Synthesis of porous carbon nanomaterials and their application in tetracycline removal from aqueous solutions

doi:10.1016/j.cjche.2022.12.014

Abstract

Abstract: The low-cost and efficient elimination of tetracycline from wastewater and to decrease the concentration in soils, sediments, rivers, underground water, or lakes are crucial to human health. Herein, three-dimensional porous carbon nanomaterials were synthesized using glucose and NH₄Cl by sugar-blowing process at 900 ℃ and then oxidized under air atmosphere for surface functional group modification. The prepared 3D porous carbon nanomaterials were applied for the removal of tetracycline from aqueous solutions. The sorption isotherms were well simulated by the Langmuir model, with the calculated sorption capacity of 2378 mg·g^-1 for C-450 at pH = 6.5, which was the highest value of today’s reported materials. The porous carbon nanomaterials showed high stability at acidic conditions and selectivity in high salt concentrations. The good recycle ability and high removal efficiency of tetracycline from natural groundwater indicated the potential application of the porous carbon nanomaterials in natural environmental antibiotic pollution cleanup. The outstanding sorption properties were attributed to the structures, surface areas and functional groups, strong interactions such as H-bonding, π-π interaction, electrostatic attraction, etc. This paper highlighted the synthesis of porous carbon nanomaterials with high specific surfaces, high sorption capacities, stability, and reusability in organic chemicals’ pollution treatment.

Key words: Porous carbon nanomaterials, Tetracycline, Sorption, Pollution management

摘要： The low-cost and efficient elimination of tetracycline from wastewater and to decrease the concentration in soils, sediments, rivers, underground water, or lakes are crucial to human health. Herein, three-dimensional porous carbon nanomaterials were synthesized using glucose and NH₄Cl by sugar-blowing process at 900 ℃ and then oxidized under air atmosphere for surface functional group modification. The prepared 3D porous carbon nanomaterials were applied for the removal of tetracycline from aqueous solutions. The sorption isotherms were well simulated by the Langmuir model, with the calculated sorption capacity of 2378 mg·g^-1 for C-450 at pH = 6.5, which was the highest value of today’s reported materials. The porous carbon nanomaterials showed high stability at acidic conditions and selectivity in high salt concentrations. The good recycle ability and high removal efficiency of tetracycline from natural groundwater indicated the potential application of the porous carbon nanomaterials in natural environmental antibiotic pollution cleanup. The outstanding sorption properties were attributed to the structures, surface areas and functional groups, strong interactions such as H-bonding, π-π interaction, electrostatic attraction, etc. This paper highlighted the synthesis of porous carbon nanomaterials with high specific surfaces, high sorption capacities, stability, and reusability in organic chemicals’ pollution treatment.

关键词: Porous carbon nanomaterials, Tetracycline, Sorption, Pollution management

Sufei Wang, Mengjie Hao, Danyang Xiao, Tianmiao Zhang, Hua Li, Zhongshan Chen. Synthesis of porous carbon nanomaterials and their application in tetracycline removal from aqueous solutions[J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 200-209.

