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Hydrodeoxygenation of Lignin-Derived Phenolic Monomers and Dimers to Alkane Fuels over Bifunctional Zeolite-Supported Metal Catalysts

机译:木质素衍生的酚醛单体和二聚体在双功能沸石负载的金属催化剂上加氢脱氧为烷烃燃料

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摘要

A bifunctional catalyst of Ru supported in zeolite HZSM-5, Ru/HZSM-5 (Si/Al = 25), exhibited excellent hydrodeoxygenation activity toward the conversion of lignin-derived phenolic monomers and dimers to cycloalkanes in aqueous solution. The oxygen-containing groups in mono- and binuclear phenols were removed through a cleavage of C-O bonds in phenolics followed by an integrated metal- and acid-catalyzed hydrogenation and dehydration. As a bifunctional catalyst Ru/HZSM-5, the presence of both the Br?nsted acid site in the pores of HZSM-5 for dehydration and a metallic function of Ru for hydrogenation was indispensible for the formation of alkanes from lignin-derived phenolics. Our findings also reveal that the Ru/HZSM-5 with the lowest Si/Al ratio of HZSM-5 proved to be most selective to cycloalkanes, indicating that more acid sites over zeolite are favorable for the dehydration of cyclohexanol during hydrodeoxygenation process, which leads higher selectivity to hydrocarbons. This approach for the construction of bifunctional catalyst highlights an efficient route for hydrodeoxygenation of lignin-derived phenolic oil to transportation biofuels.
机译:负载在沸石HZSM-5中的Ru的双功能催化剂Ru / HZSM-5(Si / Al = 25)对水溶液中木质素衍生的酚类单体和二聚体向环烷烃的转化表现出优异的加氢脱氧活性。通过裂解酚醛中的C-O键,然后进行整体的金属和酸催化的加氢和脱水作用,可以除去单核和双核酚中的含氧基团。作为双功能催化剂Ru / HZSM-5,HZSM-5孔中存在布朗斯台德酸位点以进行脱水,Ru的金属官能团用于氢化是从木质素衍生的酚类化合物形成烷烃所必需的。我们的发现还表明,具有最低HZSM-5硅/铝比的Ru / HZSM-5被证明对环烷烃具有最高的选择性,表明沸石上更多的酸位有利于加氢脱氧过程中环己醇的脱水,这导致对烃的选择性更高。这种构造双功能催化剂的方法突显了木质素衍生的酚油加氢脱氧以运输生物燃料的有效途径。

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