Bi2WO6/ZnO:一种在可见光下具有优良光催化性能的花状新型复合材料

doi:10.1016/S1872-2067(17)63004-3

催化学报 ›› 2018, Vol. 39 ›› Issue (4): 810-820.DOI: 10.1016/S1872-2067(17)63004-3

Bi₂WO₆/ZnO:一种在可见光下具有优良光催化性能的花状新型复合材料

程娟^a, 沈奕^a, 陈宽^a, 汪曦^a, 郭永福^a,b, 周晓吉^a, 白仁碧^a

a 苏州科技大学分离净化材料与技术研发中心, 江苏苏州 215009;
b 江苏高校水处理技术与材料协同创新中心, 江苏苏州 215009

收稿日期:2017-11-30 修回日期:2017-12-20 出版日期:2018-04-18 发布日期:2018-04-08
通讯作者: 郭永福, 白仁碧
基金资助:
国家自然科学基金（51578354）；江苏省六大人才高峰（2016-JNHB-067）；苏州市科技局科技计划（SS201667）；江苏省青蓝工程和江苏省研究生科研与实践创新计划（KYCX17_2067）.

Flower-like Bi₂WO₆/ZnO composite with excellent photocatalytic capability under visible light irradiation

Juan Cheng^a, Yi Shen^a, Kuan Chen^a, Xi Wang^a, Yongfu Guo^a,b, Xiaoji Zhou^a, Renbi Bai^a

a Center for Separation and Purification Materials & Technologies, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China;
b Jiangsu Collaborative Innovation Center of Water Treatment Technology and Material, Suzhou 215009, Jiangsu, China

Received:2017-11-30 Revised:2017-12-20 Online:2018-04-18 Published:2018-04-08
Contact: 10.1016/S1872-2067(17)63004-3
Supported by:
This work was supported by the National Natural Science Foundation of China (51578354), Six Talent Peaks Program (2016-JNHB-067), Suzhou Science and Technology Bureau (SS201667), and Qing Lan Project and Research Innovation Project for College Graduates of Jiangsu Province (KYCX17_2067).

摘要/Abstract

摘要：

印染废水具有水量大、色度高、难生化降解、有毒有害物质多等特点；另外抗生素废水的大量排放对水生和陆地生态系统带来了危害.光催化可有效降解有机物，因而被广泛研究和应用，其多以半导体作为光催化剂.ZnO因价廉、无毒、来源广、光催化活性高而广受关注.但是，由于其带隙较宽，只能被紫外光激发，对太阳光的利用率低，且易发生光腐蚀，光稳定性较差，从而大大降低了光催化活性，不利于其应用.将ZnO与其他半导体复合是改善其光催化活性的最有效方法之一.铋基光催化剂一直是光催化领域的研究热点，作为无机半导体纳米晶之一，Bi₂WO₆具有无毒性、适当的带隙和优异的光催化性能，因而得到广泛关注.本文将Bi₂WO₆复合到ZnO上以降低ZnO带隙能，提高其对太阳能的转换，降低电子-空穴的复合几率，促进电荷转移的有效分离，从而提高ZnO的光催化性能.
本文采用两步水热法合成了一种异质结的花状Bi₂WO₆/ZnO复合材料.通过降解亚甲基蓝（MB）和四环素，研究了其光催化性能.结果表明，该Bi₂WO₆/ZnO复合材料对MB和四环素具有优异的光催化活性，对它们的光降解效率分别是纯ZnO的246和4500倍，相应地，对这两种污染物的光降解率分别是纯ZnO的120和200倍.活性因子捕获实验结果显示，超氧自由基在光催化降解过程中起主要作用，其次是羟基自由基和光生空穴.
采用X射线衍射、透射电镜、扫描电镜、紫外-可见漫反射、N₂吸附脱附、X射线光电子能谱、荧光光谱、光电流等方法对材料的形态结构、孔结构、化学组成、带隙能、光吸收性质、载流子复合效率等进行了分析.复合后Bi₂WO₆/ZnO的形貌为微米尺寸纳米结构的花状绒球，直径约为4μm，带隙能量从3.2eV降为2.6eV.Bi₂WO₆/ZnO为介孔结构，复合后比表面积为原来的4.98倍.所制备的Bi₂WO₆/ZnO光催化剂比纯Bi₂WO₆和ZnO颗粒具有更高的瞬态光电流密度（约为4.5μA）.
综上，Bi₂WO₆和ZnO成功复合形成了异质结，降低了ZnO的禁带宽度，促进了电子和空穴的有效分离，从而提高了其光催化活性.

关键词: 钨酸铋, 氧化锌, 光催化, 亚甲基蓝, 抗生素

Abstract:

The photocatalytic ability of ZnO is improved through the addition of flower-like Bi₂WO₆ to prepare a Bi₂WO₆/ZnO composite with visible light activity. The composite is characterized by X-ray diffraction, transmission electron microscopy, scanning electron microscopy with UV-vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy and N₂ adsorption-desorption isotherms. After modification, the band gap energy of Bi₂WO₆/ZnO is reduced from 3.2 eV for ZnO to 2.6 eV. Under visible light irradiation, the Bi₂WO₆/ZnO composite shows an excellent photocatalytic activity for degrading methylene blue (MB) and tetracycline. The photo-degradation efficiencies of (0.3:1) Bi₂WO₆/ZnO for MB and tetracycline are approximately 246 and 4500 times higher than those of bare ZnO, respectively, and correspondingly, the photo-degradation rates for the two pollutants are approximately 120 and 200 times higher than those with bare ZnO, respectively. Moreover, the photocatalyst of (0.3:1) Bi₂WO₆/ZnO exhibits a higher transient photocurrent density of approximately 4.5 μA compared with those of bare Bi₂WO₆ and ZnO nanoparticles. The successful recombination of Bi₂WO₆ and ZnO enhances the photocatalytic activity and reduces the band gap energy of ZnO, which can be attributed to the effective separation of electron-hole pairs. Active species trapping experiments display that[O₂]^- is the major species involved during photocatalysis rather than·OH and h⁺. This study provides insight into designing a meaningful visible-light-driven photocatalyst for environmental remediation.

Key words: Bismuth tungstate, Zinc oxide, Photocatalysis, Methylene blue, Antibiotics

程娟, 沈奕, 陈宽, 汪曦, 郭永福, 周晓吉, 白仁碧. Bi₂WO₆/ZnO:一种在可见光下具有优良光催化性能的花状新型复合材料[J]. 催化学报, 2018, 39(4): 810-820.

Juan Cheng, Yi Shen, Kuan Chen, Xi Wang, Yongfu Guo, Xiaoji Zhou, Renbi Bai. Flower-like Bi₂WO₆/ZnO composite with excellent photocatalytic capability under visible light irradiation[J]. Chinese Journal of Catalysis, 2018, 39(4): 810-820.

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Bi₂WO₆/ZnO:一种在可见光下具有优良光催化性能的花状新型复合材料

Flower-like Bi₂WO₆/ZnO composite with excellent photocatalytic capability under visible light irradiation

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