表面钒修饰对α-Fe2O3材料光电化学性能的增强作用

引用本文: 姚利珍, 孔德生, 杜玖瑶, 王泽, 张经纬, 王娜, 李文娟, 冯媛媛. 表面钒修饰对α-Fe₂O₃材料光电化学性能的增强作用[J]. 物理化学学报, 2015, 31(10): 1895-1904. doi: 10.3866/PKU.WHXB201509074 shu

Citation: YAO Li-Zhen, KONG De-Sheng, DU Jiu-Yao, WANG Ze, ZHANG Jing-Wei, WANG Na, LI Wen-Juan, FENG Yuan-Yuan. Enhancement of the Photoelectrochemical Activity of α-Fe₂O₃ Materials by Surface Modification with Vanadium[J]. Acta Physico-Chimica Sinica, 2015, 31(10): 1895-1904. doi: 10.3866/PKU.WHXB201509074 shu

表面钒修饰对α-Fe₂O₃材料光电化学性能的增强作用

基金项目:
山东省自然科学基金(ZR2010EM026) (ZR2010EM026)

国家级大学生创新创业训练计划项目(201410446044)资助 (201410446044)

摘要:

对半导体材料进行表面化学修饰或改性, 是提高其光催化活性、有效利用光能的一种重要措施. 本文结合水热化学法、化学池沉积和后续热处理等, 分别制备了未修饰α-Fe₂O₃和钒修饰的α-Fe₂O₃光电极材料. 利用X射线粉末衍射(XRD)谱和紫外-可见漫反射光谱(UV-Vis-DRS)技术分析表征了材料的晶相结构、化学组成和光谱吸收等固体物理化学性能; 利用光电流测量和电化学交流阻抗谱(EIS)实验技术, 并基于1 mol·L^-1NaOH (pH 13.6)中的光电化学水分解反应, 研究了钒修饰对α-Fe₂O₃材料光电化学性能的增强作用. 结果表明,与未修饰的Fe₂O₃材料相比, 钒修饰α-Fe₂O₃样品出现FeVO4的XRD特征峰, 但临界光吸收波长未发生红移; 钒修饰使Fe₂O₃材料的光电流增大4-5倍、光生载流子在电极表面的复合几率降低了3/4-4/5、电极表面电荷传递速率(表观一级速率常数)明显提高. 结合Fe₂O₃/溶液界面半导体能带模型和有关研究结果, 分析了研究体系的界面电荷动力学传输过程以及钒修饰使α-Fe₂O₃材料光电化学性能增强的原因.

关键词:

English

Enhancement of the Photoelectrochemical Activity of α-Fe₂O₃ Materials by Surface Modification with Vanadium

1.
Department of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, Shandong Province, P. R. China
Received Date: 10 July 2015
Available Online: 10 October 2015
Fund Project:
山东省自然科学基金(ZR2010EM026)

国家级大学生创新创业训练计划项目(201410446044)资助

Abstract:

Surface modification of semiconductor materials is an effective way to improve their photocatalysis and photo-conversion activities. Bare and V-modified α-Fe₂O₃ photoelectrode materials were prepared using hydrothermal, chemical bath deposition and heat treatment approaches. Their physicochemical and photoelectrochemical (PEC) properties were then investigated with X-ray diffractometry (XRD), UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS), voltammetry, and electrochemical AC impedance spectroscopy (EIS) techniques. The existence of FeVO4 was indicated by its characteristic X-ray diffractometry patterns, while no significant red shifts in the photoabsorption edge were detected in UV-Vis diffuse reflectance spectroscopy spectra. With V-modified and bare Fe₂O₃ serving as a photoanode, photoelectrochemical measurements were carried out for water splitting in 1 molmol·L^-1 NaOH (pH 13.6). The enhancement of α-Fe₂O₃ photoelectrochemical activities through V-modification was indicated by significantly increased photocurrents and decreased photocharge-recombination probability. By measuring electrochemical AC impedance spectroscopy spectra, pseudo-first-order rate constants for the charge transfer at the illuminated electrode/solution interface were estimated. The rate constant for V-modification of the Fe₂O₃ electrode was higher than that of the bare Fe₂O₃ electrode. Improved interfacial charge transfer kinetics through V-modification is responsible for the enhanced photoelectrochemical activities of α-Fe₂O₃. The interfacial photocharge transfer and recombination processes and their properties are discussed with a semiconductor energy band model constructed for the electrode system.

Key words:

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