Effect of the Ce3+ concentration on the crystallite structure and optical properties of ZnO nanomaterials synthesised by sol-gel method

Thi Bich Hop Dang, Van Cuong Nguyen, Quoc Thuan Hoang, Tien Ha Le, Van Quang Nguyen, Thi Lan Huong Pham
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Abstract

In this study, Ce3+-doped ZnO nanomaterials (Zn1-xO:xCe3+ NPs) were synthesised using the sol-gel method. X-ray diffraction (XRD) pattern and Raman spectra analysis showed that at 1% doping concentration, Zn2+ ions were replaced with Ce3+ ions in the ZnO lattice. However, at higher concentrations (3 and 5%), the CeO2 phase was formed, preventing the diffusion process of Ce3+ ions into the lattice. Field emission scanning electron microscopy (FESEM) images showed that the obtained material had a particle size of several tens of nanometers. X-ray energy dispersive (EDS) spectroscopy and EDS mapping spectra revealed that the synthesised Zn1-xO:xCe3+ NPs had high purity and the Ce element was uniformly distributed in the sample. UV-Vis spectroscopy confirmed the strong interaction between Ce3+ ions and ZnO lattice, leading to increased light absorption in the visible region. The photoluminescence (PL) spectrum of ZnO showed two emission regions peaking at 389 and 650 nm, attributed to band to band recombination and defect types of ZnO such as oxygen vacancy (Vo) and/or oxygen interstitial (Oi), respectively. In comparison with ZnO, the PL spectrum of Zn1-xOx:Ce3+ (x=1-5) samples showed that the visible region emission appeared at new peak at 580 nm originating to the 3d → 4f transition of Ce3+ ions. As the doping concentration increased gradually from 1 to 5%, the 580 nm peak intensity increased, and the 389 peak intensity decreased significantly, indicating that Ce3+ ions inhibited the NBE recombination process of ZnO. This study suggested that Ce3+ doped ZnO NPs have a great potential for application in visible-light photocatalysis.
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Ce3+ 浓度对溶胶-凝胶法合成的氧化锌纳米材料晶粒结构和光学特性的影响
本研究采用溶胶-凝胶法合成了掺杂 Ce3+ 的氧化锌纳米材料(Zn1-xO:xCe3+ NPs)。X 射线衍射(XRD)图和拉曼光谱分析表明,当掺杂浓度为 1%时,ZnO 晶格中的 Zn2+ 离子被 Ce3+ 离子取代。然而,当浓度较高(3% 和 5%)时,CeO2 相形成,阻止了 Ce3+ 离子向晶格的扩散过程。场发射扫描电子显微镜(FESEM)图像显示,所得材料的粒度为几十纳米。X 射线能量色散(EDS)光谱和 EDS 图谱显示,合成的 Zn1-xO:xCe3+ NPs 纯度很高,Ce 元素均匀地分布在样品中。紫外可见光谱证实了 Ce3+ 离子与 ZnO 晶格之间的强烈相互作用,从而增加了可见光区的光吸收。氧化锌的光致发光(PL)光谱显示出两个发射区,峰值分别为 389 纳米和 650 纳米,这分别归因于带间重组和氧化锌的缺陷类型,如氧空位(Vo)和/或氧间隙(Oi)。与氧化锌相比,Zn1-xOx:Ce3+(x=1-5)样品的聚光光谱显示,可见光区的发射在 580 nm 处出现了新的峰值,这源于 Ce3+ 离子的 3d → 4f 转变。随着掺杂浓度从 1%逐渐增加到 5%,580 nm 峰强度增加,389 峰强度显著下降,表明 Ce3+ 离子抑制了 ZnO 的 NBE 重组过程。该研究表明,掺杂 Ce3+ 的 ZnO NPs 在可见光光催化中具有很大的应用潜力。
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