Ag担载介孔Pb3Nb2O8光催化剂的制备及其增强的可见光催化活性表征

doi:10.1016/S1872-2067(16)62575-5

催化学报 ›› 2017, Vol. 38 ›› Issue (1): 83-91.DOI: 10.1016/S1872-2067(16)62575-5

Ag担载介孔Pb₃Nb₂O₈光催化剂的制备及其增强的可见光催化活性表征

韩晓鹏^a, 吕佳男^a, 田莉^a, 孔令茹^a, 卢雪梅^a, 梅勇^a, 王绩伟^a,b, 范晓星^a,b

a 辽宁大学物理学院, 辽宁沈阳 110036;
b 辽宁大学辽宁省半导体发光与光催化材料重点实验室, 辽宁沈阳 110036

收稿日期:2016-08-29 修回日期:2016-10-15 出版日期:2017-01-18 发布日期:2017-01-18
通讯作者: Xiaoxing Fan,Tel:+86-24-62202306;Fax:+86-24-62202309;E-mail:xxfan@lnu.edu.cn;Jiwei Wang,Tel:+86-24-62202306;Fax:+86-24-62202309;E-mail:jiweiwang6688@yahoo.com
基金资助:
国家自然科学基金（11274150，11574124）；辽宁省教育厅项目（JG2016ZD0015）；作者感谢南京大学江苏省纳米技术重点实验室开放基金的资助.

Ag-loaded mesoporous Pb₃Nb₂O₈ photocatalysts with enhanced activity under visible-light irradiation

Xiaopeng Han^a, Jianan Lü^a, Li Tian^a, Lingru Kong^a, Xuemei Lu^a, Yong Mei^a, Jiwei Wang^a,b, Xiaoxing Fan^a,b

a School of Physics, Liaoning University, Shenyang 110036, Liaoning, China;
b Liaoning Key Laboratory of Semiconductor Light Emitting and Photocatalytic Materials, Liaoning University, Shenyang 110036, Liaoning, China

Received:2016-08-29 Revised:2016-10-15 Online:2017-01-18 Published:2017-01-18
Contact: Xiaoxing Fan,Tel:+86-24-62202306;Fax:+86-24-62202309;E-mail:xxfan@lnu.edu.cn;Jiwei Wang,Tel:+86-24-62202306;Fax:+86-24-62202309;E-mail:jiweiwang6688@yahoo.com
Supported by:
This work was supported by the National Natural Science Foundation of China (11274150, 11574124), the Education Minister of Liaoning Province (JG2016ZD0015), and the Open Research Fund of Jiangsu Provincial Key Laboratory for Nanotechnology Nanjing University.

