College of Chemistry, Liaoning University, Shenyang 110036, PR China.
College of Environment, Liaoning University, Shenyang 110036, PR China.
Ultrason Sonochem. 2018 Jul;45:150-166. doi: 10.1016/j.ultsonch.2018.03.010. Epub 2018 Mar 22.
A novel Z-scheme coated composite, Er:YAlO@Ni(FeGa)O-Au-BiVO, was designed for sonocatalytic degradation of sulfanilamide and fabricated by sol-hydrothermal and calcination methods. The prepared sample was characterized by X-ray diffractometer (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), UV-vis diffuse reflectance spectra (DRS), fourier transform infrared (FT-IR) spectra, Raman spectra and photoluminescence (PL) spectra. In Er:YAlO@Ni(FeGa)O-Au-BiVO, Ni(FeGa)O and BiVO form a Z-scheme sonocatalytic system, Er:YAlO as an up-conversion luminescence agent (from visible-light to ultraviolet-light) provides the ultraviolet-light for satisfying the energy demand of wide band-gap Ni(FeGa)O and Au nanoparticles as co-catalyst forms more active sites to enrich electrons. Also, Au nanoparticles as conductive channels promotes the electrons (e) from conduction band of BiVO to transfer to valence band of Ni(FeGa)O. Due to the characteristics of valence state diversity, the Fe and V constitute a redox reaction recombination system, which can also push electrons (e) on conduction band of BiVO to quickly transfer to valence band of Ni(FeGa)O. The sonocatalytic activity of Er:YAlO@Ni(FeGa)O-Au-BiVO nanocomposite was detected through degradation of sulfanilamide under ultrasonic irradiation. A high sonocatalytic degradation ratio (95.64%) of sulfanilamide can be obtained when the conditions of 10.00 mg/L sulfanilamide, 1.00 g/L Er:YAlO@Ni(FeGa)O-Au-BiVO, 300 min ultrasonic irradiation and 100 mL total volume were adopted. Some factors such as ultrasonic irradiation time and cycle number on the sonocatalytic degradation efficiency are also investigated by using TOC and UV-vis spectroscopy. Subsequently, the effects of hydroxyl radicals (OH) and hole scavengers were investigated to elaborate the mechanism. The researches show that the prepared Z-scheme Er:YAlO@Ni(FeGa)O-Au-BiVO coated composite displayed an excellent sonocatalytic activity in degradation of sulfanilamide under ultrasonic irradiation.
一种新型的 Z 型涂层复合材料，Er:YAlO@Ni(FeGa)O-Au-BiVO，被设计用于声催化降解磺胺，通过溶胶-水热和煅烧方法制备。通过 X 射线衍射仪（XRD）、透射电子显微镜（TEM）、扫描电子显微镜（SEM）、X 射线光电子能谱（XPS）、能谱（EDX）、紫外可见漫反射光谱（DRS）、傅里叶变换红外光谱（FT-IR）光谱、拉曼光谱和光致发光（PL）光谱对制备的样品进行了表征。在 Er:YAlO@Ni(FeGa)O-Au-BiVO 中，Ni(FeGa)O 和 BiVO 形成 Z 型声催化体系，Er:YAlO 作为上转换发光剂（从可见光到紫外线）提供紫外线，以满足宽带隙 Ni(FeGa)O 和 Au 纳米粒子的能量需求，作为共催化剂形成更多的活性位点来丰富电子。此外，Au 纳米粒子作为导电通道，促进 BiVO 导带中的电子（e）转移到 Ni(FeGa)O 的价带。由于价态多样性的特点，Fe 和 V 构成了一个氧化还原反应重组体系，也可以推动 BiVO 导带中的电子（e）快速转移到 Ni(FeGa)O 的价带。通过超声辐照下磺胺的降解，检测了 Er:YAlO@Ni(FeGa)O-Au-BiVO 纳米复合材料的声催化活性。在磺胺浓度为 10.00mg/L、Er:YAlO@Ni(FeGa)O-Au-BiVO 用量为 1.00g/L、超声辐照 300min 和总体积为 100mL 的条件下，磺胺的声催化降解率可达 95.64%。还通过 TOC 和紫外可见光谱研究了超声辐照时间和循环次数等因素对声催化降解效率的影响。随后，研究了羟基自由基（OH）和空穴清除剂的影响，以阐述其机制。研究表明，所制备的 Z 型 Er:YAlO@Ni(FeGa)O-Au-BiVO 涂层复合材料在超声辐照下磺胺的降解中表现出优异的声催化活性。
