Abstract
A simple and environment-friendly approach to prepare zinc oxide nanoaggregates was achieved by employing ethylene glycol–H2O as the reaction medium. The composition and structure of the as-fabricated ZnO products were confirmed using X-ray diffraction, scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and nitrogen adsorption measurements. By tailoring the volume ratio of ethylene glycol to water, coral-like, flower-like, and nanoparticulate ZnO nanoaggregates were successfully synthesized. The impact of the structure of the as-obtained ZnO nanoaggregates on the photocatalytic degradation of ciprofloxacin was further studied. Under simulated solar light irradiation, the photocatalytic removal rate of coral-like, flower-like, and nanoparticulate ZnO nanoaggregates for ciprofloxacin was 45%, 80%, and 90%, respectively. The reactive species trapping experiment result indicated that the generated holes, OH−, and ·O2− active species mainly contributed to the degradation of ciprofloxacin. On the basis of photoluminescence spectra and photo/electrochemical measurement results, the prevention of electron-hole recombination and the rapid charge transfer upon the ZnO nanoparticle aggregates resulted in their efficient photocatalytic activity.
Engineered zinc oxide nanoaggregates for photocatalytic removal of ciprofloxacin with structure dependence
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Ahmad S, Su X, Yang C, Wang X, Liu X, Wang J (2019) Space-confined growth of layered basic zinc acetate nanosheets and their orderly fragmented ZnO nanoparticles on clay platelets. J Hazard Mater 371(5):213–223. https://doi.org/10.1016/j.jhazmat.2019.02.111
Bai S, Jiang J, Zhang Q, Xiong Y (2015) Steering charge kinetics in photocatalysis: intersection of materials syntheses, characterization techniques and theoretical simulations. Chem Soc Rev 44(10):2893–2939. https://doi.org/10.1039/c5cs00064e
Bian Z, Zhu J, Wen J, Cao F, Huo Y, Qian X, Cao Y, Shen M, Li H, Lu Y (2011) Single-crystal-like titania mesocages. Angew Chem Int Ed 50(5):1105–1108. https://doi.org/10.1002/anie.201004972
Chen C, Ma W, Zhao J (2010) Semiconductor-mediated photodegradation of pollutants under visible-light irradiation. Chem Soc Rev 39(11):4206–4219
Chen K-H, Pu Y-C, Chang K-D, Liang Y-F, Liu C-M, Yeh J-W, Shih H-C, Hsu Y-J (2012) Ag-nanoparticle-decorated SiO2 nanospheres exhibiting remarkable plasmon-mediated photocatalytic properties. J Phys Chem C 116(35):19039–19045. https://doi.org/10.1021/jp306555j
Chen Y, Zhao H, Liu B, Yang H (2015) Charge separation between wurtzite ZnO polar {001} surfaces and their enhanced photocatalytic activity. Appl Catal B Environ 163:189–197. https://doi.org/10.1016/j.apcatb.2014.07.044
Chen C, Yu W, Liu T, Cao S, Tsang Y (2017) Graphene oxide/WS2/Mg-doped ZnO nanocomposites for solar-light catalytic and anti-bacterial applications. Sol Energy Mater Sol Cells 160:43–53. https://doi.org/10.1016/j.solmat.2016.10.020
Chen C, Liu X, Fang Q, Chen X, Liu T, Zhang M (2020) Self-assembly synthesis of CuO/ZnO hollow microspheres and their photocatalytic performance under natural sunlight. Vacuum 174:109198 https://doi.org/10.1016/j.vacuum.2020.109198
Cheng G, Yang H, Rong K, Lu Z, Yu X, Chen R (2010) Shape-controlled solvothermal synthesis of bismuth subcarbonate nanomaterials. J Solid State Chem 183(8):1878–1883. https://doi.org/10.1016/j.jssc.2010.06.004
