Abstract
Due to its hydrophilicity, the antibiotic tylosin (TYL) was challenging to remove entirely from water through traditional techniques. The design of an efficient photocatalyst for the degradation of TYL is a matter of great urgency. Herein, carboxylated cellulose beads embedded with Au-doped TiO2 nanoparticles (Au/TiO2-CCBs) were fabricated via interfacial solid-phase chemical modification with straightforward photo-deposition and TEMPO-mediated oxidation. Morphology, structure, and optical properties of Au/TiO2-CCBs have been investigated through scanning electron microscopy, energy dispersive spectrometer, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–vis Diffused reflectance spectra, and electron spin resonance (ESR). The fabricated Au/TiO2-CCBs exhibited superior photocatalytic performance, by demonstrating approx. 92% of TYL was decomposed in 180 min under visible light irradiation. However, the catalyst exhibited modest adsorption behavior. The enhanced photocatalytic activity for Au/TiO2-CCBs was attributed to the separation of photoinduced electron−hole pairs. The radical capture test and ESR experiment confirmed that ∙O2−, ∙OH, and h+ radicals were formed during the TYL degradation process. In addition, the stability of the Au/TiO2-CCBs was demonstrated by a steady photocatalytic performance after five cycles during the application. Therefore, this work indicated that the Au/TiO2-CCBs catalyst had an excellent prospect for environmental remediation.
Graphical abstract
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Atta A, Abdelhamied MM, Abdelreheem AM, Berber MR (2021) Flexible methyl cellulose/polyaniline/silver composite films with enhanced linear and nonlinear optical properties. Polymers (basel) 13:1225. https://doi.org/10.3390/polym13081225
Bhatia V, Ray AK, Dhir A (2016) Enhanced photocatalytic degradation of ofloxacin by co-doped titanium dioxide under solar irradiation. Sep Purif Technol 161:1–7. https://doi.org/10.1016/j.seppur.2016.01.028
Burda C, Chen X, Narayanan R, El-Sayed MA (2005) Chemistry and properties of nanocrystals of different shapes. Chem Rev 105:1025–1102. https://doi.org/10.1021/cr030063a
Chakraborty K, Pal T, Ghosh S (2018) RGO-ZnTe: a graphene based composite for tetracycline degradation and their synergistic effect. ACS Appl Nano Mater 1:3137–3144. https://doi.org/10.1021/acsanm.8b00295
Do TCMV, Nguyen DQ, Nguyen KT, Le PH (2019) TiO2 and Au-TiO2 nanomaterials for rapid photocatalytic degradation of antibiotic residues in aquaculture wastewater. Materials 12:2434. https://doi.org/10.3390/ma12152434
Domingues RP, Rodrigues MS, Proença M, Costa D, Alves E, Barradas NP, Oliveira FJ, Silva RF, Borges J, Vaz F (2018) Thin films composed of Au nanoparticles embedded in AlN: influence of metal concentration and thermal annealing on the LSPR band. Vacuum 157:414–421. https://doi.org/10.1016/j.vacuum.2018.09.013
French AD (2014) Idealized powder diffraction patterns for cellulose polymorphs. Cellulose 21:885–896. https://doi.org/10.1007/s10570-013-0030-4
French AD (2017) Glucose, not cellobiose, is the repeating unit of cellulose and why that is important. Cellulose 24:4605–4609. https://doi.org/10.1007/s10570-017-1450-3
Gan L, Geng A, Xu L, Chen M, Wang L, Liu J, Han S, Mei C, Zhong Q (2018) The fabrication of bio-renewable and recyclable cellulose based carbon microspheres incorporated by CoFe2O4 and the photocatalytic properties. J Clean Prod 196:594–603. https://doi.org/10.1016/j.jclepro.2018.06.086
Gao Y, Fan X-b, Zhang W-f, Zhao Q-s, Zhang G-l, Zhang F-b, Li Y (2014a) Enhanced photocatalytic degradation of methyl orange by Au/TiO2 nanotubes. Mater Lett 130:1–4. https://doi.org/10.1016/j.matlet.2014.05.076
Gao Y, Hu Y, Li C, Zhao X, Huang X, Liu R (2014b) Kiwifruit as reducing reagent for green synthesis of gold nanoparticles at room temperature. Nanosci Nanotechnol Lett 6:118–123. https://doi.org/10.1166/nnl.2014.1733
