Photocatalytic performance mesoporous Nd2O3 modified ZnO nanoparticles with enhanced degradation of tetracycline

doi:10.1016/j.cattod.2020.11.002

Catalysis Today

Volume 380, 15 November 2021, Pages 259-267

https://doi.org/10.1016/j.cattod.2020.11.002 Get rights and content

Highlights

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Mesoporous Nd₂O₃ modified ZnO were synthesized using templates approach.
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The samples were evaluated by the photodegradation of tetracycline under visible light.
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Degradation rate of 3%Nd₂O₃/ZnO was improved 8.8 and 16.3 times than ZnO and P-25.
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The photodegradation efficiency of 3%Nd₂O₃/ZnO reached up to 100 % for 2 h.
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3%Nd₂O₃/ZnO showed sufficient stability for five repeated runs without loss.

Abstract

This contribution reports the synthesis of mesoporous X% Nd₂O₃ modified ZnO (X = 1, 2, 3 and 4) during sol-gel process in existence of Pluronic F-108 for the first time. XRD indicated the construction of hexagonal ZnO nanocrystals and the isotherms exhibited of type IV with a type H2 hysteresis loop, indicating the existence of mesostructures. The synthesized samples were evaluated by photodegradation of tetracycline (TC) in visible light exposure compared to pure mesoporous ZnO nanoparticles (NPs) and commercial photocatalyst P-25. The photocatalytic efficiency mesoporous 3%Nd₂O₃/ZnO for degradation TC reached up to 100 % for 2 h compared to pure mesoporous ZnO and P-25 with 4 and 10 %, respectively. The mesoporous 3%Nd₂O₃/ZnO photocatalysts showed promoted photocatalytic performance, resulting in an improved photodegradation rate value up to 8.8 and 16.3 times that of compared to pure ZnO and P-25, which was explained by better photogenerated charge carriers separation as a result of heterojunction construction between Nd₂O₃ and ZnO interfaces. In addition, the 3%Nd₂O₃/ZnO photocatalysts showed sufficient stability for five repeated runs and created its potential utility for mitigation of organic pollutants in comparison to pure ZnO and commercial P-25.

Graphical abstract

Introduction

Advanced oxidation technologies are considered the most important approaches for remediation of organic pollutants from industrial wastewater; however, photocatalysis process has become a promising procedure in presence of semiconductors as effective photocatalyst through illumination [[1], [2], [3], [4]]. Zinc oxide (ZnO) exhibit chemical stability, high redox potential, nontoxicity and superior physical properties. ZnO is commonly employed as a photocatalyst to degrade toxic organic compounds owing to its large bandgap (3.37 eV) and strong photosensitivity; they can provide an intense driving force for oxidation and reduction reactions [[5], [6], [7]]. Sometimes, ZnO exhibits a better photodegradation efficiency of organic compounds than TiO₂ [8,9]. It offers some substantial characteristics such as stronger light absorption, considerable greater electronic mobility for its slight electron efficient mass, more simple morphology tailored features and reduce charge recombination [[10], [11], [12]]. The main disadvantageous of ZnO is the dominant absorption in the UV region, indicating to reducing its photocatalytic activity, which utilizes only for 3–5 % spectral reaching the earth from sunlight, consequently restraining its efficient wide spectral range [13]. In addition, ZnO exhibits photocorrosion, indicating a significant reduction in the ZnO photostability in the cycle runs through the illumination of UV and visible light, also minimize the ZnO potential application based photocatalysts in large scale [14]. To solve these problems, considerable potentials have been dedicated to modifying the electronic ZnO for harvesting visible light in a wide range by introducing nonmetals, anions, cations, and precious metals [15,16]. Recently, nanoscale carbonaceous materials modified ZnO to form composite and hybridization has received attention to be an effective and promising avenue to promote the stability and photocatalytic efficiency of ZnO [[17], [18], [19]].

