Synergistic photoelectrocatalytic degradation of tetracycline using a novel Z-scheme Zn_0.5Ni_0.5Fe₂O₄/SiNWs heterostructure: Towards sustainable antibiotic remediation

Abstract

Photoelectrocatalytic technology (PEC) is an emerging green and sustainable technology for treating antibiotic wastewater. However, its effectiveness is limited by the recombination of photogenerated carriers. To address this issue, the Fenton reaction, an advanced oxidation process, can be coupled with PEC technology to enhance the oxidative degradation of antibiotic wastewater. This research involved creating a Zn_0.5Ni_0.5Fe₂O₄/silicon nanowires (SiNWs) Z-type heterojunction through the spin coating technique, which was then utilized in the PEC coupled Fenton reaction to break down antibiotic wastewater. The inherent electric field and the voltage applied hastened the segregation of e⁻ and h⁺ within the system. These advantages make the Zn_0.5Ni_0.5Fe₂O₄/SiNWs heterojunction highly efficient in removing various antibiotics, including tetracycline (TC), ciprofloxacin (CIP), amoxicillin (AMX), and levofloxacin (LVX). In particular, the Zn_0.5Ni_0.5Fe₂O₄/SiNWs heterojunction demonstrated an 82.21% degradation efficiency for TC, exhibiting a kinetic constant (k) of 0.02688 min⁻¹, a rate 2.82 times (4.80 times) greater than that of SiNWs. Experimental findings reveal that Zn_0.5Ni_0.5Fe₂O₄/SiNWs exhibit superior light absorption properties and a reduced rate of photogenerated charge recombination. The doping of Zn_0.5Ni_0.5Fe₂O₄ effectively improves the catalytic performance of SiNWs. This research offers fresh insights into researching PEC-coupled Fenton reaction methods for the degradation of antibiotics and paves the way for advancing the creation of more potent photoelectrochemical catalysts in the future.

Keywords

antibiotics / Fenton / heterojunction / photoelectrocatalysis / silicon nanowires (SiNWs) / Zn _0.5Ni _0.5Fe ₂O ₄

References

[1] Arikan OA, Rice C, Codling E. Occurrence of antibiotics and hormones in a major agricultural watershed. Desalination. 2008;226(1-3):121-133.

[2] Aust MO, Godlinski F, Travis GR, et al. Distribution of sulfamethazine, chlortetracycline and tylosin in manure and soil of Canadian feedlots after subtherapeutic use in cattle. Environ Pollut. 2008;156(3):1243-1251.

[3] Qiao M, Ying GG, Singer AC, Zhu YG. Review of antibiotic resistance in China and its environment. Environ Int. 2018;110:160-172.

[4] Davis MDM, Lohm D, Flowers P, Whittaker A. Antibiotic assemblages and their implications for the prevention of antimicrobial resistance. Soc Sci Med. 2022;315:115550.

[5] Fuente-Nunez CDL, Cesaro A, Hancock REW. Antibiotic failure: beyond antimicrobial resistance. Drug Resist Updates. 2023;71:101012.

[6] Zhang QQ, Ying GG, Pan CG, Liu YS, Zhao JL. Comprehensive evaluation of antibiotics emission and fate in the river basins of China: source analysis, multimedia modeling, and linkage to bacterial resistance. Environ Sci Technol. 2015;49(11):6772-6782.

[7] Brillas E, Martínez-Huitle CA. Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods. An updated review. Appl Catal B Environ Energy. 2015;166-167:603-643.

[8] Garcia-Segura S, Brillas E. Applied photoelectrocatalysis on the degradation of organic pollutants in wastewaters. J Photoch Photobio C. 2017;31:1-35.

[9] Oturan MA, Aaron JJ. Advanced oxidation processes in water/wastewater treatment: principles and applications. A review. Crit Rev Environ Sci Technol. 2014;44(23):2577-2641.

[10] Fang YY, Liang QW, Li Y, Luo HJ. Surface oxygen vacancies and carbon dopant co-decorated magnetic ZnFe₂O₄ as photo-Fenton catalyst towards efficient degradation of tetracycline hydrochloride. Chemosphere. 2022;302:134832.

[11] Koutavarapu R, Reddy CV, Syed K, et al. Novel Z-scheme binary zinc tungsten oxide/nickel ferrite nanohybrids for photocatalytic reduction of chromium (Cr (VI)), photoelectrochemical water splitting and degradation of toxic organic pollutants. J Hazard Mater. 2022;423:127044.

