Bio-capped and green synthesis of ZnO/g-C3N4 nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation

doi:10.1016/j.cjche.2022.07.031

Chinese Journal of Chemical Engineering ›› 2023, Vol. 56 ›› Issue (4): 215-224.DOI: 10.1016/j.cjche.2022.07.031

Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation

Iltaf Khan¹, Chunjuan Wang², Shoaib Khan³, Jinyin Chen⁴, Aftab Khan², Sayyar Ali Shah¹, Aihua Yuan¹, Sohail Khan⁵, Mehwish K. Butt⁶, Humaira Asghar⁷

1. School of Environmental & Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212100, China;
2. College of Agriculture, Shihezi University, Shihezi 832003, China;
3. Key Laboratory of Biology and Genetic Improvement of Horticultural Crops, Northeast Agricultural University, Harbin 150030, China;
4. Jiangxi Key Laboratory for Postharvest Technology and Nondestructive Testing of Fruits and Vegetables, College of Agronomy, Jiangxi Agricultural University, Nanchang 330045, China;
5. Department of Pharmacy, University of Swabi, Khyber Pakhtunkhwa 94640, Pakistan;
6. Department of Physics, University of Agriculture Faisalabad, Faisalabad 38040, Pakistan;
7. Department of Chemistry, Government College University Faisalabad, Faisalabad 38000, Pakistan

Received:2022-05-07 Revised:2022-07-06 Online:2023-06-13 Published:2023-04-28
Contact: Iltaf Khan,E-mail:doctoriltafkhan@just.edu.cn;Chunjuan Wang,E-mail:wchunjuan@126.com;Sayyar Ali Shah,E-mail:sayyar786@gmail.com
Supported by:
The authors are grateful to Jiangsu University of Science and Technology for providing financial support under the “Research start-up fund for the introduction of young talent at Jiangsu University of Science and Technology (Grant no. 1112932205) and High-level Talents Program of Shihezi University (RCZK2021B25).

Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation

Iltaf Khan¹, Chunjuan Wang², Shoaib Khan³, Jinyin Chen⁴, Aftab Khan², Sayyar Ali Shah¹, Aihua Yuan¹, Sohail Khan⁵, Mehwish K. Butt⁶, Humaira Asghar⁷

1. School of Environmental & Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212100, China;
2. College of Agriculture, Shihezi University, Shihezi 832003, China;
3. Key Laboratory of Biology and Genetic Improvement of Horticultural Crops, Northeast Agricultural University, Harbin 150030, China;
4. Jiangxi Key Laboratory for Postharvest Technology and Nondestructive Testing of Fruits and Vegetables, College of Agronomy, Jiangxi Agricultural University, Nanchang 330045, China;
5. Department of Pharmacy, University of Swabi, Khyber Pakhtunkhwa 94640, Pakistan;
6. Department of Physics, University of Agriculture Faisalabad, Faisalabad 38040, Pakistan;
7. Department of Chemistry, Government College University Faisalabad, Faisalabad 38000, Pakistan

通讯作者: Iltaf Khan,E-mail:doctoriltafkhan@just.edu.cn;Chunjuan Wang,E-mail:wchunjuan@126.com;Sayyar Ali Shah,E-mail:sayyar786@gmail.com
基金资助:
The authors are grateful to Jiangsu University of Science and Technology for providing financial support under the “Research start-up fund for the introduction of young talent at Jiangsu University of Science and Technology (Grant no. 1112932205) and High-level Talents Program of Shihezi University (RCZK2021B25).