The photocatalytic performance of ZnO relies on diverse factors for instance surface area, phase purity, nature of dopants, crystallite size, and synthesis procedures [[20], [21], [22]]. ZnO is found to be a host for doping diverse metals ions and precious metals; they further modify donor and acceptor defects, the bandgap of ZnO for the required level, mobility, conductivity, and varying magnetic and optical properties [[23], [24], [25]]. Furthermore, it was considered that the oxygen vacancies in ZnO are importantly created by metals ions and precious metals doping, and therefore, the photocatalytic performance can be further promoted by boosting mobility [26,27]. For example, the bandgap energy of Cu₂O and MnO is 2.05 and 4 eV, respectively, obtained by diverse content of Cu or Mn ions; the bandgap energy has been modified from 3.3 eV to 4 eV or 2.05 eV for ZnO structure and cubic Mn_xZn_1−xO [28]. This creates the elongation of UV absorption up to the wide visible wavelengths range. The Fe ions doping ZnO mesocrystals promotes photocatalytic efficiency by 145 %. Also, transition metals co-doped ZnO indicates that the obtained ionic states with multivalent are playing an essential role in the ferromagnetism characteristics [29]. On the other hand, Neodymium oxide is one of the most important lanthanides with unique and specific electrical, electronic and optical properties, and has been closely examined for applications in the thermoluminescent and luminescent materials, thin films, advanced materials, protective coatings, photonic, and catalysts. Nd₂O₃ NPs are of interest for potential applications owing to their tunnelling, interfacial surface, and small-size effects. In recent years, the synthesis of Nd₂O₃ with various morphologies exhibited a crucial role in diverse wide potential applications [30].

Mesostructure materials as effective photocatalysts have paid huge attention for their potential applications and special properties. However, the fabrication of mesostructured materials in a one-step process is limited. A series of nanoscale and microscale materials has been widely synthesized in the existence of ethylene glycol [31]. In our previous research, we have focused our efforts in examining the principle correlation of triblock copolymer F-127 surfactant on the crystallinity and morphology of TiO₂ and ZnO [32,33]. This contribution reports the synthesis of mesoporous X% Nd₂O₃ modified ZnO (X = 1, 2, 3 and 4) via a simple chemical route using triblock co-polymer Pluronic (F-108) for the first time. The synthesized samples were assessed for TC photodegradation under the illumination of visible light compared to pure mesoporous ZnO NPs and P-25. The mesoporous 3%Nd₂O₃/ZnO photocatalysts exhibited the best photocatalytic performance among all the synthesized samples, resulting in an improved photodegradation rate value up to 8.8 and 16.3 times that of compared to pure mesoporous ZnO and P-25, which was explained by better photogenerated charge carriers separation as a result of heterojunction construction between Nd₂O₃ and ZnO interfaces.

Section snippets

Materials

Nonionic surfactant poly(ethylene glycol)-block-poly (propylene glycol)-block-poly (ethylene glycol) average M_n ∼14,600; Pluronic® F-108, Zn(NO₃)₃.6H₂O, Nd(NO₃)₃.6H₂O, CH₃COOH, HCl, and C₂H₅OH were purchased from Sigma-Aldrich.

Synthesis of mesoporous Nd₂O₃ modified ZnO NPs

Nonionic surfactant Pluronic F-108 surfactant was employed to construct a mesoporous ZnO network followed by impregnated Nd³⁺ ions at diverse contents (1−4 wt%). In particular, 0.2 g F-108 was dissolved in 30 mL of C₂H₅OH through magnetically stirring for 1 h. Afterwards, 20.3 g of Zn(NO₃)₃.6H₂O was gradually added to the above solution during the stirring and then, 0.74 mL of HCl and 2.3 mL of CH₃COOH were added as well with further stirring for 1 h. The obtained sol was dried and polymerized

Characterizations

JEOL JEM-2100 F electron microscope (Japan) was used to determine TEM images operating at 200 kV. A Thermo Scientific K-ALPHA spectrometer was used to determine X-ray photoelectron spectroscopy (XPS) data. Bruker AXS D4 Endeavour X diffractometer was employed to record XRD patterns. Quantachrome Autosorb equipment was employed to measure the N₂adsorption-desorption isotherms at 77 K after outgassing at 200 °C overnight. Perkin Elmer was employed to record Fourier transforms infrared