Cheng G, Wei Y, Xiong J, Gan Y, Zhu J, Xu F (2017) Same titanium glycolate precursor but different products: successful synthesis of twinned anatase TiO2 nanocrystals with excellent solar photocatalytic hydrogen evolution capability. Inorg Chem Front 4(8):1319–1329. https://doi.org/10.1039/c7qi00278e
Ding Y, Xu J, Chen L, Yao J, Dai S, Wu J, Hayat T, Alsaedi A (2019) Pierced ZnO nanosheets via a template-free photopolymerization in microemulsion. J Alloys Compd 787:779–785. https://doi.org/10.1016/j.jallcom.2019.02.107
Dong H, Chen YC, Feldmann C (2015) Polyol synthesis of nanoparticles: status and options regarding metals, oxides, chalcogenides, and non-metal elements. Green Chem 17(8):4107–4132. https://doi.org/10.1039/c5gc00943j
Feldmann C, Jungk H-O (2001) Polyol-mediated preparation of nanoscale oxide particles. Angew Chem Int Ed 40(2):359–362. https://doi.org/10.1002/1521-3773(20010119)40:2<359::aid-anie359>3.0.co;2-b
Feng X, Wang P, Hou J, Qian J, Wang C, Ao Y (2018) Oxygen vacancies and phosphorus codoped black titania coated carbon nanotube composite photocatalyst with efficient photocatalytic performance for the degradation of acetaminophen under visible light irradiation. Chem Eng J 352:947–956. https://doi.org/10.1016/j.cej.2018.06.037
Fiévet F, Ammar-Merah S, Brayner R, Chau F, Giraud M, Mammeri F, Peron J, Piquemal JY, Sicard L, Viau G (2018) The polyol process: a unique method for easy access to metal nanoparticles with tailored sizes, shapes and compositions. Chem Soc Rev 47(14):5187–5233. https://doi.org/10.1039/c7cs00777a
Gan Y, Wei Y, Xiong J, Cheng G (2018) Impact of post-processing modes of precursor on adsorption and photocatalytic capability of mesoporous TiO2 nanocrystallite aggregates towards ciprofloxacin removal. Chem Eng J 349:1–16. https://doi.org/10.1016/j.cej.2018.05.051
Gao F, Lu Q, Meng X, Komarneni S (2008) CdS nanorod-based structures: from two- and three-dimensional leaves to flowers. J Phys Chem C 112(35):13359–13365. https://doi.org/10.1021/jp804533z
Gong J, Bao X (2017) Fundamental insights into interfacial catalysis. Chem Soc Rev 46(7):1770–1771. https://doi.org/10.1039/c7cs90022h
Gordon TR, Cargnello M, Paik T, Mangolini F, Weber RT, Fornasiero P, Murray CB (2012) Nonaqueous synthesis of TiO2 nanocrystals using TiF4 to engineer morphology, oxygen vacancy concentration, and photocatalytic activity. J Am Chem Soc 134(15):6751–6761. https://doi.org/10.1021/ja300823a
Guo F, Shi W, Wang H, Huang H, Liu Y, Kang Z (2017) Fabrication of a CuBi2O4/g-C3N4 p–n heterojunction with enhanced visible light photocatalytic efficiency toward tetracycline degradation. Inorganic Chemistry Frontiers 4(10):1714–1720. https://doi.org/10.1039/c7qi00402h
He Y, Zhang L, Teng B, Fan M (2015) New application of Z-scheme Ag3PO4/g-C3N4 composite in converting CO2 to fuel. Environ Sci Technol 49(1):649–656. https://doi.org/10.1021/es5046309
He J, Zhang Y, Guo Y, Rhodes G, Yeom J, Li H, Zhang W (2019) Photocatalytic degradation of cephalexin by ZnO nanowires under simulated sunlight: kinetics, influencing factors, and mechanisms. Environ Int 132:105105. https://doi.org/10.1016/j.envint.2019.105105
Huang Q, Tian S, Zeng D, Wang X, Song W, Li Y, Xiao W, Xie C (2013) Enhanced photocatalytic activity of chemically bonded TiO2/graphene composites based on the effective interfacial charge transfer through the C–Ti bond. ACS Catal 3(7):1477–1485. https://doi.org/10.1021/cs400080w
Komarneni S, Li D, Newalkar B, Katsuki H, Bhalla AS (2002) Microwave−polyol process for Pt and Ag nanoparticles. Langmuir 18(15):5959–5962. https://doi.org/10.1021/la025741n
