以理論計算的方式探索費托反應於各種基底負載銠奈米團簇的產物選擇性

文化大學機構典藏 CCUR > 理工學院 > 工學院 > 化學工程與材料工程學系暨碩士班 > 博碩士論文 > Item 987654321/53030

jsp.display-item.identifier=請使用永久網址來引用或連結此文件: https://irlib.pccu.edu.tw/handle/987654321/53030

题名:	以理論計算的方式探索費托反應於各種基底負載銠奈米團簇的產物選擇性 Modulation of Fischer-Tropsch Product Selectivity via Various Substrates Supported Rhodium Nanoclusters-A DFT Study
作者:	莊宇文
贡献者:	化學工程與材料工程學系
关键词:	理論計算費托反應銠奈米團簇 Fischer-Tropsch Rhodium Nanoclusters ZSM-5 MCM4
日期:	2023
上传时间:	2024-02-23 14:46:03 (UTC+8)
摘要:	一氧化碳有潛力成為通過費-托合成 (FTS) 生產碳氫化合物的替代原油原料。 CO 和 H2 已被用於通過基於Rh 的奈米催化劑有效合成碳氫化合物。不幸的是，如果團簇沒有支撐在基材上，過小的奈米團簇 (原子顆數≤ 20) 的結構將難以定義。並且Rh 奈米團簇在不同載體上的催化活性會明顯不同，因為團簇和載體之間會形成相互作用，這取決於相互作用是產生正向的影響還是負面之影響。因此我們研究了Rh4 奈米團簇與不同負載物之間的穩定性，並進一步討論了負載物對催化效果的影響。本研究通過 DFT 計算研究了Rh4 奈米團簇接上不同載體，載體為石墨烯(Graphene)、沸石 (ZSM-5)和介孔分子篩(MCM-41)。我們以費托合成出 CHx 形式的反應機理。我們研究了CHxO (x = 1, 2, 3)、CH4、CH3OH，在Rh4 以石墨烯為載體、Rh4 以沸石為載體和 Rh4 以介孔分子篩為載體中，氫對輔助解離生成特定CHx 片段的反應選擇性。此外，我們還通過電子分析進一步了解了CHx 片段是如何被不同的載體選擇性穩定的。最後我們希望通過仔細篩選適當的載體來改變 Rh4 奈米團簇的活性，以幫助開發高選擇性費托合成催化劑，從而實現最佳之能量屏障。 Carbon monoxide is a promising alternative crude oil feedstock for producing hydrocarbons via Fischer-Tropsch synthesis (FTS). Rh-based nanocatalysts have been found to efficiently synthesize hydrocarbons from CO and H2. However, the conformation of small nanoclusters (N â¤ 20) is difficult to define without substrate support. The catalytic activity of Rhnanoclusters on different supports varies significantly due to varied interactions between cluster and support, inducing either a positive or negative effect. Therefore, this study investigates the stability of Rh4 nanoclusters on different supports and their influence on catalytic effects. Using DFT calculations, we systematically study the reaction mechanism of CHx formation in Fischer-Tropsch synthesis on Rh4@Supported (Supported = ZSM-5, and MCM-41) and investigate the selectivity of the hydrogen-assisted dissociation of CHxO (x = 1 ~ 4) on Rh4@ZSM-5, and Rh4@MCM-41 to generate specific CHx fragments. Additionally, we analyze how different Rh4@Supported selectively stabilize CHx fragments through electronic analysis. Ultimately, our goal is to identify the proper support to optimize the activity of Rh4 nanoclusters and develop high selectivity FTS catalysts with an optimal barrier. Based on our findings, Rh4@MCM-41 exhibits the highest selectivity among the chosen Rh4@Supported catalysts. This is due to the superior stability of *CHx (x= 3, 4) fragments on this catalyst, making it an excellent candidate for use in Fischer-Tropsch synthesis. We believe that these results have important implications for the development of high-performance FTS catalysts and suggest that Rh4@MCM-41 should be further investigated as a potential catalyst for industrial applications.
显示于类别:	[化學工程與材料工程學系暨碩士班] 博碩士論文

文件中的档案:

档案	描述	大小	格式	浏览次数
index.html		0Kb	HTML	79	检视/开启

检视Licence

在CCUR中所有的数据项都受到原著作权保护.

数据加载中.....