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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
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Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China

Ji, Xialin
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Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China

Xiong, Yongzhi
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Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China

Jiang, Jianchun
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Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China
Chinese Acad Forestry, Inst Chem Ind Forest Prod, Nanjing 210042, Peoples R China Huaqiao Univ, Acad Adv Carbon Convers Technol, Fujian Prov Key Lab Biomass Low Carbon Convers, Xiamen 361021, Peoples R China
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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