有机溶剂热分解法碳化硅纳米电缆合成与性能研究
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摘要
碳化硅(SiC)半导体材料是继第一代元素半导体材料(Si)和第二代化合物半导体材料(Ge、S、GaP、InP等)之后发展起来的第三代半导体材料,,具有间接宽禁带、大的击穿电场、高的热导率和高的电子饱和漂移速度等特点,使其在高温、高频、高功率和抗辐射等极端环境下工作的光电子器件制备方面有着巨大的应用前景。SiC纳米线除保留其宽带隙半导体性能外,还由于纳米尺寸效应、特定的形貌和内在的特殊结构,在力学性能、发光性能和场发射性能等方面展现出更多特异性,因此研究SiC纳米线合成、结构和性能具有重要意义。
采用有机溶剂热分解法,我们成功地合成了几种SiC基—维纳米结构,并研究了其一些性质。
1)用甲醇热分解法合成了SiC-SiO_2纳米电缆;讨论了其合成中出现的纳米电缆分支现象和多种形貌形成的机理;研究了纳米电缆的红外、拉曼光谱和光致发光光谱等光谱性质。
2)用以醇热分解法合成了具有高质量SiC单晶核部的SiC-SiO_2纳米电缆,并讨论了红外光谱中出现的一些特殊现象的起因。
3)通过调节气流速度,合成了碳纳米颗粒修饰的SiC-SiO_2纳米电缆、SiC-SiO_2-C三重同轴纳米电缆;研究了其光学及场发射性质。
4)以四氯化钛为催化剂,生长了SiC-SiO_2狼牙棒核壳纳米结构并讨论了其生长机理。
In connection with discovering of carbon nanotubes in 1991,one-dimensional nanostructures,such as nanowires,nanobelts,nanorods,and nanocables have attracted much attention in the field of material research owing to their unique structural and physical properties different form the traditional bulk materials.Resent research results show that they are valuable for the fundamental research of materials and possess potential application.Among the several materials,SiC has been focused as potential material because their outstanding properties,such as wide band-gap,high breakdown field,high saturation drift velocity,short carrier lifetime,high thermal conductivity,excellent mechanical and chemical properties,etc.Compared to bulk material,SiC nanostructures reveal outstanding optical and field emission properties caused by quantum confinement effects and novel structures.Therefore,the material studies of SiC 1D structure are of great importance for future nanoscale photonic and electronic devices.In spite of its outstanding material properties,the study of SiC-based 1D nanostructure is in primary stage.Now,exploring of several synthesis methods,characteristics of basic optical and field emission properties have become main contents of their study.Up to now,several methods such as thermal reduction of carbon nanotubes,direct heat method and chemical vapor deposition,etc.For industrial application,it needs to develop a simple method to synthesize large-scale SiC nanostructures uniformly and at low-cost.In this work,we present a simple and low-cost method to synthesize SiC nanostructures in large-scale and uniformly.Our synthesis of SiC 1D nanostructure is based on the thermal decomposition of organic solvents,i.e.,methanol and ethanol.The synthesis of SiC 1D nanostructure was carried out on the common Si substrate.The morphology,microstructure,crystal structure and several physical properties of nanostructures have been studied systematically and discussed their growth mechanisms.
Carbon monoxide is a necessary precursor for synthesis of SiC-SiO_2 core-shell nanocables.We use gaseous carbon monoxide produced by thermal decomposition of organic solvents as a precursor.The use of thermal decomposition of organic solvents in the synthesis of SiC nanostructure makes it convenient and simple.Based on this method,it is possible to synthesize high-quality and large-scale SiC-SiO_2 core-shell nanocables at low-cost.
In the works for synthesis of SiC-SiO_2 nanocables,we found that the catalyst dispersion on the Si substrate plays key role for uniform distribution of nanocable.For uniform dispersion of catalyst on the whole surface of Si substrate,we explored a noble covering method of catalyst on Si substrate and a new catalyst mixture.The dispersion state of catalyst and the distribution of resultant nanocables on the Si substrate were investigated using scanning electron microscopy and Raman microscopy.Most of nanocables did not exceed 50 nm in diameter and revealed smooth surface morphologies.Some of them were divided into two or four branches. It is found that the dividing of nanocables was due to the simultaneous formation of several crystal seeds in one catalyst droplet.Unordinary carbon-related peaks were appeared in Raman spectra recorded from the surface of Si substrate on which nanocables have been distributed nonuniformly.These unordinary carbon-related peaks were still observed after annealed at 800℃for 30min in the air.Their origins were discussed comparing with the result of SEM observation.
We also investigated the possibility of the use of ethanol for synthesis of SiC nanocables.Differing from the case of methanol,several species such as carbon,H_2O, and hydrocarbons are produced in thermal decomposition course.These species affect on the several properties of nanocables.The existence of these species gave us the possibility to control of microstructures of nanocables.By using the thermal decomposition of ethanol,we successfully synthesized SiC-SiO_2 core-shell nanocables, SiC-C-SiO_2 ternary coaxial nanocables,SiC-SiO_2 nanocables decorated with carbon nanoparticles,and SiC-SiO_2-C ternary coaxial nanocables.We also successfully controlled the diameter of SiC core and the thickness of SiO_2 shell by adjusting the flow ratio between Ar and Ar/ethanol.The former three kinds of nanostructures revealed good photoluminescence properties and the later showed potential application for field emission display.
