CeO2/NaNbO3复合物的水热合成及其光催化性能的提高

doi:10.1016/S1872-2067(17)62975-9

催化学报 ›› 2018, Vol. 39 ›› Issue (4): 682-692.DOI: 10.1016/S1872-2067(17)62975-9

CeO₂/NaNbO₃复合物的水热合成及其光催化性能的提高

钱进, 薛瑶, 敖燕辉, 王沛芳, 王超

河海大学环境学院浅水湖泊综合治理与资源开发教育部重点实验室, 江苏南京 210098

收稿日期:2017-11-27 修回日期:2017-12-15 出版日期:2018-04-18 发布日期:2018-04-08
通讯作者: 敖燕辉
基金资助:
国家自然科学基金创新研究群体科学基金（51421006）；国家自然科学基金（51422902，41430751，51679063）；国家重点研发计划（2016YFC0502203）；江苏高校优势学科建设工程（PAPD）.

Hydrothermal synthesis of CeO₂/NaNbO₃ composites with enhanced photocatalytic performance

Jin Qian, Yao Xue, Yanhui Ao, Peifang Wang, Chao Wang

Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing 210098, Jiangsu, China

Received:2017-11-27 Revised:2017-12-15 Online:2018-04-18 Published:2018-04-08
Contact: 10.1016/S1872-2067(17)62975-9
Supported by:
This work was supported by the National Science Funds for Creative Research Groups of China (51421006), the National Science Fundation of China for Excellent Young Scholars (51422902), the Key Program of National Natural Science Foundation of China (41430751), the National Key Plan for Research and Development of China (2016YFC0502203), the National Natural Science Foundation of China (51679063), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

摘要/Abstract

摘要：

钙钛矿型NaNbO₃由于其非线性光学、铁电、离子导电性、高声速、光催化性能和光折变等优良性能而备受关注.在光催化反应中，宽禁带宽度（≈3.24eV）使NaNbO₃具有较高的导带底（CBM）和较低的价带顶（VBM）.因此，它表现出强烈的光氧化和光还原能力.众所周知，钙钛矿型光催化剂光电子激发和传输能力的增强归因于其较高的对称性.因此，具有高对称性的立方NaNbO₃有利于电子激发和转移.但是，一些固有的缺点，包括电荷分离效率低、量子产率差和光催化活性差等，限制了其在光催化领域的实际应用.为了解决这些问题，一种有效的方法是与其他半导体结合，形成具有改善光催化活性的异质结复合物.CeO₂作为传统的催化剂在光催化领域得到了广泛研究.CeO₂具有稳定、无毒的特点，是一种n型半导体.目前，研究人员已经发现CeO₂与不同半导体的耦合可以提高CeO₂的光催化活性.这归因于能级水平的适当匹配.
本文通过简易水热法制备了高活性的CeO₂/NaNbO₃异质结复合物，并采用X射线粉末衍射（XRD）、扫描电子显微镜（SEM）、透射电子显微镜（TEM，HRTEM）和紫外-可见漫反射光谱（DRS）等表征技术研究了所制光催化剂的物相结构、样品形貌和光学性能.所制样品的光催化活性通过光催化降解无色抗菌环丙沙星（CIP）和染料罗丹明B（RhB）证实.结果表明，在紫外和可见光照射，CeO₂/NaNbO₃复合物比纯NaNbO₃具有更高的光催化活性.此外，CeO₂/NaNbO₃复合物中CeO₂的最佳质量比为2.0wt%.紫外光照射下光催化性能的显著提高是由于CeO₂/NaNbO₃异质结的形成不仅提高了光生电荷在界面范围内的迁移速率，而且降低了光激发产生的电子和空穴的复合率.可见光照射下内置电场的存在促进了电子和空穴的分离，提高了光催化性能.此外，利用光致发光（PL）光谱、光电流、电化学阻抗谱和捕获实验证明了样品的光催化反应机理.捕获实验结果表明，·OH自由基、·O₂^-自由基和空穴都参与了RhB的光催化降解过程.最后，探讨了提高光催化活性的可能机理.

关键词: 异质结, NaNbO₃, CeO₂, 光催化

Abstract:

A highly active photocatalyst CeO₂/NaNbO₃ is fabricated by a simple and facile hydrothermal method. The obtained photocatalyst composites are characterized by X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy and ultraviolet-visible diffuse reflectance spectroscopy. The photocatalytic activity of the obtained samples is demonstrated by the photocatalytic degradation of the colorless antibiotic agent ciprofloxacin and the dye rhodamine B. The results reveal that CeO₂/NaNbO₃ composites exhibit a higher photocatalytic property than pure NaNbO₃ under both UV and visible light irradiation. Furthermore, the optimum mass ratio of CeO₂ in the CeO₂/NaNbO₃ composites is 2.0 wt%. The improved photocatalytic activity is attributed to the higher separation rate of the photo-induced electrons and holes, and the higher migration rate of the photogenerated charge in the interfacial region. Furthermore, the photoluminescence pectra, photocurrent, electrochemical impedance spectroscopy and trapping experiment are applied to demonstrate the photocatalytic reaction mechanism of the as-prepared samples. The result of the trapping experiment indicates that·OH radicals,·O₂^- radicals and holes are all involved in the photocatalytic degradation process of RhB. Furthermore, a possible mechanism for the enhancement of the photocatalytic activity is also proposed.

Key words: Heterojunction, NaNbO₃, CeO₂, Photocatalysis

钱进, 薛瑶, 敖燕辉, 王沛芳, 王超. CeO₂/NaNbO₃复合物的水热合成及其光催化性能的提高[J]. 催化学报, 2018, 39(4): 682-692.

Jin Qian, Yao Xue, Yanhui Ao, Peifang Wang, Chao Wang. Hydrothermal synthesis of CeO₂/NaNbO₃ composites with enhanced photocatalytic performance[J]. Chinese Journal of Catalysis, 2018, 39(4): 682-692.

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CeO₂/NaNbO₃复合物的水热合成及其光催化性能的提高

Hydrothermal synthesis of CeO₂/NaNbO₃ composites with enhanced photocatalytic performance

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