. Chen, H. Xiang, L. Su, Crystalline boron significantly accelerates Fe(III)/PMS reaction as an electron donor: Iron recycling, reactive species generation, and acute toxicity evaluation, Chem. Eng. J. 452 (2023) 139154.

DOI: 10.1016/j.cej.2022.139154

[48] H. Peng, R. Chen, N. Tao, Y. Xiao, C. Li, T. Zhang, M. Ye, MoS2 boosts the Fe2+/PMS process for carbamazepine degradation, Environ. Sci. Pollut. Res. 29 (2022) 49267-49278.

DOI: 10.1007/s11356-022-19172-4