Li W, Gao S, Li L, Jiao S, Li H, Wang J, Yu Q, Zhang Y, Wang D, Zhao L (2016a) Hydrothermal synthesis of a 3D double-sided comb-like ZnO nanostructure and its growth mechanism analysis. Chem Commun 52(53):8231–8234. https://doi.org/10.1039/c6cc02072k
Li X, Yu J, Jaroniec M (2016b) Hierarchical photocatalysts. Chem Soc Rev 45:2603–2636. https://doi.org/10.1039/c5cs00838g
Li Q, Guan Z, Wu D, Zhao X, Bao S, Tian B, Zhang J (2017) Z-scheme BiOCl-Au-CdS heterostructure with enhanced sunlight-driven photocatalytic activity in degrading water dyes and antibiotics. ACS Sustain Chem Eng 5(8):6958–6968. https://doi.org/10.1021/acssuschemeng.7b01157
Li M-y, Tang Y-b, Shi W-l, Chen F-y, Shi Y, Gu H-c (2018) Design of visible-light-response core–shell Fe2O3/CuBi2O4 heterojunctions with enhanced photocatalytic activity towards the degradation of tetracycline: Z-scheme photocatalytic mechanism insight. Inorg Chem Front 5(12):3148–3154. https://doi.org/10.1039/c8qi00906f
Liu X, Chen C (2020) Mxene enhanced the photocatalytic activity of ZnO nanorods under visible light. Mater Lett 261:127127 http://202.114.202.219:80/rwt/ELSEVIER/https/MSYXTLUQPJUB/10.1016/j.matlet.2019.127127
Liu Z, Liang J, Li S, Peng S, Qian Y (2004) Synthesis and growth mechanism of Bi2S3 nanoribbons. Chem Eur J 10(3):634–640. https://doi.org/10.1002/chem.200305481
Liu Y, Tang A, Zhang Q, Yin Y (2015) Seed-mediated growth of anatase TiO2 nanocrystals with core–antenna structures for enhanced photocatalytic activity. J Am Chem Soc 137(35):11327–11339. https://doi.org/10.1021/jacs.5b04676
Maiti S, Pal S, Chattopadhyay KK (2015) Recent advances in low temperature, solution processed morphology tailored ZnO nanoarchitectures for electron emission and photocatalysis applications. CrystEngComm 17(48):9264–9295. https://doi.org/10.1039/c5ce01130b
Mei W, Lin M, Chen C, Yan Y, Lin L (2018) Low-temperature synthesis and sunlight-catalytic performance of flower-like hierarchical graphene oxide/ZnO macrosphere. J Nanopart Res 20(11):286. https://doi.org/10.1007/s11051-018-4392-2
Navakoteswara Rao V, Lakshmana Reddy N, Mamatha Kumari M, Ravi P, Sathish M, Kuruvilla KM, Preethi V, Reddy KR, Shetti NP, Aminabhavi TM, Shankar MV (2019) Photocatalytic recovery of H2 from H2S containing wastewater: surface and interface control of photo-excitons in Cu2S@TiO2 core-shell nanostructures. Appl Catal B Environ 254:174–185. https://doi.org/10.1016/j.apcatb.2019.04.090
Padhi D, Parida K, Singh SK (2016) Visible-light-induced water reduction reaction for efficient hydrogen production by N-doped In2Ga2ZnO7 nanoparticle decorated on RGO sheets. Inorg Chem Front 3(12):1582–1596. https://doi.org/10.1039/c6qi00335d
Paramanik L, Reddy KH, Parida KM (2019) An energy band compactable B-rGO/PbTiO3 p–n junction: a highly dynamic and durable photocatalyst for enhanced photocatalytic H2 evolution. Nanoscale 11(46):22328–22342. https://doi.org/10.1039/c9nr06378a
Reddy KR, Hassan M, Gomes VG (2015) Hybrid nanostructures based on titanium dioxide for enhanced photocatalysis. Appl Catal A Gen 489:1–16. https://doi.org/10.1016/j.apcata.2014.10.001
Reddy NR, Bhargav U, Kumari MM, Cheralathan KK, Shankar MV, Reddy KR, Saleh TA, Aminabhavi TM (2020) Highly efficient solar light-driven photocatalytic hydrogen production over Cu/FCNTs-titania quantum dots-based heterostructures. J Environ Manag 254:109747. https://doi.org/10.1016/j.jenvman.2019.109747
Ruqia B, Nam KM, Lee H, Lee G, Choi S-I (2017) Facile synthesis of highly crystalline ZnO nanorods with controlled aspect ratios and their optical properties. CrystEngComm 19:1454–1458. https://doi.org/10.1039/c7ce00196g
