利用理論計算探索含氮烴在 Cu(210) 表面之鍵合性質

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Title:	利用理論計算探索含氮烴在 Cu(210) 表面之鍵合性質 A computational study exploring the bonding nature of nitrogen-containing hydrocarbons on Cu(210) surface
Authors:	蕭淯文 SIAO, YU-WUN
Contributors:	化學工程與材料工程學系
Keywords:	含氮烴 nitrogen-containing hydrocarbons
Date:	2024
Issue Date:	2024-11-14 10:44:18 (UTC+8)
Abstract:	電化學還原二氧化碳反應被視為一種有效減緩溫室效應並且可獲得具有經濟價值的液體燃料以供工業上使用，Cu(210) 是少數能夠將二氧化碳催化還原成具有較高法拉第效率的單碳產物 (CHy)，可以作為本研究中 CHy 碎片的來源。同時，再引入 NHx 之類的含氮親核試劑到催化系統中形成 C-N 鍵，可以促使二氧化碳的還原，並且擴大還原產品的範圍。故在此以 Cu(210) 表面作為實驗基板，透過電子局域化函數 (Electron Localization Function, ELF) 來分析表面電子密度的分布，並且確認七種反應物單吸附在表面上最佳的吸附位置，進而探索催化劑本身對於 C-N 偶聯反應網絡之影響。在16種 C-N 鍵結的部分，觀察到含有 CH2 分子所進行反應，都可以有效降低能障，來促使反應進行。從研究結果指出，C + NH、CH2 + N 和 CH2 + NH 的反應路徑，分別有最低的活化能為 0.49 eV、0.42 eV 和0.44 eV，故可以推測這三種路徑在 Cu(210) 表面上有著極佳的反應性。 Electrochemical reduction of carbon dioxide is regarded as an effective method to mitigate greenhouse gas emissions and produce economically valuable liquid fuels for industrial use. Cu(210) is one of the few surfaces capable of catalyzing the reduction of CO2 to carbon Ce products (CHy) with high Faradaic efficiency, serving as a source of CHy fragments in this study. Additionally, introducing nitrogen-containing nucleophilic reagents like NHx into the catalytic system forms C-N bonds, promoting CO2 reduction and expanding the range of reduction products. Therefore, Cu(210) surface is chosen as the experimental substrate in this study. The surface electron density distribution is analyzed using Electron Localization Function (Electron Localization Function , ELF) to identify optimal adsorption sites for seven reactants on the surface, exploring the catalyst's impact on the C-N coupling reaction network. Among the 16 C-N bond formations studied, reactions involving CH2 molecules consistently lower the activation energy barriers, facilitating the reactions. According to the research findings, the pathways C + NH, CH2 + N, and CH2 + NH exhibit the lowest activation energies of 0.49 eV, 0.42 eV, and 0.44 eV, respectively, indicating excellent reactivity on the Cu(210) surface for these pathways.
Appears in Collections:	[Department of Chemical & Materials Engineering] thesis

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