Gao Y, Nie W, Zhu Q, Wang X, Wang S, Fan F, Li C (2020) The polarization effect in surface-plasmon-induced photocatalysis on Au/TiO2 nanoparticles. Angew Chem Int Ed 59:18218–18223. https://doi.org/10.1002/anie.202007706
Ghasemi S, Hashemian SJ, Alamolhoda AA, Gocheva I, Rahman Setayesh S (2017) Plasmon enhanced photocatalytic activity of Au@TiO 2 -graphene nanocomposite under visible light for degradation of pollutants. Mater Res Bull 87:40–47. https://doi.org/10.1016/j.materresbull.2016.11.020
Guo X, Dong H, Xia T, Wang T, Jia H, Zhu L (2018) Highly efficient degradation toward tylosin in the aqueous solution by carbon spheres/g-C3N4 composites under simulated sunlight irradiation. ACS Sustain Chem Eng 6:12776–12786. https://doi.org/10.1021/acssuschemeng.8b01967
Heiner AP, Teleman O (1997) Interface between monoclinic crystalline cellulose and water: breakdown of the odd/even duplicity. Langmuir 13:511–518. https://doi.org/10.1021/la960886d
Hieu VQ, Phung TK, Nguyen TQ, Khan A, Doan VD, Tran VA, Le VT (2021) Photocatalytic degradation of methyl orange dye by Ti3C2-TiO2 heterojunction under solar light. Chemosphere 276:130154. https://doi.org/10.1016/j.chemosphere.2021.130154
Hu D, Henderson KLD, Coats JR (2010) Environmental fate and chemistry of a veterinary antibiotic—tylosin. Veterinar Pharmaceuticals Environ 45:93–104. https://doi.org/10.1021/bk-2009-1018.ch007
Hussain H, Tocci G, Woolcot T, Torrelles X, Pang CL, Humphrey DS, Yim CM, Grinter DC, Cabailh G, Bikondoa O et al (2017) Structure of a model TiO2 photocatalytic interface. Nat Mater 16:461–466. https://doi.org/10.1038/nmat4793
Jahdi M, Mishra SB, Nxumalo EN, Mhlanga SD, Mishra AK (2020) Smart pathways for the photocatalytic degradation of sulfamethoxazole drug using F-Pd co-doped TiO2 nanocomposites. Appl Catal B 267:118716. https://doi.org/10.1016/j.apcatb.2020.118716
Jimenez-Salcedo M, Monge M, Tena MT (2022) An organometallic approach for the preparation of Au-TiO2 and Au-g-C3N4 nanohybrids: improving the depletion of paracetamol under visible light. Photochem Photobiol Sci 21:337–347. https://doi.org/10.1007/s43630-022-00172-9
Katal R, Masudy-Panah S, Tanhaei M, Farahani MHDA, Jiangyong H (2020) A review on the synthesis of the various types of anatase TiO2 facets and their applications for photocatalysis. Chem Eng J 384:123384. https://doi.org/10.1016/j.cej.2019.123384
Li B, Lai C, Zeng G, Qin L, Yi H, Huang D, Zhou C, Liu X, Cheng M, Xu P et al (2018a) Facile hydrothermal synthesis of Z-Scheme Bi2Fe4O9/Bi2WO6 heterojunction photocatalyst with enhanced visible light photocatalytic activity. ACS Appl Mater Interfaces 10:18824–18836. https://doi.org/10.1021/acsami.8b06128
Li G, Wang B, Zhang J, Wang R, Liu H (2020a) Er-doped g-C3N4 for photodegradation of tetracycline and tylosin: high photocatalytic activity and low leaching toxicity. Chem Eng J 391:123500. https://doi.org/10.1016/j.cej.2019.123500
Li G, Wang R, Wang B, Zhang J (2020b) Sm-doped mesoporous g-C3N4 as efficient catalyst for degradation of tylosin: influencing factors and toxicity assessment. Appl Surf Sci 517:146212. https://doi.org/10.1016/j.apsusc.2020.146212
Li J, Cheng R, Xiu H, Zhang M, Liu Q, Song T, Dong H, Yao B, Zhang X, Kozliak E et al (2018b) Pore structure and pertinent physical properties of nanofibrillated cellulose (NFC)-based foam materials. Carbohydr Polym 201:141–150. https://doi.org/10.1016/j.carbpol.2018.08.008
Liu S, Cheng G, Xiong Y, Ding Y, Luo X (2020) Adsorption of low concentrations of bromide ions from water by cellulose-based beads modified with TEMPO-mediated oxidation and Fe(III) complexation. J Hazard Mater 384:121195. https://doi.org/10.1016/j.jhazmat.2019.121195
Liu Y, Liu Y, Tao P, Shang W, Song C, Deng T (2014) Vertical segregation in the self-assembly of nanoparticles at the liquid/air interface. Nanoscale 6:14662–14666. https://doi.org/10.1039/c4nr04779f