References

[1] Z.B. Xu, D.C.W. Tsang, Redox-induced transformation of potentially toxic elements with organic carbon in soil, carbon res 1 (1) (2022) 9.
[2] S.C. Shao, X.W. Wu, Microbial degradation of tetracycline in the aquatic environment: A review, Crit. Rev. Biotechnol. 40 (7) (2020) 1010-1018.
[3] Z.M. Lv, W.W. Chen, Y.W. Cai, K.C. Chen, K.X. Li, M. Fang, X.L. Tan, X.K. Wang, Homogeneous Ni nanoparticles anchored on mesoporous N-doped carbon as highly efficient catalysts for Cr(VI), tetracycline and dyes reduction, Appl. Surf. Sci. 575 (2022) 151748.
[4] Y.W. Cai, Q. Ling, Y.M. Yi, Z.S. Chen, H. Yang, B.W. Hu, L.P. Liang, X.K. Wang, Application of covalent organic frameworks in environmental pollution management, Appl. Catal. A Gen. 643 (2022) 118733.
[5] Y.T. Zou, Y.Z. Hu, Z.W. Shen, L. Yao, D.Y. Tang, S. Zhang, S.Q. Wang, B.W. Hu, G.X. Zhao, X.K. Wang, Application of aluminosilicate clay mineral-based composites in photocatalysis, J. Environ. Sci. 115 (2022) 190-214.
[6] K. Zhang, H.H. Wu, H.Q. Huo, Y.L. Ji, Y. Zhou, C.J. Gao, Recent advances in nanofiltration, reverse osmosis membranes and their applications in biomedical separation field, Chin. J. Chem. Eng. 49 (2022) 76-99.
[7] H.G. Liang, C.X. Zhu, A.H. Wang, K. Palanisamy, F. Chen, Facile synthesis of NiAl₂O₄/g-C₃N₄ composite for efficient photocatalytic degradation of tetracycline, J. Environ. Sci. 127 (2023) 700-713.
[8] K. Perumal, S. Shanavas, T. Ahamad, A. Karthigeyan, P. Murugakoothan, Construction of Ag₂CO₃/BiOBr/CdS ternary composite photocatalyst with improved visible-light photocatalytic activity on tetracycline molecule degradation, J. Environ. Sci. 125 (2023) 47-60.
[9] Y.Q. Wang, K. Li, M.Y. Shang, Y.Z. Zhang, Y. Zhang, B.L. Li, Y.J. Kan, X.Q. Cao, J. Zhang, A novel partially carbonized Fe₃O₄@PANI-p catalyst for tetracycline degradation via peroxymonosulfate activation, Chem. Eng. J. 451 (2023) 138655.
[10] C.C. Wang, M.J. Cai, Y.P. Liu, F. Yang, H.Q. Zhang, J.S. Liu, S.J. Li, Facile construction of novel organic-inorganic tetra (4-carboxyphenyl) porphyrin/Bi₂MoO₆ heterojunction for tetracycline degradation: Performance, degradation pathways, intermediate toxicity analysis and mechanism insight, J. Colloid Interface Sci. 605 (2022) 727-740.
[11] L.L. Su, M.J. Chen, L. Gong, H. Yang, C. Chen, J. Wu, L. Luo, G. Yang, L.L. Lu, Boost activation of peroxymonosulfate by iron doped K_2-xMn₈O₁₆: Mechanism and properties, Chin. J. Chem. Eng. (2022)
[12] Y. Lu, Y.W. Cai, S. Zhang, L. Zhuang, B.W. Hu, S.H. Wang, J.R. Chen, X.K. Wang, Application of biochar-based photocatalysts for adsorption-(photo)degradation/reduction of environmental contaminants: Mechanism, challenges and perspective, Biochar 4 (1) (2022) 45.
[13] M.Q. Qiu, L.J. Liu, Q. Ling, Y.W. Cai, S.J. Yu, S.Q. Wang, D. Fu, B.W. Hu, X.K. Wang, Biochar for the removal of contaminants from soil and water: A review, Biochar 4 (1) (2022) 19.
[14] L. Yao, Y.Z. Hu, Y.T. Zou, Z.Y. Ji, S.X. Hu, C. Wang, P. Zhang, H. Yang, Z.W. Shen, D.Y. Tang, S. Zhang, G.X. Zhao, X.K.Wang, Selective and efficient photoextraction of aqueous Cr(VI) as a solid-state polyhydroxy Cr(V) complex for environmental remediation and resource recovery, Environ. Sci. Technol. 56 (19) (2022) 14030-14037.
