Photocatalytic hydrogen production from water–methanol mixtures using N-doped Sr2Nb2O7under visible light irradiation: effects of catalyst structure

光催化 制氢 催化作用 兴奋剂 可见光谱 材料科学 光化学 甲醇 化学工程 辐照 无机化学 化学 光电子学 物理 核物理学 有机化学 工程类
作者
Sang Min Ji,Pramod H. Borse,Hyun Gyu Kim,Dong Won Hwang,Jum Suk Jang,Sang Won Bae,Jae Sung Lee
出处
期刊:Physical Chemistry Chemical Physics [Royal Society of Chemistry]
卷期号:7 (6): 1315-1321 被引量:109
标识
DOI:10.1039/b417052k
摘要

Nitrogen-doped perovskite type materials, Sr2Nb2O7−xNx (0, 1.5 < x < 2.8), have been studied as visible light-active photocatalysts for hydrogen production from methanol–water mixtures. Nitrogen doping in Sr2Nb2O7 red-shifted the light absorption edge into the visible light range and induced visible light photocatalytic activity. There existed an optimum amount of nitrogen doping that showed the maximum rate of hydrogen production. Among the potential variables that might cause this activity variation, the crystal structure appeared to be the most important. Thus, as the extent of N-doping increased, the original orthorhombic structure of the layered perovskite was transformed into an unlayered cubic oxynitride structure. The most active catalytic phase was an intermediate phase still maintaining the original layered perovskite structure, but with a part of its oxygen replaced by nitrogen and oxygen vacancy to adjust the charge difference between oxygen and doped nitrogen. These experimental observations were explained by density functional theory calculations. Thus, in Sr2Nb2O7−xNx, N 2p orbital was the main contributor to the top of the valence band, causing band gap narrowing while the bottom of conduction band due to Nb 4d orbital remained almost unchanged.
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