Sahoo R, Mundamajhi A, Das SK (2019) Growth of ZnO nanoparticles prepared from cost effective laboratory grade ZnO powder and their application in UV photocatalytic dye decomposition. J Mater Sci Mater Electron 30(5):4541–4547. https://doi.org/10.1007/s10854-019-00743-0
Sahu K, Choudhary S, Singh J, Kuriakose S, Singhal R, Mohapatra S (2018) Facile wet chemical synthesis of ZnO nanosheets: effects of counter ions on the morphological, structural, optical and photocatalytic properties. Ceram Int 44(18):23094–23101. https://doi.org/10.1016/j.ceramint.2018.09.116
Sapkal RT, Shinde SS, Waghmode TR, Govindwar SP, Rajpure KY, Bhosale CH (2012) Photo-corrosion inhibition and photoactivity enhancement with tailored zinc oxide thin films. J Photochem Photobiol B Biol 110:15–21. https://doi.org/10.1016/j.jphotobiol.2012.02.004
Shao X, Li B, Zhang B, Shao L, Wu Y (2016) Au@ZnO core-shell nanostructures with plasmon-induced visible-light photocatalytic and photoelectrochemical properties. Inorg Chem Front 3(7):934–943. https://doi.org/10.1039/c6qi00064a
Shao B, Liu Z, Zeng G, Wu Z, Liu Y, Cheng M, Chen M, Liu Y, Zhang W, Feng H (2018) Nitrogen-doped hollow mesoporous carbon spheres modified g-C3N4/Bi2O3 direct dual semiconductor photocatalytic system with enhanced antibiotics degradation under visible light. ACS Sustain Chem Eng 6(12):16424–16436. https://doi.org/10.1021/acssuschemeng.8b03480
Sheldrick WS, Wachhold M (1997) Solventothermal synthesis of solid-state chalcogenidometalates. Angew Chem Int Ed 36(3):206–224. https://doi.org/10.1002/anie.199702061
Singh S, Barick KC, Bahadur D (2013) Shape-controlled hierarchical ZnO architectures: photocatalytic and antibacterial activities. CrystEngComm 15(23):4631–4639. https://doi.org/10.1039/c3ce27084j
Sun J, Wu K-L, Li X-Z, Dong C, Wei X-W, Wang X-W, Zhang B, Zhang Z-X, Huang J-R (2014) Self-assembly of single-crystalline α-Fe2O3 nanoplates into columnar superstructures: controllable synthesis, growth mechanism, and properties. CrystEngComm 16(30):6873–6881. https://doi.org/10.1039/c4ce00001c
Sun L, Wu W, Tian Q, Lei M, Liu J, Xiao X, Zheng X, Ren F, Jiang C (2016) In situ oxidation and self-assembly synthesis of dumbbell-like α-Fe2O3/Ag/AgX (X = Cl, Br, I) heterostructures with enhanced photocatalytic properties. ACS Sustain Chem Eng 4(3):1521–1530. https://doi.org/10.1021/acssuschemeng.5b01473
Vu TT, del Río L, Valdés-Solís T, Marbán G (2013) Fabrication of wire mesh-supported ZnO photocatalysts protected against photocorrosion. Appl Catal B Environ 140-141:189–198. https://doi.org/10.1016/j.apcatb.2013.04.023
Wang T, Jiao Z, Chen T, Li Y, Ren W, Lin S, Lu G, Ye J, Bi Y (2013) Vertically aligned ZnO nanowire arrays tip-grafted with silver nanoparticles for photoelectrochemical applications. Nanoscale 5(16):7552–7557. https://doi.org/10.1039/c3nr01459b
Wei J, Xiao X, Yang Y, Xiong R, Pan C-X, Shi J (2016) Photo-reactivity and mechanism of g-C3N4 and Ag co-modified Bi2WO6 microsphere under visible light irradiation. ACS Sustain Chem Eng 4(6):3017–3023. https://doi.org/10.1021/acssuschemeng.5b01701
Wei Y, Cheng G, Xiong J, Xu F, Chen R (2017) Positive Ni(HCO3)2 as a novel cocatalyst for boosting the photocatalytic hydrogen evolution capability of mesoporous TiO2 nanocrystals. ACS Sustain Chem Eng 5(6):5027–5038. https://doi.org/10.1021/acssuschemeng.7b00417
Wei Y, Zhu J, Gan Y, Cheng G (2018) Titanium glycolate-derived TiO2 nanomaterials: synthesis and applications. Adv Powder Technol 29(10):2289–2311. https://doi.org/10.1016/j.apt.2018.05.016