[15] L. Yao, Z.W. Shen, Z.Y. Ji, Y.Z. Hu, D.Y. Tang, G.X. Zhao, X.K. Wang, Cr(VI) detoxification and simultaneous selective recovery of Cr resource from wastewater via photo-chemical extraction using biomass, Sci. Bull. (Beijing) 67 (21) (2022) 2154-2157.
[16] Y.F. Zhang, H.X. Liu, F.X. Gao, X.L. Tan, Y.W. Cai, B.W. Hu, Q.F. Huang, M. Fang, X.K. Wang, Application of MOFs and COFs for photocatalysis in CO₂ reduction, H₂ generation, and environmental treatment, EnergyChem 4 (4) (2022) 100078.
[17] P. Yukhajon, T. Somboon, S. Sansuk, Enhanced adsorption and colorimetric detection of tetracycline antibiotics by using functional phosphate/carbonate composite with nanoporous network coverage, J. Environ. Sci. (China) 126 (2023) 365-377.
[18] Y.C. Jiang, M.F. Luo, Z.N. Niu, S.Y. Xu, Y. Gao, Y. Gao, W.J. Gao, J.J. Luo, R.L. Liu, In-situ growth of bimetallic FeCo-MOF on magnetic biochar for enhanced clearance of tetracycline and fruit preservation, Chem. Eng. J. 451 (2023) 138804.
[19] Z.L. Yin, Y.L. Liu, S.H. Zhou, Z. Yang, W.B. Yang, Constructing zirconium based metal-organic frameworks based electrically-driven self-cleaning membrane for removal of tetracycline: Effect of ligand substitution, Chem. Eng. J. 450 (2022) 138100.
[20] P. Yadav, A. Yadav, P.K. Labhasetwar, Sustainable adsorptive removal of antibiotics from aqueous streams using Fe₃O₄-functionalized MIL101(Fe) chitosan composite beads, Environ Sci Pollut Res 29 (25) (2022) 37204-37217.
[21] J.W. Zhao, F. Gao, Y. Sun, W.Y. Fang, X.H. Li, Y.J. Dai, New use for biochar derived from bovine manure for tetracycline removal, J. Environ. Chem. Eng. 9 (4) (2021) 105585.
[22] H.D. Liu, G.R. Xu, G.B. Li, Preparation of porous biochar based on pharmaceutical sludge activated by NaOH and its application in the adsorption of tetracycline, J. Colloid Interface Sci. 587 (2021) 271-278.
[23] B. Li, Y. Zhang, J. Xu, Y.L. Mei, S.S. Fan, H.C. Xu, Effect of carbonization methods on the properties of tea waste biochars and their application in tetracycline removal from aqueous solutions, Chemosphere 267 (2021) 129283.
[24] X.L. Liu, G. Verma, Z.S. Chen, B.W. Hu, Q.F. Huang, H. Yang, S.Q. Ma, X.K. Wang, Metal-organic framework nanocrystal-derived hollow porous materials: Synthetic strategies and emerging applications, Innov. 3 (5) (2022) 100281.
[25] S. Zhang, Y. Liu, R. Ma, D.S. Jia, T. Wen, Y.J. Ai, G.X. Zhao, F. Fang, B.W. Hu, X.K.Wang, Molybdenum (VI)-oxo clusters incorporation activates g-C₃N₄ with simultaneously regulating charge transfer and reaction centers for boosting photocatalytic performance, Adv. Funct. Mater. 32 (38) (2022) 2204175.
[26] Z.X. Liu, Z.Y. Xu, L.F. Xu, F. Buyong, T.C. Chay, Z. Li, Y.W. Cai, B.W. Hu, Y.L. Zhu, X.K. Wang, Modified biochar: Synthesis and mechanism for removal of environmental heavy metals, carbon res 1 (1) (2022) 8.
[27] H. Yang, Y.F. Liu, Z.S. Chen, G.I.N. Waterhouse, S.Q. Ma, X.K. Wang, Emerging technologies for uranium extraction from seawater, Sci. China Chem. 65 (12) (2022) 2335-2337.
