MoVO/P-AC催化剂组成调控及其在甘油气相高值化转化中的应用

Composition Regulation of MoVO/P-AC Catalyst and Its Application In High Value Transformation of Petroleum and Gas Phase

甘油是重要的生物质平台化合物之一,其制取高附加值丙烯醛、丙烯醇等工艺开发有助减少石化资源的利用和碳排放。本文以磷酸处理的活性炭(AC)为载体,采用过量浸渍法制备MoVO/P-AC(Cat^(x),x=Mo∶V,n∶n)催化剂用于甘油气相脱水反应中,并采用BET、XRD、XPS、H_(2)-TPR和NH 3-TPD对催化剂物理化学性质进行表征。结果表明:Cat^(x)主要存在于高分散的MoO_(3)-V_(2)O_(5)和(VO)_(2)P_(2)O_(7)中,且与P-AC载体之间存在强相互作用,Cat^(x)表面仅存在弱酸和中强酸中心;Mo/V用量调控了Cat^(x)中活性组分间的协同作用、氧化还原能力和酸性强度。Cat^(x)对甘油催化转化性能(丙烯醛、丙烯醇和乙醛的收率)高低顺序为:Cat^(5.0)>Cat^(4.0)>Cat^(6.0)>Cat^(3.0)>Cat^(2.0)。310℃反应时,Cat^(5.0)上甘油的转化率达到85.9%,丙烯醛、丙烯醇的选择性分别为51.8%、10.5%,且展现出较好的再生性,为甘油制丙烯醛和丙烯醇高性能催化剂开发提供理论基础和依据。

Glycerin is one of the important biomass platform compounds,and the development of processes for producing high value-added acrolein and propylene alcohol can help reduce the utilization of petrochemical resources and carbon emissions.This article use activated carbon(AC)treated with phosphoric acid as the carrier and excessive impregnation method to prepare MoVO/P-AC(Cat^(x),x=Mo∶V,n∶n)catalyst for glycerol gas phase dehydration reaction.The physical and chemical properties of the catalyst are characterized by using BET,XRD,XPS,H 2-TPR and NH 3-TPD.The results showed that Cat^(x)mainly contain highly dispersed MoO_(3)-V_(2)O_(5)and(VO)_(2)P_(2)O_(7),and there was a strong interaction with P-AC support.Cat^(x)only had weak and medium strong acid centers on its surface.The amount of Mo/V regulated the synergistic effect,redox ability,and acidic strength between the active components in Cat^(x).The catalytic conversion performance of Cat^(x)for glycerol(yield of acrolein,propanol and acetaldehyde)was in the order of Cat^(5.0)>Cat^(4.0)>Cat^(6.0)>Cat^(3.0)>Cat^(2.0)at 310℃,the conversion rate of glycerol on Cat^(5.0)reached 85.9%,the selectivity of acrolein,allyl alcohol were 51.8%and 10.5%,respectively,showing good regeneration performance,provide theoretical basis and basis for the development of high-performance catalysts for glycerol to acrolein and propylene alcohol production.