Abstract

Abstract: In this research study, we have synthesized the bio-capped ZnO/g-C₃N₄ nanocomposites by employing lemon juice (Citrus limon) as a stabilizer and mediator. Fruitfully, lemon juice which contains various acidic functional groups and citric acid has the capability to block the surface of g-C₃N₄ from chemical reactivity and activated the surface of g-C₃N₄ for various reactions. Consequently, the agglomeration behavior and controlled shape of g-C₃N₄ has also been achieved. Our experimental results i.e. XRD, TEM, HRTEM, PL, FS, XPS, and PEC have confirmed that the lemon juice mediated and green g-C₃N₄ (L-CN) have good performances and remarkable visible light photocatalytic activities as compared to the chemically synthesized g-C₃N₄ (CN). Furthermore, the small surface area and low charge separation of g-C₃N₄ is upgraded by coupling with ZnO nanoparticles. It is proved that the coupling of ZnO worked as a facilitator and photoelectron modulator to enhance the charge separation of g-C₃N₄. Compared to pristine lemon-mediated green g-C₃N₄ (L-CN), the most active sample 5ZnO/L-CN showed ~ 5-fold improvement in activities for ciprofloxacin (CIP) and methylene blue (MB) degradation. More specifically, the mineralization process and degradation pathways, and the mineralization process of ciprofloxacin (CIP) and methylene blue (MB) are suggested. Finally, our present novel research work will provide new access to synthesize the eco-friendly and bio-caped green g-C₃N₄ nanomaterials and their employment for pollutants degradation and environmental purification.

Key words: Bio-caped green g-C₃N₄, Lemon juice mediators, ZnO/g-C₃N₄ nanocomposite, Environmental remediation, Degradation pathways

摘要： In this research study, we have synthesized the bio-capped ZnO/g-C₃N₄ nanocomposites by employing lemon juice (Citrus limon) as a stabilizer and mediator. Fruitfully, lemon juice which contains various acidic functional groups and citric acid has the capability to block the surface of g-C₃N₄ from chemical reactivity and activated the surface of g-C₃N₄ for various reactions. Consequently, the agglomeration behavior and controlled shape of g-C₃N₄ has also been achieved. Our experimental results i.e. XRD, TEM, HRTEM, PL, FS, XPS, and PEC have confirmed that the lemon juice mediated and green g-C₃N₄ (L-CN) have good performances and remarkable visible light photocatalytic activities as compared to the chemically synthesized g-C₃N₄ (CN). Furthermore, the small surface area and low charge separation of g-C₃N₄ is upgraded by coupling with ZnO nanoparticles. It is proved that the coupling of ZnO worked as a facilitator and photoelectron modulator to enhance the charge separation of g-C₃N₄. Compared to pristine lemon-mediated green g-C₃N₄ (L-CN), the most active sample 5ZnO/L-CN showed ~ 5-fold improvement in activities for ciprofloxacin (CIP) and methylene blue (MB) degradation. More specifically, the mineralization process and degradation pathways, and the mineralization process of ciprofloxacin (CIP) and methylene blue (MB) are suggested. Finally, our present novel research work will provide new access to synthesize the eco-friendly and bio-caped green g-C₃N₄ nanomaterials and their employment for pollutants degradation and environmental purification.

关键词: Bio-caped green g-C₃N₄, Lemon juice mediators, ZnO/g-C₃N₄ nanocomposite, Environmental remediation, Degradation pathways

Iltaf Khan, Chunjuan Wang, Shoaib Khan, Jinyin Chen, Aftab Khan, Sayyar Ali Shah, Aihua Yuan, Sohail Khan, Mehwish K. Butt, Humaira Asghar. Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation[J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 215-224.

