太阳光响应型Ag2S/Ag3PO4复合材料的制备及催化降解水杨酸

doi:10.7503/cjcu20140003

摘要/Abstract

摘要：

以AgNO₃, Na₂HPO₄和硫粉为原料, 采用共沉淀-水热法合成了具有太阳光响应型Ag₂S/Ag₃PO₄复合材料, 运用扫描电子显微镜(SEM)、 X射线粉末衍射(XRD)、 X射线光电子能谱(XPS)和紫外-可见漫反射(UV-Vis DR)光谱等方法对样品进行了表征, 并在模拟太阳光条件下, 考察了Ag₂S/Ag₃PO₄对水杨酸的光催化降解效率. 结果表明, 与Ag₃PO₄相比, Ag₂S的负载量为1%(质量分数)时Ag₂S/Ag₃PO₄粒径变小, 呈立方晶相结构; Ag₂S/Ag₃PO₄复合材料可以有效促进光生电子-空穴分离, 使Ag₃PO₄禁带宽度降低到2.24 eV, 并增强了可见光的吸收能力. 在Ag₂S负载量为1%, 120 ℃水热4 h条件下, Ag₂S/Ag₃PO₄复合材料具有最佳光催化活性, 经模拟太阳光照射60 min对10 mg/L的水杨酸去除率达到88.2%.

关键词: 硫化银, 磷酸银, 光催化, 模拟太阳光, 水杨酸

Abstract:

An efficient sunlight responsive Ag₂S/Ag₃PO₄ composite was prepared by co-precipitation method combined with hydrothermal treatment. The morphology, composition, surface physical and chemical property and optical absorption property were characterized by scanning electron microscope(SEM), X-ray powder diffraction(XRD), X-ray photoelectron spectroscopy(XPS) and ultraviolet-visible diffuse reflection(UV-Vis DR). The 1%Ag₂S/Ag₃PO₄ composite has rough surface with smaller particle size less than 0.8 μm and wider bandgap(2.24 eV) compared to Ag₃PO₄. The photocatalytic activity of Ag₂S/Ag₃PO₄ was evaluated by degradation of salicylic acid which is a typical material in pharmaceuticals and personal care products(PPCPs) and harmful to human health and ecosystems. The results show that Ag₂S/Ag₃PO₄ composite doped 1%Ag₂S with hydrothermal treated at 120 ℃ for 4 h exhibits excellent salicylic acid degradation efficiency reached to 88.2% under simulated sunlight irradiation for 60 min and the light source current intensity is 15 A, when Ag₂S/Ag₃PO₄ used 0.15 g, the initial concentration of salicylic acid is 10 mg/L and pH is 6.0, respectively. The contribution of various parameters for the enhanced photocatalytic activities is revealed in detail. The primary reasons for the increased simulated sunlight photocatalyst activity are contribution to the perfect cubic crystal structure, smaller particle size and broaden the visible spectral response. Doping sulfide is benefit to absorb sunlight and separate the electron-hole effectively.

Key words: Silver sulfide, Silver phosphate, Photocatalysis, Simulated sunlight, Salicylic acid

中图分类号:

O649.4

TrendMD:

朱遂一, 徐东方, 方帅, 耿直, 杨霞. 太阳光响应型Ag₂S/Ag₃PO₄复合材料的制备及催化降解水杨酸. 高等学校化学学报, 2014, 35(6): 1286.

ZHU Suiyi, XU Dongfang, FANG Shuai, GENG Zhi, YANG Xia. Sunlight-Responsive Ag₂S/Ag₃PO₄ Composite Preparation and Degradation of Salicylic Acid^†. Chem. J. Chinese Universities, 2014, 35(6): 1286.

图/表 12

Fig.1 SEM images of Ag3PO4(A) and 1%Ag2S/Ag3PO4(B) treated by hydrothermal 120 ℃ for 4 h, and EDS of 1%Ag2S/Ag3PO4(C)

Fig.2 X-Ray diffraction patterns of Ag3PO4(a), 1%Ag2S/Ag3PO4(b) and 20%Ag2S/Ag3PO4(c) treated at 120 ℃ for 4 h

Fig.3 X-Ray diffraction patterns of 1%Ag2S/Ag3PO4 treated at 40 ℃(a), 120 ℃(b), 160 ℃(c) for 4 h

Fig.4 XPS spectra of Ag3d(A), P2p(B) and O1s(C) of Ag3PO4(a) and 1%Ag2S/Ag3PO4(b) treated at 120 ℃ for 4 h

Fig.5 UV-Vis DR spectra for Ag3PO4(a), 0.5%Ag2S/Ag3PO4(b), 1%Ag2S/Ag3PO4(c) and 2%Ag2S/Ag3PO4(d) with hydrothermal treated at 120 ℃ for 4 h

Fig.6 Influence of Ag2S doping in Ag2S/Ag3PO4 with hydrothermal treated at 120 ℃ for 4 h on degradation of salicylic acida. Ag3PO4; b. 0.5%Ag2S/Ag3PO4; c. 1%Ag2S/Ag3PO4; d. 2%Ag2S/Ag3PO4.

Fig.7 Influence of hydrothermal temperature of 1%Ag2S/Ag3PO4 with hydrothermal treated for 4 h on degradation of salicycic acida. 40 ℃; b. 80 ℃; c. 120 ℃; d. 160 ℃.

Fig.8 Influence of hydrothermal time of 1%Ag2S/Ag3PO4 with hydrothermal treated at 120 ℃ on degradation of salicylic aeidTime/h: a. 2; b. 4; c. 8; d. 16.

Fig.9 Influence of different light source current intensity on degradation of salicylic acid by 1%Ag2S/Ag3PO4pH value of salicylic acid is 6.0; c0=20 mg/L; amount of catalysts is 0.15 g. I/A: a. 10; b. 15; c. 20.

Fig.10 Influence of initial pH value in solution on degradation of salicylic acid by 1%Ag2S/Ag3PO4Light source current intensity is 15 A; the amount of catalysts is 0.15 g; c0=20 mg/L. a. pH=4.0; b. pH=6.0; c. pH=8.0.

Fig.11 Photolysis of salicylic acid(a) and influence of catalyst amount(c—d) on degradation of salicylic acid by 1%Ag2S/Ag3PO4Light source current intensity is 15 A; V=100 mL, pH=6.0; c0=20 mg/L. m(1%Ag2S/Ag3PO4)/g: a. 0; b. 0.05; c. 0.15; d. 0.25.

Fig.12 Influence of initial concentration of salicylic acid on degradation of salicylic acid by 1%Ag2S/Ag3PO4Light source current intensity is 15 A; pH value is 6.0; the amount of catalysts is 0.15 g. csalicylic acid/(mg·L-1): a. 10; b. 20; c. 30.

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太阳光响应型Ag₂S/Ag₃PO₄复合材料的制备及催化降解水杨酸

Sunlight-Responsive Ag₂S/Ag₃PO₄ Composite Preparation and Degradation of Salicylic Acid^†

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