At the end,we synthesized a noble SiO_2 hierarchical nanostructure on SiC nanowires by using a mixture of ethanol and titanium tetrachloride as a precursor.On the basis of SEM and HRTEM observation,the growth mechanism of this noble nanostructure was proposed.
采用有机溶剂热分解法,我们成功地合成了几种SiC基—维纳米结构,并研究了其一些性质。
1)用甲醇热分解法合成了SiC-SiO_2纳米电缆;讨论了其合成中出现的纳米电缆分支现象和多种形貌形成的机理;研究了纳米电缆的红外、拉曼光谱和光致发光光谱等光谱性质。
2)用以醇热分解法合成了具有高质量SiC单晶核部的SiC-SiO_2纳米电缆,并讨论了红外光谱中出现的一些特殊现象的起因。
3)通过调节气流速度,合成了碳纳米颗粒修饰的SiC-SiO_2纳米电缆、SiC-SiO_2-C三重同轴纳米电缆;研究了其光学及场发射性质。
4)以四氯化钛为催化剂,生长了SiC-SiO_2狼牙棒核壳纳米结构并讨论了其生长机理。
In connection with discovering of carbon nanotubes in 1991,one-dimensional nanostructures,such as nanowires,nanobelts,nanorods,and nanocables have attracted much attention in the field of material research owing to their unique structural and physical properties different form the traditional bulk materials.Resent research results show that they are valuable for the fundamental research of materials and possess potential application.Among the several materials,SiC has been focused as potential material because their outstanding properties,such as wide band-gap,high breakdown field,high saturation drift velocity,short carrier lifetime,high thermal conductivity,excellent mechanical and chemical properties,etc.Compared to bulk material,SiC nanostructures reveal outstanding optical and field emission properties caused by quantum confinement effects and novel structures.Therefore,the material studies of SiC 1D structure are of great importance for future nanoscale photonic and electronic devices.In spite of its outstanding material properties,the study of SiC-based 1D nanostructure is in primary stage.Now,exploring of several synthesis methods,characteristics of basic optical and field emission properties have become main contents of their study.Up to now,several methods such as thermal reduction of carbon nanotubes,direct heat method and chemical vapor deposition,etc.For industrial application,it needs to develop a simple method to synthesize large-scale SiC nanostructures uniformly and at low-cost.In this work,we present a simple and low-cost method to synthesize SiC nanostructures in large-scale and uniformly.Our synthesis of SiC 1D nanostructure is based on the thermal decomposition of organic solvents,i.e.,methanol and ethanol.The synthesis of SiC 1D nanostructure was carried out on the common Si substrate.The morphology,microstructure,crystal structure and several physical properties of nanostructures have been studied systematically and discussed their growth mechanisms.
Carbon monoxide is a necessary precursor for synthesis of SiC-SiO_2 core-shell nanocables.We use gaseous carbon monoxide produced by thermal decomposition of organic solvents as a precursor.The use of thermal decomposition of organic solvents in the synthesis of SiC nanostructure makes it convenient and simple.Based on this method,it is possible to synthesize high-quality and large-scale SiC-SiO_2 core-shell nanocables at low-cost.
In the works for synthesis of SiC-SiO_2 nanocables,we found that the catalyst dispersion on the Si substrate plays key role for uniform distribution of nanocable.For uniform dispersion of catalyst on the whole surface of Si substrate,we explored a noble covering method of catalyst on Si substrate and a new catalyst mixture.The dispersion state of catalyst and the distribution of resultant nanocables on the Si substrate were investigated using scanning electron microscopy and Raman microscopy.Most of nanocables did not exceed 50 nm in diameter and revealed smooth surface morphologies.Some of them were divided into two or four branches. It is found that the dividing of nanocables was due to the simultaneous formation of several crystal seeds in one catalyst droplet.Unordinary carbon-related peaks were appeared in Raman spectra recorded from the surface of Si substrate on which nanocables have been distributed nonuniformly.These unordinary carbon-related peaks were still observed after annealed at 800℃for 30min in the air.Their origins were discussed comparing with the result of SEM observation.
We also investigated the possibility of the use of ethanol for synthesis of SiC nanocables.Differing from the case of methanol,several species such as carbon,H_2O, and hydrocarbons are produced in thermal decomposition course.These species affect on the several properties of nanocables.The existence of these species gave us the possibility to control of microstructures of nanocables.By using the thermal decomposition of ethanol,we successfully synthesized SiC-SiO_2 core-shell nanocables, SiC-C-SiO_2 ternary coaxial nanocables,SiC-SiO_2 nanocables decorated with carbon nanoparticles,and SiC-SiO_2-C ternary coaxial nanocables.We also successfully controlled the diameter of SiC core and the thickness of SiO_2 shell by adjusting the flow ratio between Ar and Ar/ethanol.The former three kinds of nanostructures revealed good photoluminescence properties and the later showed potential application for field emission display.
At the end,we synthesized a noble SiO_2 hierarchical nanostructure on SiC nanowires by using a mixture of ethanol and titanium tetrachloride as a precursor.On the basis of SEM and HRTEM observation,the growth mechanism of this noble nanostructure was proposed.
引文
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