References

[1] R.K. Ibrahim, M. Hayyan, M.A. AlSaadi, A. Hayyan, S. Ibrahim, Environmental application of nanotechnology: air, soil, and water, Environ. Sci. Pollut. Res. Int. 23 (14) (2016) 13754–13788.
[2] I. Khan, M. Luo, L. Guo, S. Khan, C. Wang, A. Khan, M. Saeed, S. Zaman, K. Qi, Q.l. Liu, Enhanced visible-light photoactivities of porous LaFeO₃ by synchronously doping Ni²⁺ and coupling TS-1 for CO₂ reduction and 2,4,6-trinitrophenol degradation, Catalysis Science & Technology, 11 (2021) 6793-6803.
[3] C.P. Xu, P.R. Anusuyadevi, C. Aymonier, R. Luque, S. Marre, Nanostructured materials for photocatalysis, Chem. Soc. Rev. 48 (14) (2019) 3868–3902.
[4] A. Zada, M. Khan, M.A. Khan, Q. Khan, A. Habibi-Yangjeh, A.L. Dang, M. Maqbool, Review on the hazardous applications and photodegradation mechanisms of chlorophenols over different photocatalysts, Environ. Res. 195 (2021) 110742.
[5] L. Jiang, X. Yuan, G. Zeng, Z. Wu, J. Liang, X. Chen, L. Leng, H. Wang, H. Wang, Metal-free efficient photocatalyst for stable visible-light photocatalytic degradation of refractory pollutant, Applied Catalysis B: Environmental, 221 (2018) 715-725.
[6] H.T. Fang, A.S. Oberoi, Z.Q. He, S.K. Khanal, H. Lu, Ciprofloxacin-degrading Paraclostridium sp. isolated from sulfate-reducing bacteria-enriched sludge: Optimization and mechanism, Water Res. 191 (2021) 116808.
[7] M. Adeel, M. Saeed, I. Khan, M. Muneer, N. Akram, Synthesis and characterization of co–ZnO and evaluation of its photocatalytic activity for photodegradation of methyl orange, ACS Omega 6 (2) (2021) 1426–1435.
[8] D. Sana, S. Jalila, A comparative study of adsorption and regeneration with different agricultural wastes as adsorbents for the removal of methylene blue from aqueous solution, Chin. J. Chem. Eng. 25 (9) (2017) 1282–1287.
[9] I. Khan, N. Sun, Y. Wang, Z.J. Li, Y. Qu, L.Q. Jing, Synthesis of SnO₂/yolk-shell LaFeO₃ nanocomposites as efficient visible-light photocatalysts for 2, 4-dichlorophenol degradation, Mater. Res. Bull. 127 (2020) 110857.
[10] E.S. Massima Mouele, J.O. Tijani, O.O. Fatoba, L.F. Petrik, Degradation of organic pollutants and microorganisms from wastewater using different dielectric barrier discharge configurations: a critical review, Environ. Sci. Pollut. Res. Int. 22 (23) (2015) 18345–18362.
[11] S. Zhang, P. Gu, R. Ma, C.Y. Luo, T. Wen, G. Zhao, W. Cheng, X. Wang, Recent developments in fabrication and structure regulation of visible-light-driven g-C₃N₄-based photocatalysts towards water purification: A critical review, Catalysis Today, (2019).
[12] S. Zhang, P.C. Gu, R. Ma, C.T. Luo, T. Wen, G.X. Zhao, W.C. Cheng, X.K. Wang, Recent developments in fabrication and structure regulation of visible-light-driven g-C₃N₄-based photocatalysts towards water purification: a critical review, Catal. Today 335 (2019) 65–77.
[13] I. Khan, N. Sun, Z.Q. Zhang, Z.J. Li, M. Humayun, S. Ali, Y. Qu, L.Q. Jing, Improved visible-light photoactivities of porous LaFeO₃ by coupling with nanosized alkaline earth metal oxides and mechanism insight, Catal. Sci. Technol. 9 (12) (2019) 3149–3157.
