形貌调控的Bi_2S_3基纳米晶光催化剂合成及性能研究
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摘要
半导体纳米晶作为光催化剂在污水处理领域中有着非常重要的作用。本论文即主要研究了Bi2S3纳米结构和Bi2S3-TiO2异质结构的形貌控制合成,以及它们的光催化性能。
本文第一章综述了半导体非均相光催化的基本理论及光催化剂Bi2S3纳米结构的研究进展。
本文第二章主要介绍了不同维度Bi2S3纳米结构的合成及它们在降解三种典型染料时的光催化性能。本实验利用单一前驱物Bi(S2CNEt2)3在有机胺中热分解得到了高质量的Bi2S3纳米点,纳米棒和分散的单晶纳米片。通过对结构的进一步研究发现Bi2S3纳米棒和纳米片分别是由纳米点和纳米棒自组装而成的,并在此基础上提出了粘附-重结晶的生长机理。在光催化方面,这三种纳米晶体可以选择性地光降解罗丹明B,亚甲基蓝和甲基橙这三种染料,并且不同维度的Bi2S3纳米结构催化活性不同。
为了提高Bi2S3在可见光下的催化效率,本文的第三章通过水热法简便地合成出了Bi2S3-TiO2异质结构。实验条件对产物的结构和形貌有着显著的影响。在优化铋源浓度,钛源与铋源浓度比例和丙酮含量等实验参数后,我们确定了使Bi2S3纳米棒对TiO2纳米颗粒负载率较高,且Bi2S3-TiO2异质结构催化性能最优的实验条件。同时,通过对比研究Bi2S3-TiO2异质结构,德固赛P 25,空白的TiO2和Bi2S3,以及二者的机械混合物的在可见光下的催化活性,我们发现Bi2S3和TiO2之间的协同作用促使了电子-空穴对的转移,从而使Bi2S3-TiO2异质结构具有优异的催化性能。
Nano-scaled semiconductors have received increasing interests to serve as photocatalysts in wastewater treatment. In this thesis, morphology-tunable Bi2S3 nanostructures and Bi2S3-TiO2 heterostructures have been synthesized and their morphology-dependent photocatalytic performances have been studied.
In Chapter 1, the principle theories of heterogenerous photocatalysis and recent progress of Bi2S3 nanostructures have been reviewed.
In Chapter 2, Bi2S3 nanostructures with different dimensionalities have been synthesized and the research of their photocatalytic performance on three different dyes has been carried out. Bi2S3 nanostructures including nanodots, nanorods, and discrete single-crystal nanosheets were synthesized through the thermal decomposition of a single-source precursor Bi(S2CNEt2)3 in amine media. The morphology evolution revealed that the Bi2S3 nanorods and nanosheets were developed through the assembling of metastable nanodots and nanorods, and an attachment-recrystallization growth mechanism was proposed for the formation of nanorods and nanosheets. As for the photocatalysis, the three kinds of nanocrystals could selectively enhance the photodegradation of three typical dyes including rhodamine B, methylene blue, methyl orange, and the efficiencies were dependent on dimensionalities.
In order to improve the photocatalytic efficiency of Bi2S3 under visible light irradiation, in Chapter 3, Bi2S3-TiO2 heterostructures were conveniently synthesized by hydrothermal method. Experimental variables had obvious influence on the structure and morphology of the heterostructures. After optimizing the experimental parameters, such as the concentration of Bi precursor, molar ratio of Ti/Bi and the volume of acetone, we determined the most suitable conditions, under which there was a high coverage of TiO2 nanoparticles on Bi2S3 nanorods, and the photocatalytic activities of Bi2S3-TiO2 heterostructures reached the maximum. Through the comparison of photocatalytic activities between Bi2S3-TiO2 heterostructures and P 25, blank TiO2 and Bi2S3, as well as the mechanical mixture of them, we found that there was an interaction between TiO2 and Bi2S3, leading to an improved electron-hole pairs separation and causing the excellent photocatalytic performance.
本文第一章综述了半导体非均相光催化的基本理论及光催化剂Bi2S3纳米结构的研究进展。
本文第二章主要介绍了不同维度Bi2S3纳米结构的合成及它们在降解三种典型染料时的光催化性能。本实验利用单一前驱物Bi(S2CNEt2)3在有机胺中热分解得到了高质量的Bi2S3纳米点,纳米棒和分散的单晶纳米片。通过对结构的进一步研究发现Bi2S3纳米棒和纳米片分别是由纳米点和纳米棒自组装而成的,并在此基础上提出了粘附-重结晶的生长机理。在光催化方面,这三种纳米晶体可以选择性地光降解罗丹明B,亚甲基蓝和甲基橙这三种染料,并且不同维度的Bi2S3纳米结构催化活性不同。
为了提高Bi2S3在可见光下的催化效率,本文的第三章通过水热法简便地合成出了Bi2S3-TiO2异质结构。实验条件对产物的结构和形貌有着显著的影响。在优化铋源浓度,钛源与铋源浓度比例和丙酮含量等实验参数后,我们确定了使Bi2S3纳米棒对TiO2纳米颗粒负载率较高,且Bi2S3-TiO2异质结构催化性能最优的实验条件。同时,通过对比研究Bi2S3-TiO2异质结构,德固赛P 25,空白的TiO2和Bi2S3,以及二者的机械混合物的在可见光下的催化活性,我们发现Bi2S3和TiO2之间的协同作用促使了电子-空穴对的转移,从而使Bi2S3-TiO2异质结构具有优异的催化性能。
Nano-scaled semiconductors have received increasing interests to serve as photocatalysts in wastewater treatment. In this thesis, morphology-tunable Bi2S3 nanostructures and Bi2S3-TiO2 heterostructures have been synthesized and their morphology-dependent photocatalytic performances have been studied.
In Chapter 1, the principle theories of heterogenerous photocatalysis and recent progress of Bi2S3 nanostructures have been reviewed.
In Chapter 2, Bi2S3 nanostructures with different dimensionalities have been synthesized and the research of their photocatalytic performance on three different dyes has been carried out. Bi2S3 nanostructures including nanodots, nanorods, and discrete single-crystal nanosheets were synthesized through the thermal decomposition of a single-source precursor Bi(S2CNEt2)3 in amine media. The morphology evolution revealed that the Bi2S3 nanorods and nanosheets were developed through the assembling of metastable nanodots and nanorods, and an attachment-recrystallization growth mechanism was proposed for the formation of nanorods and nanosheets. As for the photocatalysis, the three kinds of nanocrystals could selectively enhance the photodegradation of three typical dyes including rhodamine B, methylene blue, methyl orange, and the efficiencies were dependent on dimensionalities.
In order to improve the photocatalytic efficiency of Bi2S3 under visible light irradiation, in Chapter 3, Bi2S3-TiO2 heterostructures were conveniently synthesized by hydrothermal method. Experimental variables had obvious influence on the structure and morphology of the heterostructures. After optimizing the experimental parameters, such as the concentration of Bi precursor, molar ratio of Ti/Bi and the volume of acetone, we determined the most suitable conditions, under which there was a high coverage of TiO2 nanoparticles on Bi2S3 nanorods, and the photocatalytic activities of Bi2S3-TiO2 heterostructures reached the maximum. Through the comparison of photocatalytic activities between Bi2S3-TiO2 heterostructures and P 25, blank TiO2 and Bi2S3, as well as the mechanical mixture of them, we found that there was an interaction between TiO2 and Bi2S3, leading to an improved electron-hole pairs separation and causing the excellent photocatalytic performance.
引文
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