[12] Zhang JZ, Yuan GQ, Wang HH, et al. Preparation of core/shell-structured ZnFe₂O₄@ZnIN₂S₄ catalysts and its ultrafast microwave catalytic reduction performance for aqueous Cr(VI). Chem Eng J. 2023;451:138182.

[13] Belakehal R, Atacan K, Güy N, Megriche A, Özacar M. Fabrication of heterostructured CdS/g-C₃N₄/ZnFe₂O₄ nanocomposite synthesized through ultrasonic-assisted method for efficient photocatalytic hydrogen production. Appl Surf Sci. 2022;602:154315.

[14] Domínguez-Arvizu JL, Jiménez-Miramontes JA, Hernández-Majalca BC, et al. Study of NiFe₂O₄/Cu₂O p-n heterojunctions for hydrogen production by photocatalytic water splitting with visible light. J Mater Res Technol. 2022;21:4184-4199.

[15] Jia Y, Han HR, Luo Y, Wang QZ, Wha Lee B, Liu CL. SrTiO₃ nanosheets decorated with ZnFe₂O₄ nanoparticles as Z-scheme photocatalysts for highly efficient photocatalytic degradation and CO₂ conversion. Sep Purif Technol. 2023;306:122667.

[16] Pang SX, Dong YL, Xu DY, et al. Strong interface interaction and internal electric field promote electron transfer of Bi₂O₂S/NiFe₂O₄ heterojunction for photocatalytic antibiotic degradation. J Mater Sci Technol. 2023;158:145-155.

[17] Qin HD, Cheng H, Shi W, et al. Heterogeneous degradation of cefotaxime sodium with peroxymonosulfate activated by an effective and magnetically separable Ni_0.5ZN_0.5Fe₂O₄ catalyst. J Environ Chem Eng. 2023;11(1):109070.

[18] Huang ZP, Wang CF, Pan L, Tian F, Zhang XX, Zhang C. Enhanced photoelectrochemical hydrogen production using silicon nanowires@MoS₃. Nano Energy. 2013;2(6):1337-1346.

[19] Ifires M, Hadjersi T, Chegroune R, et al. One-step electrodeposition of superhydrophobic NiO-Co(OH)₂ urchin-like structures on Si nanowires as photocatalyst for RhB degradation under visible light. J Alloys Compd. 2019;774:908-917.

[20] Wang B, Yao L, Xu GQ, et al. Highly efficient photoelectrochemical synthesis of ammonia using plasmon-enhanced black silicon under ambient conditions. ACS Appl Mater Interfaces. 2020;12(18):20376-20382.

[21] Lan JS, He B, Haw C, et al. Band engineering of ZnO/Si nanowire arrays in Z-scheme heterojunction for efficient dye photodegradation. Appl Surf Sci. 2020;529:147023.

[22] Yao L, He XM, Lv J, et al. Efficient degradation of ciprofloxacin by CO₃O₄/Si nanoarrays heterojunction activated peroxymonosulfate under simulated sunlight: performance and mechanism. J Environ Chem Eng. 2022;10(3):107397.

[23] Li XC, Shi CJ, Feng ZX, et al. Construction of Si nanowires/ZnFe₂O₄/Ag photocatalysts with enhanced photocatalytic activity under visible light and magnetic field. J Alloys Compd. 2023;946:169467.

[24] Naffeti M, Zaïbi MA, Nefzi C, García-Arias AV, Chtourou R, Postigo PA. Highly efficient photodegradation of methylene blue by a composite photocatalyst of bismuth nanoparticles on silicon nanowires. Environ Technol Innov. 2023;30:103133.

[25] Shen WQ, Dong Y, Wu JJ, et al. Visible light-driven photoelectrocatalytic degradation of tetracycline on NiFe₂O₄/SiNWs heterojunction. Appl Surf Sci. 2024;647:158880.

[26] Aali H, Azizi N, Baygi NJ, et al. High antibacterial and photocatalytic activity of solution combustion synthesized Ni_0.5ZN_0.5Fe₂O₄ nanoparticles: effect of fuel to oxidizer ratio and complex fuels. Ceram Int. 2019;45(15):19127-19140.

[27] Huang YC, Li KS, Li SQ, Lin Y, Liu H, Tong YX. Ultrathin Bi₂MoO₆ nanosheets for photocatalysis: performance enhancement by atomic interfacial engineering. ChemistrySelect. 2018;3(26):7423-7428.

[28] Kim JH, Jang YJ, Kim JH, Choi SH, Lee JS. Defective ZnFe₂O₄ nanorods with oxygen vacancy for photoelectrochemical water splitting. Nanoscale. 2015;7(45):19144-19151.

