二維奈米材料硼氮碳、氮化硼、二硫化鉬的合成、 鑑定與應用

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Title:	二維奈米材料硼氮碳、氮化硼、二硫化鉬的合成、鑑定與應用
Other Titles:	Synthesis, Characterization, and Applications of Few Layered Boron Carbonitride, Boron Nitride, and Molybdenum Disulfide Nanosheets
Authors:	張鋅權 Zhang, Xin-Quan
Contributors:	林宗吾 Lin, Tsung-Wu 化學系
Keywords:	石墨烯;氮化硼;二硫化鉬;奈米薄片;取代反應;場效電晶體 graphene;boron nitride;molybdenum disulfide;nanosheets;substitution reaction;field effect transistor
Date:	2012
Issue Date:	2014-02-13T03:41:24Z (UTC)
Abstract:	在2004 年， Prof. Andre Geim 和Dr. Konstantin Novoselov 等人利用簡單的力學剝離法，獲得單層石墨的結構---亦即所謂的石墨烯，並發現石墨烯具有優異的電子與力學性質，開啟了各種層狀材料結構的特性與應用的探討。本碩士研究內容為二維奈米材料之合成、鑑定與應用，其工作包含摻雜氧化石墨烯來合成硼氮碳奈米薄片、用水熱法剝離氮化硼塊材形成奈米薄片、以及利用化學氣相沉積法合成大面積單層二硫化鉬。第一章內容主要陳述石墨烯、硼碳氮奈米薄片、氮化硼奈米薄片以及二硫化鉬奈米薄片基本的結構與性質，與目前研究的發展。第二章為本碩士工作的實驗合成方法以及所使用的鑑定儀器。第三章為硼氮碳奈米薄片合成的結果與討論，藉由硼與氮原子對石墨烯中的碳原子進行部分取代，進而摻雜六方氮化硼於石墨烯中。根據X 射線光電子能譜(XPS)的資料，BN 摻雜的濃度會隨著反應溫度的的增加而升高。除此之外，發現在摻雜氮化硼的實驗中，氣態氨氣的使用有助於降低反應溫度。在不同合成溫度下 BCN 樣品的拉曼光譜顯示 I(D)/I(G) 比值與石墨烯中摻雜 BN 的濃度成正比。除此之外，本工作也使用電子能損譜儀鑑定 BCN 樣品中 BN 區塊的空間分布。最後，不同摻雜濃度 BCN 薄膜的 UV 光譜證實 BN 摻雜打開並調控石墨烯的光學能隙;並且討論硼氮碳奈米薄片場效電晶體的電性表現。第四章為氮化硼奈米薄片的合成，實驗中成功藉由水熱反應在氮化硼粉末上修飾 OH 官能團，並藉以震盪得氮化硼奈米薄片，由原子力顯微鏡的結果可看出高度與縱向寬度會隨反應溫度時間的增加而降低；XPS 的結果顯示OH 修飾的濃度，會隨著反應溫度與時間增加而提高，此點並由UV 光譜儀的結果所驗證，隨著OH 修飾濃度的增加，樣品在水溶液中具有較佳的分散性。最後再藉由π-π交互作用力進行氮化硼奈米薄片對?四甲酸四甲鹽(PTAS)分子的吸脫附，實驗發現氮化硼奈米薄片上OH 官能團修飾濃度的上升會阻礙PTAS 分子的吸附。第五章則討論二硫化鉬的合成，實驗上藉由化學氣相沉積法直接在 SiO2/Si基板上合成出大面積二硫化鉬奈米薄片。此研究係利用還原氧化石墨烯(rGO)，?四甲酸四甲鹽(PTAS)和?四甲酸二酐(PTCDA)等分子做為晶種來協助薄膜之生長且形成的薄膜包含單層、雙層以及其他少層結構。此研究藉由 XPS 確認MoS2 的計量數及價態等化學組態，並討論單層二硫化鉬在拉曼光譜以及光致光光譜的表現。穿透式電子顯微鏡(TEM) 以及選區電子繞射(SAED)的觀察發現單層二硫化鉬具有六重對稱的六方晶系以及良好的結晶性質。電性量測方面，單層二硫化鉬場效電晶體為典型的 N-type 半導體，其開關電流比為10000。最後，第六章為此碩士工作的結論以及未來工作。 It was since 2004 that Prof. Andre Geim and Dr. Konstantin Novoselov used mechanical exfoliation method to gain monolayered graphite ---graphene. They have found it has significant electronic behavior and mechanical strength, and opened a route to study the optical and electric behaviors and application of few layered inorganic materials. This study focus on the synthesis of BCN nanosheets via chemical decoration of graphene oxide, hydrothermal exfoliations of boron nitride with the aid of hydrogen peroxide, and the synthesis of few layered structure of molybdenum disulfide by CVD process.In Chapter 1, it is about the basic structure, characteristics and recently progress of graphene, boron carbonitride, boron nitride and molybdenum disulfide nanosheets. In Chapter 2, it is about the experimental sections and investigating instrument. Chapter 3 is about the synthesis of BCN nanosheets, we have successfully doped GO nanosheets with BN via partial substitution of carbon atoms in graphene by boron and nitrogen atoms. Based on the XPS data, the doping concentration of BN increases with the increasing of the reaction temperature. Furthermore, we found that the use of gaseous ammonia allows the doping of graphene allows the doping of graphene with BN to be carried out at the lower temperature. The Raman spectra of the BCN sample synthesized at the various temperatures showed that I(D)/I(G) ratio is proportional to the doping concentration of BN in graphene. Furthermore, the estimate value of graphene nanocrystallite size decreases with the increase in the degree of doping in graphene. Finally, UV spectra of BCN sample with various doping concentration of BN have verified that the band gap of graphene is opened and dependent on atomic composition in nanosheets. For the electrical measurements, we will fabricate the bottom gated field-effect transistors by using the BN-doped graphene. For the studies of BN domain distribution in graphene, we will characterize the BCN samples by using electron energy loss spectroscopy. It is expected that the difference in current between graphene and BN domain can be observed.Chapter 4 is the synthesis of BN nanosheets, we have succesfully decorate BN with OH group via hydrothermal reactions with hydrogen peroxide, and sequentially exfoliated via sonication to gain BN nanosheets. Based on the AFM data, lateral size and height of BN nanosheets decreaes with increasing the reaction temperature.UV spectra of BN nanosheets have verified increased solubility with increased OH group . Finally, we use BN nanosheets to absorb perylene-3,4,9,10-tetracarboxylic acid tetrapotassium salt (PTAS) molecule with π-π interaction and desorption with KOH. We found that with the increase of OH concentration desorption concentration decreases caused by blocking of OH group.Chapter 5 is the synthesis of MoS2 layered structure, large-area MoS2 films are directly synthesized on SiO2/Si substrates with chemical vapor deposition. It is noteworthy that the growth of MoS2 is not unique to SiO2 substrates and it is also observed on other insulating substrates such as sapphire. The as-synthesized films are consisted of monolayer, bilayer and other few-layer MoS2. Chemical configurations, including stoichiometry and valence states of MoS2 layers are confirmed with XPS. Raman spectra and PL performance of the monolayer MoS2 are presented. TEM and SAED demonstrate that the monolayer MoS2 exhibits six-fold symmetry hexagonal lattice and high crystallinity. The electric measurement for the bottom-gate transistor shows a N-type semiconductor behavior and the on-off current ratio is approximately 1 x 104. The seeding approach can be further used to grow other transition metal dichalcogenides. Finally, Chapter 6 is the conclusion and future work.
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