Luo B, Xu D, Li D, Wu G, Wu M, Shi W, Chen M (2015) Fabrication of a Ag/Bi3TaO7 plasmonic photocatalyst with enhanced photocatalytic activity for degradation of tetracycline. ACS Appl Mater Interfaces 7:17061–17069. https://doi.org/10.1021/acsami.5b03535
Luo X, Liu L, Wang L, Liu X, Cai Y (2019) Facile synthesis and low concentration tylosin adsorption performance of chitosan/cellulose nanocomposite microspheres. Carbohydr Polym 206:633–640. https://doi.org/10.1016/j.carbpol.2018.11.009
Ma J, Guo X, Zhang Y, Ge H (2014) Catalytic performance of TiO2@Ag composites prepared by modified photodeposition method. Chem Eng J 258:247–253. https://doi.org/10.1016/j.cej.2014.06.120
Makula P, Pacia M, Macyk W (2018) How to correctly determine the band gap energy of modified semiconductor photocatalysts based on UV-Vis spectra. J Phys Chem Lett 9:6814–6817. https://doi.org/10.1021/acs.jpclett.8b02892
Orooji Y, Tanhaei B, Ayati A, Tabrizi SH, Alizadeh M, Bamoharram FF, Karimi F, Salmanpour S, Rouhi J, Afshar S et al (2021) Heterogeneous UV-Switchable Au nanoparticles decorated tungstophosphoric acid/TiO2 for efficient photocatalytic degradation process. Chemosphere 281:130795. https://doi.org/10.1016/j.chemosphere.2021.130795
Panayotov DA, Frenkel AI, Morris JR (2017) Catalysis and photocatalysis by nanoscale Au/TiO2: perspectives for renewable energy. ACS Energy Lett 2:1223–1231. https://doi.org/10.1021/acsenergylett.7b00189
Phutanon N, Motina K, Chang YH, Ummartyotin S (2019) Development of CuO particles onto bacterial cellulose sheets by forced hydrolysis: a synergistic approach for generating sheets with photocatalytic and antibiofouling properties. Int J Biol Macromol 136:1142–1152. https://doi.org/10.1016/j.ijbiomac.2019.06.168
Saito T, Isogai A (2004) TEMPO-mediated oxidation of native cellulose. the effect of oxidation conditions on chemical and crystal structures of the water-insoluble fractions. Biomacromol 5:1983–1989. https://doi.org/10.1021/bm0497769
Schneider J, Matsuoka M, Takeuchi M, Zhang J, Horiuchi Y, Anpo M, Bahnemann DW (2014) Understanding TiO2 photocatalysis: mechanisms and materials. Chem Rev 114:9919–9986. https://doi.org/10.1021/cr5001892
Serna P, Corma A (2015) Transforming nano metal nonselective particulates into chemoselective catalysts for hydrogenation of substituted nitrobenzenes. ACS Catal 5:7114–7121. https://doi.org/10.1021/acscatal.5b01846
Shan AY, Ghazi TIM, Rashid SA (2010) Immobilisation of titanium dioxide onto supporting materials in heterogeneous photocatalysis: a review. Appl Catal A 389:1–8. https://doi.org/10.1016/j.apcata.2010.08.053
Shan X, Guo X, Yin Y, Miao Y, Dong H (2017) Surface modification of graphene oxide by goethite with enhanced tylosin photocatalytic activity under visible light irradiation. Colloids Surf, A 520:420–427. https://doi.org/10.1016/j.colsurfa.2017.01.077
Shi J, Chen J, Li G, An T, Yamashita H (2017) Fabrication of Au/TiO 2 nanowires@carbon fiber paper ternary composite for visible-light photocatalytic degradation of gaseous styrene. Catal Today 281:621–629. https://doi.org/10.1016/j.cattod.2016.06.026
Sun H, Wu H, Jin Y, Lv Y, Ju G, Chen L, Feng Z, Hu Y (2019) Photocatalytic titanium dioxide immobilized on an ultraviolet emitting ceramic substrate for water purification. Mater Lett 240:100–102. https://doi.org/10.1016/j.matlet.2018.12.135
Sun Z, Liu C, Li X-S, Fang Y, Zhu X, Zhu A-M (2022) Semi-transparent nanofilms of plasmonic Au/TiO2 for visible-light photocatalysis. Mater Chem Phys 280:125773. https://doi.org/10.1016/j.matchemphys.2022.125773
Tanaka A, Hashimoto K, Kominami H (2012) Preparation of Au/CeO2 exhibiting strong surface plasmon resonance effective for selective or chemoselective oxidation of alcohols to aldehydes or ketones in aqueous suspensions under irradiation by green light. J Am Chem Soc 134:14526–14533. https://doi.org/10.1021/ja305225s
