加氢脱氧
氢解
催化作用
化学
木质素
脱氢
选择性
有机化学
酒
作者
Haichuan Zhang,Yang Liu,Shiyu Fu,Yulin Deng
标识
DOI:10.1016/j.ijbiomac.2020.12.092
摘要
Upgrading of lignin derived bio-oil is an essential step for producing sustainable bio-based chemicals and fuel. Taken into account that α hydroxyl is the abundant functional group in lignin, high effective and selective catalytic alcoholysis for cleaving the Cα-OH linkages would be desirable. However, an in-depth understanding of the reaction mechanisms involved in the cleavage of Caromatic-Cα and Cα-O bonds over a novel catalyst is still needed. Herein, we report an efficient liquid-phase hydrogen transfer strategy for the selective hydrodeoxygenation of a non-phenolic lignin model compound, 3,4-dimethoxybenzyl (veratryl) alcohol, under mild conditions. By employing iso-propanol as solvent and H-donor, and palladium nanoparticles immobilized on nitrogen-doped carbon (Pd/CNX) as efficient multifunctional catalyst, veratryl alcohol dehydroxylation exhibited almost 100% conversion along with very high selectivity for 1,2-dimethoxy-benzene (46%) and 3,4-dimethoxytoluene (54%). Compared with other Pd catalysis, the Pd/CNX has excellent catalytic performances and exhibits higher selectivity for 3,4-dimethoxytoluene under incorporation with 1% HCOOH at 220 °C. The proportion of Pd (0) significantly increases in Pd/CNX catalyst when introduced into N precursor because of its highly dispersed Pd NPs and preventing the reoxidation of Pd (0). The dehydrogenation reaction occurred through the hydrogen generation of a secondary alcohol. Then, the Cα-OH and Caromatic-Cα bonds of veratryl alcohol were selectively cleaved by catalytic transfer hydrogenolysis. The alcoholysis mechanism is supported by dispersion-corrected density functional theory computations.
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