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標題: | 硼陽離子催化硼烷氨脫氫聚合反應 Dehydrogenation and Polymerization of Ammonia-borane Using Boron Cations |
作者: | Wei-An Yen 顏瑋恩 |
指導教授: | 邱靜雯(Ching-Wen Chiu) |
關鍵字: | 硼烷氨,脫氫反應,硼陽離子, ammonia-borane,dehydrogenation,polyborazylene,boron cations, |
出版年 : | 2020 |
學位: | 碩士 |
摘要: | 硼烷氨(NH3BH3)在常溫、常壓下是一種固體,因含氫重量百分率高達19.5 %,可作為優良的儲氫材料。此外,硼烷氨也是常見的有機合成氫化反應的氫氣來源。然而,要將硼烷氨中的氫氣釋放出來,並非輕而易舉之事,所有在100 oC以下釋放氫氣的反應都需要催化劑的參與,除了傳統上使用以過渡金屬為主的催化劑,近期研究亦指出硼烷氨的分解反應可使用主族元素為主的催化劑,如:P/Al乃至於P/B受阻路易士酸鹼對(Frustrated Lewis Pairs),更甚者,脫氫反應可在無路易士鹼的參與下進行,具有高度酸性的二硼烷化合物及反應中即時產生的硼陽離子皆能催化釋氫過程。為了驗證硼陽離子在硼烷氨脫氫反應中的應用,吾人製備了一系列的硼陽離子並研究其催化活性。除氫氣之外,我們也分離並鑑定了其脫氫副產物——polyborazylene。 Ammonia-borane (AB, NH3BH3), a solid molecule under ambient condition, is one of the promising hydrogen storage materials because of its high hydrogen content of 19.5 w/w %. Besides, ammonia-borane can also be utilized as a hydrogen source for organic synthesis. However, the release of hydrogen from ammonia-borane at temperature lower than 100 oC requires the use of catalysts. In addition to the transition-metal-based catalysts, recent studies demonstrated that dehydrogenation of ammonia-borane could be catalyzed by P/Al and P/B Frustrated Lewis Pairs (FLP). Interestingly, the dehydrogenation could even be triggered in the absence of Lewis base. Highly acidic diborane compound and the in-situ generated boronium cation could also catalyze the H2 release process. To probe the potential application of boron cations in dehydrogenation of ammonia-borane, we have examined a series of boron cations and dications for ammonia-borane dehydrogenation application. The dehydrogenation efficiency of boron cations is summarized and the resulting BN-containing byproducts polyborazylene are also isolated and characterized. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/59073 |
DOI: | 10.6342/NTU202003450 |
全文授權: | 有償授權 |
顯示於系所單位: | 化學系 |
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