Tang Y, Li N, Liu A, Ding S, Yi C, Liu H (2012) Effect of spinning conditions on the structure and performance of hydrophobic PVDF hollow fiber membranes for membrane distillation. Desalination 287:326–339. https://doi.org/10.1016/j.desal.2011.11.045
Veziroglu S, Obermann AL, Ullrich M, Hussain M, Kamp M, Kienle L, Leissner T, Rubahn HG, Polonskyi O, Strunskus T et al (2020) Photodeposition of Au nanoclusters for enhanced photocatalytic dye degradation over TiO2 thin film. ACS Appl Mater Interfaces 12:14983–14992. https://doi.org/10.1021/acsami.9b18817
Wu S, Li X, Tian Y, Lin Y, Hu YH (2021) Excellent photocatalytic degradation of tetracycline over black anatase-TiO2 under visible light. Chem Eng J. https://doi.org/10.1016/j.cej.2020.126747
Yan J, Li X, Jin B, Zeng M, Peng R (2020) Synthesis of TiO2/Pd and TiO2/PdO hollow spheres and their visible light photocatalytic activity. Int J Photoenergy 2020:1–9. https://doi.org/10.1155/2020/4539472
Yang J, Luo X (2021) Ag-doped TiO2 immobilized cellulose-derived carbon beads: one-pot preparation, photocatalytic degradation performance and mechanism of ceftriaxone sodium. Appl Surf Sci. https://doi.org/10.1016/j.apsusc.2020.148724
Yang Z, Xia X, Shao L, Wang L, Liu L (2021) Efficient photocatalytic degradation of tetracycline under visible light by Z-scheme Ag3PO4/mixed-valence MIL-88A(Fe) heterojunctions: mechanism insight, degradation pathways and DFT calculation. Chem Eng J. https://doi.org/10.1016/j.cej.2021.128454
Yu Y, Liu S, Pei Y, Luo X (2021) Growing Pd NPs on cellulose microspheres via in-situ reduction for catalytic decolorization of methylene blue. Int J Biol Macromol 166:1419–1428. https://doi.org/10.1016/j.ijbiomac.2020.11.021
Zhang G, Huang G, Yang C, Chen S, Xu Y, Zhang S, Lu P, Sun J, Zhu Y, Yang D (2021) Efficient photoelectrocatalytic degradation of tylosin on TiO2 nanotube arrays with tunable phosphorus dopants. J Environ Chem Eng. https://doi.org/10.1016/j.jece.2020.104742
Zhang N, Zang GL, Shi C, Yu HQ, Sheng GP (2016) A novel adsorbent TEMPO-mediated oxidized cellulose nanofibrils modified with PEI: preparation, characterization, and application for Cu(II) removal. J Hazard Mater 316:11–18. https://doi.org/10.1016/j.jhazmat.2016.05.018
Zhang R, Zeng K (2021) A novel flower-like dual Z-scheme BiSI/Bi2WO6/g-C3N4 photocatalyst has excellent photocatalytic activity for the degradation of organic pollutants under visible light. Diam Relat Mater. https://doi.org/10.1016/j.diamond.2021.108343
Acknowledgements
This work was supported by the National Natural Science Foundation of China (51773159), Special Projects of the Central Government in Guidance of Local Science and Technology Development in Hubei Province (2020ZYYD040), the second batch of the Key Research and Development Project of Hubei Province (2020BAB073), Outstanding Young and Middle-aged Scientific Innovation Team of Colleges and Universities of Hubei Province: "Biomass chemical technologies and materials" (Grant No. T201908), the Innovation Project of Key Laboratory of Novel Biomass-based Environmental and Energy Materials in Petroleum and Chemical Industry (22BEEA01) and the Open Funding of Hubei Three Gorges Laboratory (SC211005).
Author information
Authors and Affiliations
Contributions
PZ: Conceptualization, Methodology, Data curation, Writing- Original Draft preparation. YY: Visualization, Investigation, Writing—Review & Editing. YP: Writing—Review & Editing, Resources, Supervision. XL: Writing—Review & Editing, Resources, Supervision, Project administration, Funding acquisition.
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Zhao, P., Yang, Y., Pei, Y. et al. TEMPO-oxidized cellulose beads embedded with Au-doped TiO2 nanoparticles for photocatalytic degradation of Tylosin. Cellulose 30, 1133–1147 (2023). https://doi.org/10.1007/s10570-022-04935-6
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-022-04935-6