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Characterization of tin（Ⅱ） sulfide defects/vacancies and correlation with their photocurrent

Nano Research 2017年第1期10卷 218-228页

作者： Mingyang Liu Luqing Wang Linan Zhou Sidong Lei Jarin Joyner Yingchao Yang Robert Vajtai Pulickel Ajayan Boris I. Yakobson Pol Spanos Department of Materials Science and Nanoengineering Rice University Houston Texas 77005 USA Department of Chemistry Rice University Houston Texas 77005 USA

The presence of defects/vacancies in nanomaterials influences the electronic structure of materials, and thus, it is necessary to study the correlation between the optoelectronic properties of a nanomaterial and its defects/vacancies. Herein, we report a facile solvothermal route to synthesize three-dimensional （3D） SnS nanostructures formed by {131} faceted nanosheet assembly. The 3D SnS nanostructures were calcined at temperatures of 350, 400, and 450 ~C and used as counter electrodes, before their photocurrent properties were investigated. First principle computation revealed the photocurrent properties depend on the defect/vacancy concentration within the samples. It is very interesting that characterization with positron annihilation spectrometry confirmed that the density of defects/vacancies increased with the calcination temperature, and a maximum photocurrent was realized after treatment at 400 ℃. Further, the defect/vacancy density decreased when the calcination temperature reached 450℃ as the higher calcination temperature enlarged the mesopores and densified the pore walls, which led to a lower photocurrent value at 450℃ than at 400℃.

关键词： SnS microspheres mesoporous nanosheetassembly defects/vacancies positron annihilationspectrometry photocurrent.

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Correlation between types of defects/vacancies of Bi2S3 nanostructures and their transient photocurrent

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Nano Research 2017年第7期10卷 2405-2414页

作者： Mingyang Liu Luqing Wang Pei Dong Liangliang Dong Xifan Wang Jarin Joyner Xiangjian Wan Boris I. Yakobson Robert Vajtai Pulickel Ajayan PolSpanos Department of Materials Science and Nanoengineeriing Rice University Houston TX 77005 USA Department of Chemistry Rice University Houston TX 77005 USA College of Chemistry Nankai University Tianjin 300071 China

Crystalline nanostructures possess defects/vacancies that affect their physical and chemical properties. In this regard, the electronic structure of materials can be effectively regulated through defect engineering; therefore, the correlation between defects/vacancies and the properties of a material has attracted extensive attention. Here, we report the synthesis of Bi2S3 microspheres by nanorod assemblies with exposed {211} facets, and the investigation of the types and concentrations of defects/vacancies by means of positron annihilation spectrometry. Our studies revealed that an increase in the calcined temperature, from 350 to 400 ℃, led the predominant defect/vacancy densities to change from isolated bismuth vacancies （VBi） to septuple Bi3＋-sulfur vacancy associates （VBiBiBiSSSS）. Furthermore, the concentration of septuple BiB＋-sulfur vacancy associates increased as the calcined temperature was increased from 400 to 450 ℃. The characterized transient photocurrent spectrum demonstrates that the photocurrent values closely correlate with the types and concentrations of the predominant defects/vacancies. Our theoretical computation, through first principles, showed that VBiBiBiSSSS strongly absorbs I2（sol）, easily desorbs I-（sol）, and enhances the electrocatalytic activity of the nanostructures.

关键词： Bi2S3 microspheres nanorod assembly defects/vacancies positron annihilationspectrometry transient photocurrent

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