Photocatalytic evaluation

The photocatalytic efficiency of mesoporous Nd₂O₃ modified ZnO photocatalysts was performed for degradation of TC [20 mg/L] under the illumination of visible light with λ > 420 nm. The xenon lamp with 300 W intensity was fixed above the photoreactor (250 mL), which cooling through H₂O circulation. 0.6−3 g/l of the catalyst was suspended in the TC solution through air pumping to obtain oxygen. Before the illumination, the suspension was stirred for 30 min to get adsorption equilibrium of the

Results and discussion

To stabilize ZnO NPs with highly dispersed, a F-108 template was introduced as a soft template to construct a mesoporous ZnO network. This approach was found to be extremely efficient in improving the construction of a dispersed Nd₂O₃ NPs within a mesoporous ZnO matrix. The synthesis of mesoporous ZnO NPs at diverse Nd₂O₃ contents (1−4 wt %) using Pluronic® F-108 was achieved in two steps, firstly, mesoporous ZnO NPs were synthesized via a simple chemical route with controlling decomposition of

Photodegradation performance of mesoporous Nd₂O₃ modified ZnO photocatalysts

It is well-known that few factors are playing a crucial role in enhancing photocatalytic efficiencies, such as light availability, catalyst composition, and surface area. However, it is difficult to explore a clear and direct correlation between the photocatalytic efficiency and effecting factors due to the complication of the photocatalysis mechanism. The photocatalytic efficiency of mesoporous ZnO NPs and 1, 2, 3 and 4% Nd₂O₃/ZnO photocatalysts for TC photodegradation was evaluated under the

Conclusions

A green precursor-based route with a convenient and an economical for synthesizing mesoporous Nd₂O₃ modified ZnO photocatalysts was achieved. The synthesized mesoporous ZnO NPs exhibited a hexagonal structure with the construction of the mesopores structure. The modifying of Nd₂O₃ into mesoporous ZnO NPs was obtained an outstanding effect on its photocatalytic performance for TC degradation compared to mesoporous ZnO NPs and commercial P-25. The k values of 1, 2, 3 and 4% Nd₂O₃/ZnO

Declaration of Competing Interest

The authors report no declarations of interest.

Acknowledgements

This project was funded by the Deanship of Scientific Research (DSR) at King Abdulaziz University, Jeddah, Saudi Arabia under grant no. KEP-PhD-7-130-41. The authors, therefore, acknowledge with thanks DSR for technical and financial support

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Photocatalytic performance mesoporous Nd2O3 modified ZnO nanoparticles with enhanced degradation of tetracycline

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Materials

Synthesis of mesoporous Nd2O3 modified ZnO NPs

Characterizations

Photocatalytic evaluation

Results and discussion

Photodegradation performance of mesoporous Nd2O3 modified ZnO photocatalysts

Conclusions

Declaration of Competing Interest

Acknowledgements

Arabian J. Chem.

J. Taiwan Inst. of Chem. Eng.

Mater. Lett.

Mater. Chem. Phys.

J. Mol. Catal. A Chem.

J. Hazard. Mater. B

Mater. Lett.

Appl. Surf. Sci.

Carbon

Appl. Catal. B

Superlattices Microstruct.

Mater. Des.

Catal. Today

Surf. Coat. Technol.

Powder Technol.

J. Electron. Spectrosc. Relat. Phenom.

J. Magn. Magn. Mater.

J. Photochem. Photobiol. A: Chem.

Surf. Sci.

Chemosphere

Microporous Mesoporous Mater.

Chem. Phys.

Chem. Eng. J.

J. Mol. Catal. A Chem.

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Comparison of ZnO and TiO2 nanowires for photoanode of dye sensitized solar cells

J. Alloys. Compd.

Photocatalytic performance mesoporous Nd₂O₃ modified ZnO nanoparticles with enhanced degradation of tetracycline

Synthesis of mesoporous Nd₂O₃ modified ZnO NPs

Photodegradation performance of mesoporous Nd₂O₃ modified ZnO photocatalysts

Highly efficient and recyclable catalyst: porous Fe₃O₄–Au magnetic nanocomposites with tailored synthesis

A Novel Au@Cu₂O-Ag ternary nanocomposite with highly efficient catalytic performance: towards rapid reduction of methyl orange under dark condition

Comparison of ZnO and TiO₂ nanowires for photoanode of dye sensitized solar cells