[14] X.Y. Chu, Y. Qu, A. Zada, L.L. Bai, Z.J. Li, F. Yang, L.N. Zhao, G.L. Zhang, X.J. Sun, Z.D. Yang, L.Q. Jing, Ultrathin phosphate-modulated co phthalocyanine/g-C 3 N 4 heterojunction photocatalysts with single co–N 4 (II) sites for efficient O 2 activation, Adv. Sci. 7 (16) (2020) 2001543.
[15] I. Khan, S. Khan, J.Y. Chen, S.A. Shah, A.H. Yuan, Biological inspired green synthesis of TiO₂ coupled g-C₃N₄ nanocomposites and its improved activities for sulfadiazine and bisphenol A degradation, J. Clust. Sci. (2022) 1–12.
[16] I. Khan, M. Luo, S. Khan, H. Asghar, M. Saeed, S. Khan, A. Khan, M. Humayun, L. Guo, B. Shi, Green synthesis of SrO bridged LaFeO₃/g-C₃N₄ nanocomposites for CO₂ conversion and bisphenol A degradation with new insights into mechanism, Environmental Research, 207 (2022) 112650.
[17] K. Zhao, I. Khan, K.Z. Qi, Y. Liu, A. Khataee, Ionic liquid assisted preparation of phosphorus-doped g-C₃N₄ photocatalyst for decomposition of emerging water pollutants, Mater. Chem. Phys. 253 (2020) 123322.
[18] M. Humayun, H. Ullah, L. Shu, X. Ao, A.A. Tahir, C. Wang, W. Luo, Plasmon assisted highly efficient visible light catalytic CO₂ reduction over the noble metal decorated Sr-incorporated g-C₃N₄, Nano Micro Lett. 13 (1) (2021) 1–18.
[19] J. Singh, T. Dutta, K.H. Kim, M. Rawat, P. Samddar, P. Kumar, ‘Green’ synthesis of metals and their oxide nanoparticles: applications for environmental remediation, J. Nanobiotechnology 16 (2018) 84.
[20] H.H. Duan, D.S. Wang, Y.D. Li, Green chemistry for nanoparticle synthesis, Chem. Soc. Rev. 44 (16) (2015) 5778–5792.
[21] S. Singh, I.C. Maurya, A. Tiwari, P. Srivastava, L. Bahadur, Green synthesis of TiO₂ nanoparticles using Citrus limon juice extract as a bio-capping agent for enhanced performance of dye-sensitized solar cells, Surfaces and Interfaces, 28 (2022) 101652.
[22] N. Ain Samat, R. Md Nor, Sol-gel synthesis of zinc oxide nanoparticles using Citrus aurantifolia extracts, Ceram. Int. 39 (2013) S545–S548.
[23] K.Z. Qi, W.X. Lv, I. Khan, S.Y. Liu, Photocatalytic H₂ generation via CoP quantum-dot-modified g-C₃N₄ synthesized by electroless plating, Chin. J. Catal. 41 (1) (2020) 114–121.
[24] S.Y. Zhang, I. Khan, X.H. Qin, K.Z. Qi, Y. Liu, S.C. Bai, Construction of 1D Ag-AgBr/AlOOH plasmonic photocatalyst for degradation of tetracycline hydrochloride, Front. Chem. 8 (2020) 117.
[25] M. Saeed, M. Usman, M. Ibrahim, A.U. Haq, I. Khan, H. Ijaz, F. Akram, Enhanced photo catalytic degradation of methyl orange using p–n Co₃O₄-TiO₂ hetero-junction as catalyst, Int. J. Chem. React. Eng. 18 (5–6) (2020).
[26] M. Humayun, A. Zada, Z.J. Li, M.Z. Xie, X.L. Zhang, Y. Qu, F. Raziq, L.Q. Jing, Enhanced visible-light activities of porous BiFeO₃ by coupling with nanocrystalline TiO₂ and mechanism, Appl. Catal. B Environ. 180 (2016) 219–226.
[27] M. Saeed, I. Khan, M. Adeel, N. Akram, M. Muneer, Synthesis of a CoO–ZnO photocatalyst for enhanced visible-light assisted photodegradation of methylene blue, New J. Chem. 46 (5) (2022) 2224–2231.
