增强可见光光电催化活性的二维BiOI纳米片/一维BiPO4纳米棒p-n异质结复合电极的制备

doi:10.1016/S1872-2067(18)63186-9

催化学报 ›› 2019, Vol. 40 ›› Issue (3): 446-457.DOI: 10.1016/S1872-2067(18)63186-9

增强可见光光电催化活性的二维BiOI纳米片/一维BiPO₄纳米棒p-n异质结复合电极的制备

刘森, 赵梦雨, 和泽田, 钟义, 丁浩, 陈代梅

中国地质大学(北京)材料科学与工程学院, 北京 100083

收稿日期:2018-08-31 修回日期:2018-10-13 出版日期:2019-03-18 发布日期:2019-02-22
通讯作者: 陈代梅
基金资助:
国家自然科学基金（21577132）；中央大学基础研究基金（2652017377，2652017378）.

Preparation of a p-n heterojunction 2D BiOI nanosheet/1DBiPO₄ nanorod composite electrode for enhanced visible light photoelectrocatalysis

Sen Liu, Mengyu Zhao, Zetian He, Yi Zhong, Hao Ding, Daimei Chen

Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China

Received:2018-08-31 Revised:2018-10-13 Online:2019-03-18 Published:2019-02-22
Supported by:
This work was partly supported by the National Natural Science Foundations of China (21577132) and the Fundamental Research Funds for the Central Universities (2652017377, 2652017378).

摘要/Abstract

摘要：

光电催化是一种新型催化技术，在去除水中有机物方面具有独特的优势.在光电协同作用下具有较高的量子效率，电子-空缺负荷率低，稳定性好等优势.BiPO₄具有较宽的禁带宽度，只能响应有限的紫外光区域，极大限制了其光电催化效率.因此，本文在电化学三电极体系下，通过简单的两步电沉积法将BiPO₄纳米棒/BiOI纳米片复合薄膜沉积固定在FTO玻璃上，制备了BiPO₄/BiOI/FTO复合光电极材料.通过场发射扫描电镜，透射电子电镜，X射线光单子能谱、紫外可见漫反射光谱以及电化学测试对其组成、晶体形貌结构和光学性质进行表征.考察了外加工作电压、碘氧铋电极沉积时间等因素对四环素去除效果的影响.结果表明，BiOI纳米片生长在BiPO₄纳米棒上，形成了异质结结构，BiPO₄/BiOI/FTO复合薄膜电极具有良好的光吸收性能和优异的电荷转移特性.当碘氧铋沉积时间为150s，外加偏压为1.2V时，复合薄膜电极具有最佳的四环素去除效率，4h达到80%.在相同的实验条件下，BiPO₄/BiOI/FTO复合薄膜电极对四环素的去除效率分别是BiPO₄/FTO电极和BiOI/FTO电极的1.6倍和1.4倍.在光电协同作用下，BiPO₄/BiOI/FTO复合光电极对污染物的去除效率是单纯光催化和电催化对污染物去除效率的2.8倍和2.5倍.同时该复合光电极具有好的稳定性，经过四次16h的循环实验，光电极对四环素的去除效果基本保持不变.
根据一系列表征结果和p-n异质结形成的方式，推测了p-n异质结的结构和反应过程.在光激发作用下，BiOI导带上的光生电子有效的转移到BiPO₄导带上，然后在外加偏压的作用下通过外电路转移到铂丝电极上，光生电子与氧气反应生产超氧自由基降解有机污染物.另一方面，光生空穴从BiPO₄价带上转移到BiOI价带上，与水反应生产羟基自由基，作为光电催化反应过程中的主要活性物种.总之，增强的光电催化活性BiOI/BiPO₄异质结构可能主要归因于p-n异质结结构改善催化剂的光吸收能力和有效的电子-空穴转移过程.

关键词: 电沉积, 光电催化, BiOI/BiPO₄/FTO, 四环素

Abstract:

In this study, a 2D BiOI nanosheet/1D BiPO₄ nanorod/fluorine-doped tin oxide (FTO) composite electrode with a p-n heterojunction structure was prepared by a two-step electrodeposition method. Field-emission scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, UV-visible diffuse reflectance spectroscopy, and electrochemical testing were used to characterize its composition, crystal morphology, and optical properties. The BiOI/BiPO₄/FTO composite electrode has higher photoelectrocatalytic (PEC) activity for the degradation of tetracycline than pure BiPO₄ and BiOI. The PEC activity of the composite was 1.98 times and 2.46 times higher than those of the BiOI/FTO and BiPO₄/FTO electrodes, respectively. The effects of the working voltage and BiOI deposition time on the degradation of tetracycline were investigated. The optimum BiOI deposition time was found to be 150 s and the optimum working voltage is 1.2 V. Trapping experiments showed that hydroxyl radicals (·OH) and superoxide radicals (·O₂^-) are the major reactive species in the PEC degradation process. The BiOI/BiPO₄/FTO composite electrode has good stability, and the tetracycline removal efficiency remains substantially unchanged after four cycles in a static system. The reason for the PEC efficiency enhancement in the BiOI/BiPO₄/FTO composite electrode is the increased visible light absorption range and the p-n heterojunction structure, which promotes the separation and migration of the photogenerated electrons and holes.

Key words: Electrodeposition, Photoelectrocatalysis, BiOI/BiPO₄/FTO, Tetracycline

刘森, 赵梦雨, 和泽田, 钟义, 丁浩, 陈代梅. 增强可见光光电催化活性的二维BiOI纳米片/一维BiPO₄纳米棒p-n异质结复合电极的制备[J]. 催化学报, 2019, 40(3): 446-457.

Sen Liu, Mengyu Zhao, Zetian He, Yi Zhong, Hao Ding, Daimei Chen. Preparation of a p-n heterojunction 2D BiOI nanosheet/1DBiPO₄ nanorod composite electrode for enhanced visible light photoelectrocatalysis[J]. Chinese Journal of Catalysis, 2019, 40(3): 446-457.

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增强可见光光电催化活性的二维BiOI纳米片/一维BiPO₄纳米棒p-n异质结复合电极的制备

Preparation of a p-n heterojunction 2D BiOI nanosheet/1DBiPO₄ nanorod composite electrode for enhanced visible light photoelectrocatalysis

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