[29] Zhou YP, Jiao WY, Xie Y, et al. Enhanced photocatalytic CO₂-reduction activity to form CO and CH₄ on S-scheme heterostructured ZnFe₂O₄/Bi₂MoO₆ photocatalyst. J Colloid Interface Sci. 2022;608:2213-2223.

[30] Zhu HR, Zhang C, Xie KF, Li XG, Liao GF. Photocatalytic degradation of organic pollutants over MoS₂/Ag-ZnFe₂O₄ Z-scheme heterojunction: revealing the synergistic effects of exposed crystal facets, defect engineering, and Z-schem. mechanism. Chem Eng J. 2023;453:139775.

[31] Agboola PO, Shakir I, Haider S. Development of internal electric field induced NiFe₂O₄/CdO p-n nano-heterojunctions for solar light activated photodegradation of methylene blue dye. Ceram Int. 2022;48(10):13572-13579.

[32] Fan RL, Mao J, Yin ZH, et al. Efficient and stable silicon photocathodes coated with vertically standing nano-MoS₂ films for solar hydrogen production. ACS Appl Mater Interfaces. 2017;9(7):6123-6129.

[33] Zeng C, Hu YM, Zhang TR, Dong F, Huang H. Core-satellite structured Z-scheme catalyst Cd_0.5ZN_0.5S/BiVO₄ for highly efficiency and stable photocatalytic water splitting. J Mater Chem A. 2018;6(35):16932-16942.

[34] Wang KY, Liang GZ, Waqas M, et al. Peroxymonosulfate enhanced photoelectrocatalytic degradation of ofloxacin using an easily coated cathode. Sep Purif Technol. 2020;236:116301.

[35] Shi WL, Wang LJ, Wang J, et al. Magnetically retrievable CdS/reduced graphene oxide/ZnFe₂O₄ ternary nanocomposite for self-generated H₂O₂ towards photo-Fenton removal of tetracycline under visible light irradiation. Sep Purif Technol. 2022;292:120987.

[36] Zhang YH, Shi J, Xu ZW, Chen Y, Song DM. Degradation of tetracycline in a schorl/H₂O₂ system: proposed mechanism and intermediates. Chemosphere. 2018;202:661-668.

[37] Nawaz M, Shahzad A, Tahir K, et al. Photo-Fenton reaction for the degradation of sulfamethoxazole using a multi-walled carbon nanotube-NiFe₂O₄ composite. Chem Eng J. 2020;382:123053.

[38] Feng C, Zhang H, Liu Y, et al. Surface structure regulation of sulfidated zero-valent iron by H₂O₂ for efficient pH self-regulation and proton cycle to boost heterogeneous Fenton-like reaction for pollutant control. Appl Catal B Environ Energy. 2024;345:123667.

[39] Zu DY, Lai YY, Wang YY, et al. Cathodic polarization sustaining MXene-mediated fenton-like reactions: performance, reaction mechanisms, and life cycle assessment. Chem Eng J. 2024;487:150503.

[40] Cao JY, Xiong ZK, Lai B. Effect of initial pH on the tetracycline (TC) removal by zero-valent iron: adsorption, oxidation and reduction. Chem Eng J. 2018;343:4920499.

[41] Zhao GS, Ding J, Zhou FY, et al. Construction of a visible-light-driven magnetic dual Z-scheme BiVO₄/g-C₃N₄/NiFe₂O₄ photocatalyst for effective removal of ofloxacin: mechanisms and degradation pathway. Chem Eng J. 2021;405:126704.

[42] Sun JW, Wu T, Liu ZF, et al. Peroxymonosulfate activation induced by spinel ferrite nanoparticles and their nanocomposites for organic pollutants removal: a review. J Clean Prod. 2022;346:131143.

[43] Quan Y, Liu ML, Wu HL, et al. Rational design and construction of S-scheme CeO₂/AgCl heterojunction with enhanced photocatalytic performance for tetracycline degradation. Appl Surf Sci. 2024;642:158601.

[44] Liu QQ, Shen JY, Yang XF, Zhang T, Tang H. 3D reduced graphene oxide aerogel-mediated Z-scheme photocatalytic system for highly efficient solar-driven water oxidation and removal of antibiotics. Appl Catal B Environ Energy. 2018;232:562-573.

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2024 The Author(s). EcoEnergy published by John Wiley & Sons Australia, Ltd on behalf of China Chemical Safety Association.