Effect of gadollunium doping on visible light photocatalytic performance of Ag3PO4: Evaluation of activity in degradation of an anthraquinone dye and mechanism study

E. Ghazalian , N. Ghasemi , A.R. Amani-Ghadim
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引用次数: 32

Abstract

Gadolinium (Gd)-doped silver orthophosphate (Ag3PO4) nanoparticles, with spherical morphology, were synthesized by a co-precipitation method and their photocatalytic activities were evaluated in degradation of Reactive Blue 19 (RB19), as a model organic pollutant. The synthesized Ag3PO4 and Gd-doped Ag3PO4 were characterized using X-ray diffraction pattern analysis, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, diffuse reflectance UV–vis spectroscopy and photoluminescence spectroscopy. In comparison with Ag3PO4, the experimental results revealed a considerable enhancement in photocatalytic activity of Gd-doped Ag3PO4. The optimum mole fraction of Gd loading in Ag3PO4 was 3%. Lower photocatalytic degradation efficiency of RB19 in the presence of oxalate anion and p-benzoquinone indicated the crucial role of photogenerated holes and superoxide anion-radicals in photocatalysis on Gd-doped Ag3PO4. The enhancement of photocatalytic activity was attributed to scavenge the photoexcited electrons, and to suppress their recombination with holes and generation of active oxygen species. A nonlinear empirical kinetic model was introduced to predict the apparent first order rate constant (kapp) as a function of operational parameters, including initial RB19 concentration, Gd-doped Ag3PO4 dosage and light intensity. Degradation byproducts were identified using gas chromatography-mass spectrometry and a probable pathway was proposed. Moreover, Gd-doped Ag3PO4 samples displayed adequate reusability after three successive experiments.

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钆掺杂对Ag3PO4可见光催化性能的影响:降解蒽醌染料的活性评价及机理研究
采用共沉淀法合成了球状的钆掺杂正磷酸银(Ag3PO4)纳米颗粒,并对其降解活性蓝19 (RB19)的光催化活性进行了研究。采用x射线衍射图分析、扫描电镜、能量色散x射线能谱、透射电镜、漫反射紫外-可见光谱、光致发光光谱等方法对合成的Ag3PO4和gd掺杂的Ag3PO4进行了表征。实验结果表明,与Ag3PO4相比,gd掺杂Ag3PO4的光催化活性显著增强。Ag3PO4中Gd的最佳摩尔分数为3%。在草酸阴离子和对苯醌存在下,RB19的光催化降解效率较低,说明光生空穴和超氧阴离子自由基在gd掺杂Ag3PO4的光催化中起着至关重要的作用。光催化活性的增强归因于清除光激发电子,抑制它们与空穴的复合和活性氧的生成。引入非线性经验动力学模型,预测表观一阶速率常数(kapp)随RB19初始浓度、gd掺杂Ag3PO4剂量和光强的变化规律。采用气相色谱-质谱联用技术对降解副产物进行了鉴定,并提出了可能的降解途径。此外,经过三次连续实验,gd掺杂Ag3PO4样品显示出足够的可重复使用性。
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期刊介绍: The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.
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