[28] M.J. Hao, Z.S. Chen, X.L. Liu, X.H. Liu, J.Y. Zhang, H. Yang, G.I.N. Waterhouse, X.K. Wang, S.Q.Ma, Converging cooperative functions into the nanospace of covalent organic frameworks for efficient uranium extraction from seawater, CCS Chem. 4 (7) (2022) 2294-2307.
[29] X.L. Liu, Y.H. Xie, M.J. Hao, Z.S. Chen, H. Yang, G.I.N. Waterhouse, S.Q. Ma, X.K. Wang, Highly efficient electrocatalytic uranium extraction from seawater over an amidoxime-functionalized In-N-C catalyst, Adv. Sci. (Weinh) 9 (23) (2022) e2201735.
[30] M.Q. Qiu, B.W. Hu, Z.S. Chen, H. Yang, L. Zhuang, X.K. Wang, Challenges of organic pollutant photocatalysis by biochar-based catalysts, Biochar 3 (2) (2021) 117-123.
[31] X.B. Wang, Y.J. Zhang, C.Y. Zhi, X. Wang, D.M. Tang, Y.B. Xu, Q.H. Weng, X.F. Jiang, M. Mitome, D. Golberg, Y. Bando, Three-dimensional strutted graphene grown by substrate-free sugar blowing for high-power-density supercapacitors, Nat. Commun. 4 (2013) 2905.
[32] Z.S. Chen, X. He, Q. Li, H. Yang, Y. Liu, L.N. Wu, Z.X. Liu, B.W. Hu, X.K. Wang, Low-temperature plasma induced phosphate groups onto coffee residue-derived porous carbon for efficient U(VI) extraction, J. Environ. Sci. 122 (2022) 1-13.
[33] M.J. Hao, Z.S. Chen, H. Yang, G.I.N. Waterhouse, S.Q. Ma, X.K. Wang, Pyridinium salt-based covalent organic framework with well-defined nanochannels for efficient and selective capture of aqueous ⁹⁹TcO₄^-, Sci. Bull. 67 (9) (2022) 924-932.
[34] S.D. Perera, R.G. Mariano, K. Vu, N. Nour, O. Seitz, Y. Chabal, K.J. Balkus Jr, Hydrothermal synthesis of graphene-TiO₂ nanotube composites with enhanced photocatalytic activity, ACS Catal. 2 (6) (2012) 949-956.
[35] H. Ren, D.D. Kulkarni, R. Kodiyath, W.N. Xu, I. Choi, V.V. Tsukruk, Competitive adsorption of dopamine and rhodamine 6G on the surface of graphene oxide, ACS Appl. Mater. Interfaces 6 (4) (2014) 2459-2470.
[36] M. Thommes, K. Kaneko, A.V. Neimark, J.P. Olivier, F. Rodriguez-Reinoso, J. Rouquerol, K.S.W.Sing, Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report), Pure Appl. Chem. 87 (9-10) (2015) 1051-1069.
[37] Y.C. Si, E.T. Samulski, Synthesis of water soluble graphene, Nano Lett. 8 (6) (2008) 1679-1682.
[38] X.L. Wang, S. Tao, B.S. Xing, Sorption and competition of aromatic compounds and humic acid on multiwalled carbon nanotubes, Environ. Sci. Technol. 43 (16) (2009) 6214-6219.
[39] X.Y. Chen, S. Shi, X.M. Han, M. Li, Y. Nian, J. Sun, W.T. Zhang, T.L. Yue, J.L. Wang, Insights into high-efficient removal of tetracycline by a codoped mesoporous carbon adsorbent, Chin. J. Chem. Eng. 44 (2022) 148-156.
[40] M.B. Cao, X. Liu, H.B. Yang, Facile construction of high-performance 3D Co₂C-doped CoAl₂O₄ fiber composites for capturing and decomposing tetracycline from aqueous solution, J. Hazard. Mater. 424 (2022) 127307.
[41] B.Y. Zhang, H. Xu, M.M. Wang, L.H. Su, S.J. Zhang, Y.T. Zhang, Q.G. Wang, Bismuth (III)-based metal-organic framework for tetracycline removal via adsorption and visible light catalysis processes, J. Environ. Chem. Eng. 10 (5) (2022) 108469.