[28] I. Khan, M.S. Luo, L. Guo, S. Khan, S.A. Shah, I. Khan, A. Khan, C.J. Wang, B.H. Ai, S. Zaman, Synthesis of phosphate-bridged g-C₃N₄/LaFeO₃ nanosheets Z-scheme nanocomposites as efficient visible photocatalysts for CO₂ reduction and malachite green degradation, Appl. Catal. A Gen. 629 (2022) 118418.
[29] N. Sun, Y. Qu, C.H. Yang, Z.D. Yang, R. Yan, W. E, Z.Q. Zhang, Z.J. Li, H.N. Li, I. Khan, R. Sun, L.Q. Jing, H.G. Fu, Efficiently photocatalytic degradation of monochlorophenol on in situ fabricated BiPO₄/β-Bi₂O₃ heterojunction microspheres and O₂-free hole-induced selective dechloridation conversion with H₂ evolution, Appl. Catal. B Environ. 263 (2020) 118313.
[30] H. Kumar, K. Bhardwaj, D.S. Dhanjal, E. Nepovimova, F. Ṣen, H. Regassa, R. Singh, R. Verma, V. Kumar, D. Kumar, S.K. Bhatia, K. Kuča, Fruit extract mediated green synthesis of metallic nanoparticles: a new avenue in pomology applications, Int. J. Mol. Sci. 21 (22) (2020) 8458.
[31] Y. Humaira, Z. Amir, S.X. Liu, Surface plasmon resonance electron channeled through amorphous aluminum oxide bridged ZnO coupled g-C₃N₄ significantly promotes charge separation for pollutants degradation under visible light, J. Photochem. Photobiol. A Chem. 400 (2020) 112681.
[32] W. Yaseen, M. Xie, B.A. Yusuf, Y.G. Xu, M. Rafiq, N. Ullah, P.Y. Zhou, X. Li, J.M. Xie, Hierarchical Co/MoO₂@N-doped carbon nanosheets derived from waste lotus leaves for electrocatalytic water splitting, Int. J. Hydrog. Energy 47 (35) (2022) 15673–15686.
[33] A. Nisar, M. Saeed, M. Muneer, M. Usman, I. Khan, Synthesis and characterization of ZnO decorated reduced graphene oxide (ZnO-rGO) and evaluation of its photocatalytic activity toward photodegradation of methylene blue, Environ. Sci. Pollut. Res. 29 (1) (2022) 418–430.
[34] A. Nisar, M. Saeed, M. Usman, M. Muneer, M. Adeel, I. Khan, J. Akhtar, Kinetic modeling of ZnO-rGO catalyzed degradation of methylene blue, Int. J. Chem. Kinet. 52 (10) (2020) 645–654.
[35] R. Mohammadi, H. Alamgholiloo, B. Gholipour, S. Rostamnia, S. Khaksar, M. Farajzadeh, M. Shokouhimehr, Visible-light-driven photocatalytic activity of ZnO/g-C₃N₄ heterojunction for the green synthesis of biologically interest small molecules of thiazolidinones, J. Photochem. Photobiol. A Chem. 402 (2020) 112786.
[36] X. Li, H.P. Jiang, C.C. Ma, Z. Zhu, X.H. Song, H.Q. Wang, P.W. Huo, X.Y. Li, Local surface plasma resonance effect enhanced Z-scheme ZnO/Au/g-C₃N₄ film photocatalyst for reduction of CO₂ to CO, Appl. Catal. B Environ. 283 (2021) 119638.
[37] D.R. Paul, S. Gautam, P. Panchal, S.P. Nehra, P. Choudhary, A. Sharma, ZnO-modified g-C₃N₄: a potential photocatalyst for environmental application, ACS Omega 5 (8) (2020) 3828–3838.
[38] K.Z. Qi, A. Zada, Y. Yang, Q.Y. Chen, A. Khataee, Design of 2D–2D NiO/g-C₃N₄ heterojunction photocatalysts for degradation of an emerging pollutant, Res. Chem. Intermed. 46 (12) (2020) 5281–5295.
