Ni/Ce co-doping metal-organic framework catalysts with oxygen vacancy for catalytic transfer hydrodeoxygenation of lignin derivatives vanillin

被引:30
作者
Chen, Changzhou [1 ]
Ji, Xialin [1 ]
Xiong, Yongzhi [1 ]
Jiang, Jianchun [1 ,2 ]
机构
[1] Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China
[2] Chinese Acad Forestry, Inst Chem Ind Forest Prod, Nanjing 210042, Peoples R China
关键词
Metal -organic framework; Vanillin; Hydrodeoxygenation; 2-methoxy-4-methylphenol; NI; CARBON; HYDROTREATMENT; EFFICIENT; BIOMASS;
D O I
10.1016/j.cej.2024.148555
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Exploring an advanced catalytic strategy for the high value utilization of lignin derived chemicals into value-added aromatics has attracted tremendous sights for green manufacturing. In this paper, a series of bifunctional 3D rod-shaped mesoporous NiCe metal-organic framework catalysts coupling with hydrogen-donner solvent were reported for the hydrodeoxygenation of vanillin to obtain 2-methoxy-4-methylphenol. Under the optimal conditions, 3Ni-Ce/C catalyst realized the highest conversion of vanillin (>95.0%) and selectivity of 81.4%. The characterization results indicated that the interaction of metallic Ni and CeO2 promoted the generation of Ni-CeO2-x interface and oxygen vacancies (Ov), which could efficiently adsorb and activate aldehyde group of vanillin to obtain reactive intermediates. And then metallic Ni sites activated the hydrogen-donner solvent to form adsorbed H atoms, which then spilled over to the adjacent Ov to stabilized reactive intermediates. Whereafter, bifunctional 3D rod-shaped mesoporous NiCe metal-organic framework catalysts achieved the hydrodeoxygenation upgrading of vanillin to obtain 2-methoxy-4-methylphenol. Density functional theory (DFT) calculations further revealed that the synergistic effect of Ni-CeO2 and oxygen vacancies promoted the activation and dissociation of aldehyde group bond in vanillin, enhanced the ability of protonation hydrogenolysis. Additionally, 3Ni-Ce/C catalyst displayed robust activity for no less than four recycles, which provided a feasible method for the build of simultaneous utilization of lignin derivates to value-added fuels and chemicals.
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页数:16
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