Wei Y, Cheng G, Xiong J, Zhu J, Gan Y, Zhang M, Li Z, Dou S (2019) Synergistic impact of cocatalysts and hole scavenger for promoted photocatalytic H2 evolution in mesoporous TiO2-NiSx hybrid. J Energy Chem 32:45–56. https://doi.org/10.1016/j.jechem.2018.05.013
Xia P, Zhu B, Cheng B, Yu J, Xu J (2018) 2D/2D g-C3N4/MnO2 nanocomposite as a direct Z-scheme photocatalyst for enhanced photocatalytic activity. ACS Sustain Chem Eng 6(1):965–973. https://doi.org/10.1021/acssuschemeng.7b03289
Xiong J, Cheng G, Qin F, Wang R, Sun H, Chen R (2013) Tunable BiOCl hierarchical nanostructures for high-efficient photocatalysis under visible light irradiation. Chem Eng J 220:228–236. https://doi.org/10.1016/j.cej.2013.01.033
Xiong J, Li W, Gan Y, Wei Y, Cheng G, Dou S, Li Z (2018) Extremely rapid engineering of zinc oxide nanoaggregates with structure-dependent catalytic capability towards removal of ciprofloxacin antibiotic. Inorg Chem Front 5(10):2432–2444. https://doi.org/10.1039/c8qi00435h
Xu Y, Liu J, Xie M, Jing L, Yan J, Deng J, Xu H, Li H, Xie J (2018) Graphene oxide-modified LaVO4 nanocomposites with enhanced photocatalytic degradation efficiency of antibiotics. Inorg Chem Front 5(11):2818–2828. https://doi.org/10.1039/c8qi00864g
Yao KX, Yin XM, Wang TH, Zeng HC (2010) Synthesis, self-assembly, disassembly, and reassembly of two types of Cu2O nanocrystals unifaceted with {001} or {110} planes. J Am Chem Soc 132(17):6131–6144. https://doi.org/10.1021/ja100151f
Yu C, Li G, Kumar S, Yang K, Jin R (2014) Phase transformation synthesis of novel Ag2O/Ag2CO3 heterostructures with high visible light efficiency in photocatalytic degradation of pollutants. Adv Mater 26(6):892–898. https://doi.org/10.1002/adma.201304173
Yuan X, Shen D, Zhang Q, Zou H, Liu Z, Peng F (2019) Z-scheme Bi2WO6/CuBi2O4 heterojunction mediated by interfacial electric field for efficient visible-light photocatalytic degradation of tetracycline. Chem Eng J 369:292–301. https://doi.org/10.1016/j.cej.2019.03.082
Yue H, Zhao Y, Ma X, Gong J (2012) Ethylene glycol: properties, synthesis, and applications. Chem Soc Rev 41(11):4218–4244. https://doi.org/10.1039/c2cs15359a
Zhang P, Wang T, Chang X, Gong J (2016) Effective charge carrier utilization in photocatalytic conversions. Acc Chem Res 49(5):911–921. https://doi.org/10.1021/acs.accounts.6b00036
Zhu J, Wang J, Lv F, Xiao S, Nuckolls C, Li H (2013) Synthesis and self-assembly of photonic materials from nanocrystalline titania sheets. J Am Chem Soc 135(12):4719–4721. https://doi.org/10.1021/ja401334j
Zhu J, Xiong J, Cheng G, Li W, Dou S (2019) Promoting solar-to-hydrogen evolution on Schottky interface with mesoporous TiO2-Cu hybrid nanostructures. J Colloid Interface Sci 545:116–127. https://doi.org/10.1016/j.jcis.2019.03.007
Funding
This work was supported by the Hubei Provincial Natural Science Foundation (2019CFB386) and the Central Committee Guides Local Science and Technology Development Special Project of Hubei Province (No. 2019ZYYD073). The authors are grateful for the Technology Innovation Program of Wuhan Textile University. WL thanks the Australia Research Council for funding through a Discovery Early Career Researcher Award (DECRA, No. DE180101478).
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Xiong, J., Li, W., Zhao, K. et al. Engineered zinc oxide nanoaggregates for photocatalytic removal of ciprofloxacin with structure dependence. J Nanopart Res 22, 155 (2020). https://doi.org/10.1007/s11051-020-04881-z
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DOI: https://doi.org/10.1007/s11051-020-04881-z