[39] M. Humayun, Q.Y. Fu, Z.P. Zheng, H.L. Li, W. Luo, Improved visible-light catalytic activities of novel Au/P-doped g-C₃N₄ photocatalyst for solar fuel production and mechanism, Appl. Catal. A Gen. 568 (2018) 139–147.
[40] S.A. Shah, I. Khan, A.H. Yuan, MoS 2 as a co-catalyst for photocatalytic hydrogen production: a mini review, Molecules 27 (10) (2022) 3289.
[41] N. D, M. Humayun, D. Bhattacharyya, D.J. Fu, Hierarchical Sr-ZnO/g-C₃N₄ heterojunction with enhanced photocatalytic activities, J. Photochem. Photobiol. A Chem. 396 (2020) 112515.
[42] Z. Mirzaeifard, Z. Shariatinia, M. Jourshabani, S.M. Rezaei Darvishi, ZnO Photocatalyst revisited: effective photocatalytic degradation of emerging contaminants using S-Doped ZnO nanoparticles under visible light radiation, Industrial & Engineering Chemistry Research, 59 (2020) 15894-15911.
[43] A. Naseri, M. Samadi, A. Pourjavadi, S. Ramakrishna, A.Z. Moshfegh, Enhanced photocatalytic activity of ZnO/g-C₃N₄ nanofibers constituting carbonaceous species under simulated sunlight for organic dye removal, Ceram. Int. 47 (18) (2021) 26185–26196.
[44] M. Gayathri, M. Sakar, E. Satheeshkumar, E. Sundaravadivel, Insights into the mechanism of ZnO/g–C₃N₄ nanocomposites toward photocatalytic degradation of multiple organic dyes, Journal of Materials Science: Materials in Electronics, 33 (2022) 9347-9357.
[45] X.Q. Yan, H. An, Z.H. Chen, G.D. Yang, Significantly enhanced charge transfer efficiency and surface reaction on NiP₂/g-C₃N₄ heterojunction for photocatalytic hydrogen evolution, Chin. J. Chem. Eng. 43 (2022) 31–39.
[46] F. Guo, Z.H. Chen, X.L. Huang, L.W. Cao, X.F. Cheng, W.L. Shi, L.Z. Chen, Ternary Ni₂P/Bi₂MoO₆/g-C₃N₄ composite with Z-scheme electron transfer path for enhanced removal broad-spectrum antibiotics by the synergistic effect of adsorption and photocatalysis, Chin. J. Chem. Eng. 44 (2022) 157–168.
[47] S.Y. Chen, Z.Y. Mu, R. Yan, X.L. Zhang, I. Khan, Z.J. Li, N. Sun, Q.Y. Zhang, L.Q. Jing, Improved photoactivities for CO₂ conversion and phenol degradation of α-Fe₂O₃ nanoparticles by co-coupling nano-sized BiPO₄ and CuO to modulate electrons, J. Alloys Compd. 800 (2019) 231–239.
[48] Z. Lu, Y. Ling, X. Wang, S. Li, X. Ao, W. Wang, C. Li, W. Sun, T. Huang, Insight into the degradation of ciprofloxacin by medium-pressure UV-activated monochloramine process, Science of The Total Environment, 832 (2022) 154850.
[49] A. Houas, H. Lachheb, M. Ksibi, E. Elaloui, C. Guillard, J.-M. Herrmann, Photocatalytic degradation pathway of methylene blue in water, Applied Catalysis B: Environmental, 31 (2001) 145-157.
[50] M.A. Qamar, S. Shahid, M. Javed, S. Iqbal, M. Sher, M.B. Akbar, Highly efficient g-C₃N₄/Cr-ZnO nanocomposites with superior photocatalytic and antibacterial activity, Journal of Photochemistry and Photobiology A: Chemistry, 401 (2020) 112776.

Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation

Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 0

Recommended Articles

Metrics

Comments