【摘要】：二氧化碳不僅是一種主要的溫室氣體,而且也是最為廉價(jià)易得的C1資源。二氧化碳的綜合利用和減排已成為人類社會(huì)可持續(xù)發(fā)展所面臨的重大機(jī)遇與挑戰(zhàn)。但由于二氧化碳熱力學(xué)上的穩(wěn)定性,使其活化需提供較高能量,因此如何高效地實(shí)現(xiàn)二氧化碳的化學(xué)轉(zhuǎn)化一直是催化與合成領(lǐng)域的一個(gè)具有挑戰(zhàn)性的課題.甲酸不僅是一種重要的有機(jī)化工原料,而且有望作為液體儲(chǔ)氫材料而應(yīng)用于燃料電池。二氧化碳催化氫化制備甲酸已被廣泛研究,其中催化劑是促進(jìn)該反應(yīng)進(jìn)一步發(fā)展的關(guān)鍵。目前對(duì)催化劑的研究主要集中在貴金屬催化劑,而對(duì)第一過渡系金屬催化劑的研究還較少。我們合成了系列三羰基(η4-環(huán)戊二烯酮)鐵絡(luò)合物,并將其成功應(yīng)用到NaHCO3的催化氫化反應(yīng)中制備甲酸鹽。隨后,通過PH值的調(diào)節(jié),我們也成功實(shí)現(xiàn)了CO2的高效催化氫化制備甲酸鹽的反應(yīng)。最后,我們還合成了一種新穎的水溶性的手性鐵絡(luò)合物Ⅱ-4,初步研究發(fā)現(xiàn)該絡(luò)合物可在純水作為溶劑的反應(yīng)條件下催化氫化NaHCO3制備甲酸鹽,盡管其催化活性還有待提高,但該研究為我們進(jìn)一步發(fā)展高效的水溶性鐵氫化催化劑奠定了一定的基礎(chǔ)。甲醇不僅是基礎(chǔ)的有機(jī)化工原料,而且也是重要的燃料之一。鑒于其重要的應(yīng)用前景和價(jià)值,發(fā)展高效合成甲醇的方法具有重要的理論和實(shí)際意義。甲酸酯類衍生物的氫化反應(yīng)是制備甲醇最為重要的方法之一。我們應(yīng)用空氣穩(wěn)定的二羰基(吡啶)(η4-環(huán)戊二烯酮)鐵絡(luò)合物m-3,成功實(shí)現(xiàn)了在溫和反應(yīng)條件下高效催化氫化系列甲酸酯衍生物制備甲醇的反應(yīng)。該研究為我們發(fā)展廉價(jià)催化劑體系于二氧化碳直接催化氫化制備甲醇奠定了重要的基礎(chǔ)。
[Abstract]:Carbon dioxide is not only a major greenhouse gas, but also the cheapest and most readily available C1 resource. The comprehensive utilization and emission reduction of carbon dioxide has become a great opportunity and challenge for the sustainable development of human society. However, due to the thermodynamic stability of carbon dioxide, it is necessary to provide high energy for its activation. Therefore, how to efficiently realize the chemical conversion of carbon dioxide has always been a challenging task in the field of catalysis and synthesis. Formic acid is not only an important organic chemical material, but also is expected to be used as a liquid hydrogen storage material in fuel cells. The catalytic hydrogenation of carbon dioxide to formic acid has been widely studied, among which catalyst is the key to promote the further development of the reaction. At present, the research on catalyst is mainly focused on precious metal catalyst, but the research on first transition metal catalyst is less. A series of tricarbonyl (畏 4-cyclopentadienone) iron complexes were synthesized and successfully applied to the catalytic hydrogenation of NaHCO3 to prepare formate. Subsequently, we successfully realized the catalytic hydrogenation of CO2 to formate by adjusting PH value. Finally, we also synthesized a novel water-soluble chiral iron complex 鈪，

本文編號(hào)：2453856