基于二维催化剂电子密度调控的乙醇氢转移选择性加氢餐厨油脂的机理及应用

餐厨油脂的资源化利用可促进我国循环经济的可持续发展。油脂通过选择性加氢可制备烃类柴油或脂肪醇，然而，目前对油脂选择性加氢的机理还未有深入的研究；且该反应需在无水、高温和高压的条件下进行。我们前期的研究显示：1）通过改变负载金属的电子密度，可调控反应体系中氢气的活化裂解方式，实现油脂选择性加氢为烃类柴油或脂肪醇；2）生物质醇氢转移获得的氢源活性高于生物质醇水相重整的氢源活性。基于此，本项目将以乙醇氢转移为原位氢源，引入二维材料负载的金属原子级分散催化剂，通过改变二维载体的结构性质，调变负载金属的电子密度，从而影响乙醇的活化裂解方式，最终实现在温和的反应条件下，清洁高效地将高含水量的餐厨油脂催化转化为烃类柴油或脂肪醇。本项目的顺利实施将有助于理解乙醇的低温活化制氢机理，及其在原位选择性加氢中的作用，还将为其他生物质选择性加氢转化为高附加值产物提供实验和理论支持。

The upgrading and utilization of waste kitchen oils can promote the sustainable development of China's recycling economy. Selective hydrogenation of oils can produce diesel-range hydrocarbons or fatty alcohols. However, the mechanism of selective hydrogenation of oils has not been thoroughly studied at present, and the reactions need to be carried out under anhydrous, high temperature and high pressure conditions. Our previous research shows that: 1) By changing the electron density of supported metals, the activation and dissociation of hydrogen in the reaction system can be adjusted to achieve the selective hydrogenation of oils into diesel-range hydrocarbons or fatty alcohols; 2) The activity of hydrogen species derived from the hydrogen transfer of bio-alcohols is higher than that from the aqueous phase reforming of bio-alcohols. Based on these, this project will adopt the hydrogen transfer of ethanol as an in-situ hydrogen source, and two-dimensional materials supported atom-level dispersed metals as catalysts. By changing the structural properties of the two-dimensional supports, the electron density of the supported metals can be adjusted, thereby affecting the modes of ethanol activation and dissociation. This finally results in the production of diesel-range hydrocarbons or fatty alcohols from waste kitchen oils with high water content under mild reaction conditions in a clean and efficient way. The successful implementation of this project will help to understand the mechanism of the low-temperature activation of ethanol for hydrogen production as well as its role in the in-situ selective hydrogenation reactions. It will also provide an experimental and theoretical basis for upgrading of other biomass into high value-added products by selective hydrogenation.