微波液相法一步合成H3PW12O40/Bi2WO6光催化剂及其脱氮性能

doi:10.7503/cjcu20140021

摘要/Abstract

摘要：

采用微波液相法一步合成了固载型H₃PW₁₂O₄₀/Bi₂WO₆光催化剂. 通过紫外-可见漫反射光谱(UV-Vis)、场发射扫描电子显微镜(SEM)、表面积及孔隙度(BET)测定、氨气程序升温脱附(NH₃-TPD)、吡啶吸附红外光谱(Py-FTIR)和X射线衍射(XRD)对所合成催化剂的结构和性质进行了考察, 并以吡啶浓度为15 mg/g的模拟油对光催化剂的脱氮效果进行评价. 结果表明, 与传统浸渍固载法相比, 微波液相一步法不仅能高效合成H₃PW₁₂O₄₀/Bi₂WO₆光催化剂, 且所合成的催化剂能被低能量的光激发. 固载H₃PW₁₂O₄₀不但能提高Bi₂WO₆纳米颗粒的表面酸量, 还能通过改变Bi₂WO₆前驱液的酸强度来调控催化剂形貌. 在H₃PW₁₂O₄₀固载量为15%(质量分数), 微波功率为800 W, 反应时间为90 min条件下得到的H₃PW₁₂O₄₀/Bi₂WO₆的光催化脱氮活性最高, 在催化剂与模拟油质量比为1/300, 500 W氙灯光照60 min的最佳光催化反应条件下, 模拟油脱氮率达到92.63%.

关键词: 微波, 一步合成, 磷钨酸, 钨酸铋, 光催化, 脱氮

Abstract:

Immobilized nano-photocatalysts H₃PW₁₂O₄₀/Bi₂WO₆ was prepared by microwave liquid one-step process. The morphology, structure and properties of the prepared catalysts were characterized and investigated by UV-Vis diffuse reflectance spectra, scanning electron microscopy(SEM), NH₃ temperature programmed desorption(NH₃-TPD), pyridine adsorption Fourier transform infrared spectroscopy(Py-FTIR) and X-ray diffraction(XRD), respectively. Their photocatalytic denitrification properties were evaluated by using the model oil with 15 mg/g pyridine. The results show that H₃PW₁₂O₄₀/Bi₂WO₆ photocatalysts could be more efficiently synthesized by microwave liquid one-step process, and it could be excited by lower photon energy than that synthesized by common impregnation immobilization method. Immobilization of H₃PW₁₂O₄₀ on Bi₂WO₆ could improve the acid content in Bi₂WO₆ nanoparticle surface, change the acid strength of Bi₂WO₆ precursor solution thereby controll the catalyst morphology. The influences of preparation conditions on photocatalytic properties of H₃PW₁₂O₄₀/Bi₂WO₆ were investigated. It was found that H₃PW₁₂O₄₀/Bi₂WO₆ nano-photocatalyst, with the H₃PW₁₂O₄₀ loading(mass fraction) of 15%, prepared by microwave liquid one-step process under microwave power 800 W for 90 min possessed the best performance in the photocatalytic denitrification of model oil containing photocatalysts(mass ratio of catalyst to model oil was 1/300) after 500 W Xe lamp irradiation for 60 min, with the denitrification rate reached 92.63%.

Key words: Microwave, One-step, H3PW12O40, Bi2WO6, Photocatalysis, Denitrification

中图分类号:

O644

TrendMD:

陈颖, 邢宸, 姬生伦, 梁宏宝, 张宏宇, 陈艳. 微波液相法一步合成H₃PW₁₂O₄₀/Bi₂WO₆光催化剂及其脱氮性能. 高等学校化学学报, 2014, 35(6): 1277.

CHEN Ying, XING Chen, JI Shenglun, LIANG Hongbao, ZHANG Hongyu, CHEN Yan. One-step Preparation of H₃PW₁₂O₄₀/Bi₂WO₆Nano-photocatalysts by Microwave Liquid Process and Its Photocatalysis Denitrification Properties^†. Chem. J. Chinese Universities, 2014, 35(6): 1277.

图/表 14

Fig.1 XRD patterns of Bi2WO6 prepared under 800 W microwave power for different reaction timet/min: a. 10; b. 30; c. 60; d. 90; e. 120.

Fig.2 SEM images of Bi2WO6 prepared under 800 W microwave power for different reaction timet/min: (A) 10; (B) 30; (C) 60; (D) 90; (E) 120.

Fig.3 XRD patterns of H3PW12O40/Bi2WO6 with different H3PW12O40 loadingsw(H3PW12O40)(%): a. 5; b. 10; c. 15; d. 20; e. 25.

Fig.4 SEM images of H3PW12O40/Bi2WO6 with different H3PW12O40 loadingsw(H3PW12O40)(%): (A) 5; (B) 10; (C) 15; (D) 20; (E) 25.

Fig.5 NH3-TPD spectra of H3PW12O40/Bi2WO6 with different H3PW12O40 loadingsw(H3PW12O40)(%): a. 5; b. 10; c. 15; d. 20; e. 25.

Fig.6 Pyridine adsorption FTIR spectrum of 15%H3PW12O40/Bi2WO6

Fig.7 N2 adsorption-desorption isotherms for 15%H3PW12O40/Bi2WO6(a) and Bi2WO6(b)

Fig.8 BJH pore size distribution curves of 15%H3PW12O40/Bi2WO6(a) and Bi2WO6(b)

Fig.9 UV-Vis diffuse reflectance spectra of Bi2WO6(a), H3PW12O40/Bi2WO6(T)(b) and H3PW12O40/Bi2WO6(c) catalysts

Fig.10 Mechanism of H3PW12O40/Bi2WO6 for coupling

Table 1 Results of denitrification performance of H3PW12O40/Bi2WO6(microwave power: 800 W; reaction time: 90 min) with different loadings of H3PW12O40 with or without light(photocatalytic time: 60 min)

w(H₃PW₁₂O₄₀)(%)	0	5	10	15	20	25
Denitrification rate(%)	80.78	82.29	85.96	92.63	89.21	86.46
Denitrification rate(without light)(%)	22.83	27.69	30.24	36.21	31.18	24.83

Fig.11 Denitrification performance of H3PW12O40/Bi2WO6 catalysts prepared under 800 W microwave power for different time and with different H3PW12O40 loadingsXenon lamp: 500 W; photocatalytic time: 60 min; mcatalyst/msimulated oil: 1/300. Sythestic time of catalysts/min: a. 10; b. 30; c. 60; d. 90; e. 120.

Fig.12 Denitrification rate of simulated oil with di-fferent addition amount of 15%H3PW12O40/Bi2WO6 and photocatalytic timeXenon lamp: 500 W; mcatalysts/msimulated oil: a. 1/500; b. 1/400; c. 1/300; d. 1/200.

Fig.13 Denitrification performance of catalysts for different cycle timesXenon lamp: 500 W; photocatalytic time: 60 min; mcatalysts/msimulated oil: 1/300.

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微波液相法一步合成H₃PW₁₂O₄₀/Bi₂WO₆光催化剂及其脱氮性能

One-step Preparation of H₃PW₁₂O₄₀/Bi₂WO₆Nano-photocatalysts by Microwave Liquid Process and Its Photocatalysis Denitrification Properties^†

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