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通过结构-性质分析识别赤铁矿光电阳极中的质子†
Identifying protons trapped in hematite photoanodes through structure–property analysis

Chemical Science(中文翻译) ( IF 9.346 ) Pub Date : 2019-12-16 , DOI: 10.1039/c9sc04853g
YutongLiu; Rodney D. L.Smith

人们难以确定赤铁矿中结构缺陷的性质及其对材料性能和光电催化水氧化的特定影响,这阻碍了其发展为光电阳极。作者对一系列赤铁矿薄膜进行了结构-性质分析,这些赤铁矿薄膜是通过在不同的温度、退火时间和气氛下对纤铁矿薄膜进行退火制成的,并通过追踪形式拉曼非活性振动模式的相对强度找到了晶格畸变幅度的梯度。结构-性质分析表明,拉曼光谱中的这一特征与光电流密度、半导体能带位置和光电催化发生有关。该文章提出光电催化的发生与起着带内重组位点作用的缺陷的位置有关;结构畸变程度的增加将这些状态移向导带,从而促进重组。作者对关键拉曼振动的性质、X射线衍射图和合成条件进行了分析,结果表明,变形的原因为晶格捕获质子所引起的铁空位。快速诊断特定结构缺陷的能力将有助于优化赤铁矿光电阳极的制备方案。


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Uncertainty regarding the nature of structural defects in hematite and their specific impacts on material properties and photoelectrocatalytic water oxidation inhibits their development as photoanodes. We perform structure–property analysis on a series of hematite films fabricated by annealing lepidocrocite films with varied temperatures, annealing times and atmospheres and find a gradient in the magnitude of a crystal lattice distortion by tracking the relative intensity of a formally Raman inactive vibrational mode. Structure–property analysis reveals that this feature in the Raman spectrum correlates to photocurrent density, semiconductor band positions, and the onset of photoelectrocatalysis. We propose that the onset of photoelectrocatalysis is linked to the location of defects that act as intraband recombination sites; an increase in the degree of structural distortion shifts these states towards the conduction band, thereby facilitating recombination. Analysis of the nature of the key Raman vibrations, X-ray diffraction patterns, and the synthetic conditions leads us to assign the distortion to iron vacancies that are induced by the trapping of protons within the crystal lattice. The ability to rapidly diagnose a specific structural defect will aid in the optimization of fabrication protocols for hematite photoanodes.
更新日期:2019-12-17

 

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