کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
---|---|---|---|---|
60946 | 47555 | 2014 | 9 صفحه PDF | دانلود رایگان |
• A framework was built to predict the type of reactive oxygen species produced during photoexcitation of semiconductors.
• We used electron spin resonance spectroscopy to study the reactive oxygen species and photogenerated electrons.
• ZnS can generate O2−, OH and O21; CdS can produce O2− and O21, In2S3 can generate O2− while Bi2S3 neither generate ROS.
• We correlated the ROS and electrons information with photocatalytic oxidation and reduction of photocatalysts.
• This theoretical and experimental model should be of great value for understanding semiconductor photocatalysis.
A broadly applicable theoretical and experimental framework was developed for understanding the photocatalytic mechanism of semiconductors. Using this framework, we found that it is possible to predict the type and reactivity of reactive oxygen species and electrons produced during photoexcitation of semiconductors by comparing the band edge energies of semiconductors with the redox potentials of relevant species. In addition, we could experimentally verify these predictions using electron spin resonance spectroscopy (ESR) with spin trapping and spin labeling techniques. We selected four types of metal sulfides (CdS, ZnS, In2S3, and Bi2S3) to elucidate the applicability of this model system. Using ESR technique, we found that these four sulfides are significantly different in the types of produced reactive oxygen species. When irradiated, ZnS can generate superoxide (O2−), hydroxyl radicals (OH), and singlet oxygen (1O2); CdS and In2S3 can produce O2−, while irradiation of Bi2S3 generates none of these reactive oxygen species. These results are correlated with the photocatalytic oxidation and reduction activities of metal sulfide structures.
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Journal: Journal of Catalysis - Volume 320, December 2014, Pages 97–105