摘要/Abstract

摘要：

光催化技术在环境净化方面，尤其是降解有机污染物应用上表现出潜在价值.可见光响应型光催化剂具有优异的光吸收特性和高的光催化活性，因而备受人们关注并被大量研究.Pb₃Nb₂O₈光催化剂由于其自身的稳定性以及对可见光响应的能力是一种潜在的高效光催化材料.但是，有报道表明Pb₃Nb₂O₈光催化剂对可见光降解有机物活性较低，这主要归因于它较小的比表面积以及较高的电子-空穴复合率.为了解决这个问题，本文采用蒸发自组装技术制备了大比表面积的介孔Pb₃Nb₂O₈，采用光沉积方式在介孔Pb₃Nb₂O₈上负载了均匀分散的纳米Ag颗粒，并对不同焙烧温度、载Ag量以及进一步的热处理对光催化活性的影响作了深入研究.
XRD结果表明，在400℃和500℃焙烧条件下获得的样品属于Pb₃Nb₂O₈相，600℃焙烧使得介孔Pb₃Nb₂O₈发生相变.氮气吸附-脱附表征表明，升高焙烧温度使样品比表面积从最大69 m²/g（400℃）减小到19 m²/g（600℃）.透射电子显微镜分析结果表明，所获得样品具有蠕虫状介孔孔道结构，并且Ag纳米颗粒均匀分散在介孔Pb₃Nb₂O₈表面.紫外-可见吸收光谱表明，介孔Pb₃Nb₂O₈的吸收边拖尾到530-550 nm，担载Ag之后光吸收发生显著变化，光吸收拓展到700 nm.
光催化活性测试采用可见光催化氧化脱氢异丙醇气体至丙酮反应.结果表明，在420 nm以上可见光照射下，1 h内的光催化反应过程中，采用高温固态反应制备的Pb₃Nb₂O₈上丙酮生成速率为2.9 ppm/min，而介孔Pb₃Nb₂O₈催化剂上最高可达55.5 ppm/min.介孔Pb₃Nb₂O₈负载Ag之后，400℃焙烧的介孔Pb₃Nb₂O₈光催化活性显著提高，降解速率达120.7 ppm/min.
通过介孔Pb₃Nb₂O₈和固相合成Pb₃Nb₂O₈的光催化活性对比发现，大比表面积样品的光催化活性显著提高.这可归结为大的比表面积提供了大量的催化反应活性位点，从而提高了光催化反应活性，此外介孔材料的孔壁结构为纳米结构，有利于光生电子-空穴传输到表面参加反应.担载Ag后介孔Pb₃Nb₂O₈的光催化活性进一步提高，主要是因为助催化剂Ag纳米颗粒促进了光生电子-空穴分离，延长了载流子寿命，从而提高了光催化活性.

关键词: 介孔, Pb₃Nb₂O₈, 光催化, 银担载, 气相降解

Abstract:

Mesoporous Pb₃Nb₂O₈ photocatalysts were synthesized by the evaporation-induced self-assembly (EISA) method. Ag was deposited on the surface of mesoporous Pb₃Nb₂O₈ by a facile photoreduction process. The as-prepared samples were characterized by TG-DSC, XRD, N₂ adsorption, HR-TEM and UV-Vis spectroscopy. The results revealed that mesoporous Pb₃Nb₂O₈ has a large specific surface area and uniform pore size distribution both before and after Ag deposition. The photodegradation of 2-propanol and acetaldehyde gas under visible-light (λ>420 nm) irradiation was employed to evaluate the photocatalytic activities of the samples. The results showed that the photocatalytic activity of mesoporous Pb₃Nb₂O₈ is greatly improved by the Ag co-catalyst. These mesoporous Pb₃Nb₂O₈ exhibit photocatalytic activities as much as 41 times higher when compared with the Pb₃Nb₂O₈ prepared by the solid state reaction method. The content of loaded Ag ranged from 0.5% to 5% (Ag₂SO₄). The optimal loading was determined to be 1% corresponding the highest photo-catalytic activity. These results clearly indicate that the activity of Pb₃Nb₂O₈ can be improved to obtain an outstanding performance for the photodegradation of organic pollutants.

Key words: Mesopore, Pb₃Nb₂O₈, Photocatalysis, Ag loading, Gas-phase degradation

韩晓鹏, 吕佳男, 田莉, 孔令茹, 卢雪梅, 梅勇, 王绩伟, 范晓星. Ag担载介孔Pb₃Nb₂O₈光催化剂的制备及其增强的可见光催化活性表征[J]. 催化学报, 2017, 38(1): 83-91.

Xiaopeng Han, Jianan Lü, Li Tian, Lingru Kong, Xuemei Lu, Yong Mei, Jiwei Wang, Xiaoxing Fan. Ag-loaded mesoporous Pb₃Nb₂O₈ photocatalysts with enhanced activity under visible-light irradiation[J]. Chinese Journal of Catalysis, 2017, 38(1): 83-91.

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Ag担载介孔Pb₃Nb₂O₈光催化剂的制备及其增强的可见光催化活性表征

Ag-loaded mesoporous Pb₃Nb₂O₈ photocatalysts with enhanced activity under visible-light irradiation

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