铁催化二氧化碳和甲酸酯衍生物的氢化反应研究
发布时间：2019-04-04 13:20
【摘要】：二氧化碳不仅是一种主要的温室气体,而且也是最为廉价易得的C1资源。二氧化碳的综合利用和减排已成为人类社会可持续发展所面临的重大机遇与挑战。但由于二氧化碳热力学上的稳定性,使其活化需提供较高能量,因此如何高效地实现二氧化碳的化学转化一直是催化与合成领域的一个具有挑战性的课题.甲酸不仅是一种重要的有机化工原料,而且有望作为液体储氢材料而应用于燃料电池。二氧化碳催化氢化制备甲酸已被广泛研究,其中催化剂是促进该反应进一步发展的关键。目前对催化剂的研究主要集中在贵金属催化剂,而对第一过渡系金属催化剂的研究还较少。我们合成了系列三羰基(η4-环戊二烯酮)铁络合物,并将其成功应用到NaHCO3的催化氢化反应中制备甲酸盐。随后,通过PH值的调节,我们也成功实现了CO2的高效催化氢化制备甲酸盐的反应。最后,我们还合成了一种新颖的水溶性的手性铁络合物Ⅱ-4,初步研究发现该络合物可在纯水作为溶剂的反应条件下催化氢化NaHCO3制备甲酸盐,尽管其催化活性还有待提高,但该研究为我们进一步发展高效的水溶性铁氢化催化剂奠定了一定的基础。甲醇不仅是基础的有机化工原料,而且也是重要的燃料之一。鉴于其重要的应用前景和价值,发展高效合成甲醇的方法具有重要的理论和实际意义。甲酸酯类衍生物的氢化反应是制备甲醇最为重要的方法之一。我们应用空气稳定的二羰基(吡啶)(η4-环戊二烯酮)铁络合物m-3,成功实现了在温和反应条件下高效催化氢化系列甲酸酯衍生物制备甲醇的反应。该研究为我们发展廉价催化剂体系于二氧化碳直接催化氢化制备甲醇奠定了重要的基础。
[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，
本文编号：2453856
[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，
本文编号：2453856
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