2020-01-012024-05-18https://scholars.lib.ntu.edu.tw/handle/123456789/699575摘要：二氧化碳是具化學惰性的分子，將二氧化碳轉換為更複雜的化學結構常常需要親核、高能量或過渡金屬試劑。此外，嚴苛的反應條件，如高溫及高壓，也常需使用。美國化學會預估許多過渡金屬在一百年內將面臨含量不足或用盡的可能性。因此，開發地球含量豐富的試劑於溫和的反應條件下來進行二氧化碳官能基化有其研究的必要性。在此計畫中，我們會釐清現存的二氧化碳偶合反應的工作原理並進一步開發新型態的反應，以擴充合成上的多樣性。預計研究的反應包含α氨基酸的合成、丙烯酸的合成、草酸的合成、及水楊酸的合成。於這些合成反應中，單電子轉移機制會是主要的使用方式。密度泛函理論計算亦會採用來探討反應機制及協助尋找於二氧化碳偶合反應有活性的反應試劑。我們預估所取得的知識及技術不僅具有學術上的價值亦有工業上的應用性。<br> Abstract: CO2 is a chemically inert molecule. The conversion of CO2 into complex structures often require nucleophilic, high-energy, or transition metal-based reagents. Moreover, harsh conditions, such as high temperature and pressure, are also involved. American chemical society estimates that many transition metals are faced with limited availability, rising threat, or serious threat in the next 100 years. Therefore, to develop the CO2 functionalization by the use of earth-abundant reagents, such as carbon or iron-based molecules, under mild reaction conditions appears to be a promising approach. In this proposal, we aim at investigating the existing CO2 coupling reactions and expanding the synthetic applicability to access to other substances. The CO2 coupling reactions include synthesis of α-amino acids, synthesis of acrylic acid, synthesis of oxalic acid, and synthesis of salicylic acid. Single electron transfer is the primary tactic in the syntheses. DFT calculations will be carried out to look into the reaction mechanism and assist in finding suitable reagents being active in the CO2 coupling reactions. It is envisaged that the acquired knowledge and techniques will be not only academically intriguing, but also industrially applicable.二氧化碳轉化偶合反應地球含量豐富的試劑密度泛函理論計算單電子轉移CO2 conversioncoupling reactionearth-abundant reagentDFT calculationssingle electron transfer