2018-01-012024-05-17https://scholars.lib.ntu.edu.tw/handle/123456789/674049摘要：將可再生及廢棄資源以綠色製程循環再生成高值化材料已成為台灣社會永續發展的重要課題。本計畫擬透過關鍵觸媒的研發，開發以二氧化碳(可再生資源)及醇類(如廢甘油，生質柴油的副產物)作為原料的低能耗且低成本碳酸酯綠色製程。在反應熱力學限制及反應物物化性質的考量下，本計畫將著重研究碳酸酯製程中的兩個核心催化反應─(1)氣相催化二氧化碳及醇類(甲醇或乙醇)反應生成碳酸烷基酯(副產物為水)，及(2)液相催化甘油(丙三醇)及碳酸烷基酯轉酯化生成碳酸甘油酯(副產物為醇類─可循環使用)。本研究將設計製備多功能酸鹼混合金屬氧化物觸媒，期望透過調節表面酸鹼活性基的強度與密度，及控制表面結構如比表面積、孔洞大小及方向分佈等方式提升碳酸酯產率；並輔以原位光譜分析技術建立觸媒催化表現及表面性質間的直接關聯性作為觸媒的改良依據。本計畫將整合觸媒化學、表面科學及反應工程等專業知識，致力於將二氧化碳及醇類在接近常溫常壓下轉換生成用途廣泛且富經濟價值的碳酸酯。預期執行本研究將可促進相關循環材料的再利用技術，及推動相關化工產業的製程轉型─對天然資源缺乏且人均二氧化碳排放量高的台灣在經濟、產業及環境保護上有所貢獻。<br> Abstract: Converting renewable and waste resources via green chemistry processes　circularly into value-added materials has been an important topic for　sustainable development of Taiwan society. This research project aims　at developing catalysts for green, energy-efficient, cost-effective synthesis processes of carbonate esters from carbon dioxide (a renewable　resource) and alcohols (e.g., waste glycerol, a by-product of biodiesel　synthesis). Considering the thermodynamic limitation of reactions and　physiochemical properties of reactants, this research project will focus　on two catalytic reactions in the synthesis processes of carbonate esters: (1) gas-phase catalysis of carbon dioxide and alcohols (methanol　and ethanol) to form dialkyl carbonates (with water as by-product), and　(2) liquid-phase catalytic transesterification between glycerol and　dialkyl carbonate to form glycerol carbonate (with methanol as byproduct,　which can be recycled for later use). We will design and　synthesize multifunctional acid-base mixed-metal-oxide catalysts to　increase carbonate ester yields through the strength and density　adjustment of acidic and basic sites on the surface, and the control of　surface structures such as specific surface area, and pore　size/orientation distributions. We will also perform in-situ　spectroscopy analyses to establish direct correlations between catalytic　performance and surface properties, and then use them as a guideline to　improve our catalysts. We will integrate our expertise of catalyst chemistry, surface science, and reaction engineering to engage in　converting carbon dioxide and alcohols into versatile and value-added　carbonate esters under near-ambient conditions. The implementation of　this project is expected to advance the reutilization technologies of related recycled materials, and to promote the process reorganization of　related chemical industries, by which make contributions to Taiwan,　where the natural resources are scarce and per capita CO2 emission is　high, on the economics, industries, and environmental protection.二氧化碳甘油碳酸酯綠色製程異相酸鹼觸媒carbon dioxideglycerolcarbonate estergreen chemistry processheterogeneous acid-base catalyst