Defect-rich ZrO2 anchored Pd nanoparticles for selective hydrodeoxygenation of bio-models at room temperature

Defect-rich ZrO2 anchored Pd nanoparticles catalysts were prepared for selective hydrodeoxygenation of bio-models at room temperature. The excellent HDO performance of this catalyst originates from the formation of Zr3+-O-Zr4+ structure. The oxygen vacancies not only promote the adsorption and activ...

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Bibliographic Details
Published in:Fuel (Guildford) 2022-06, Vol.318, p.123529, Article 123529
Main Authors: Jiang, Jingyun, Ding, Wentao, Zhang, Wei, Li, Hao
Format: Article
Language:English
Subjects:
Catalysts
Cetyltrimethylammonium bromide
CTAB
Electronic structure
Energy shortages
Hydrodeoxygenation
Hydrogenolysis
Nanoparticles
Oxygen
Oxygen vacancy
Palladium
Reagents
Room temperature
Selectivity
Vacancies
Vanillin
Zirconium
Zirconium dioxide
Zr3+-Ov-Zr4+ structure
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Summary:Defect-rich ZrO2 anchored Pd nanoparticles catalysts were prepared for selective hydrodeoxygenation of bio-models at room temperature. The excellent HDO performance of this catalyst originates from the formation of Zr3+-O-Zr4+ structure. The oxygen vacancies not only promote the adsorption and activation of carbonyl oxygen, but also modulate the surface electronic structure of metallic palladium and zirconium, where electron-rich Pd can efficiently adsorb and activate hydrogen to promote the hydrogenation process; the presence of Zr3+ provides the required acidic sites for the deoxygenation process. [Display omitted] •Preparation of defect-rich ZrO2 anchored Pd nanoparticles.•Efficient catalytic hydrodeoxygenation of vanillin to MMP at room temperature.•The formation of Zr3+ provided acidic sites for the deoxygenation process.•Investigated the mechanism of efficient catalytic vanillin HDO by Zr3+-Ov-Zr4+ structure. The hydrodeoxygenation (HDO) of biomass-derived compounds into high-quality fuels and chemicals is an effective solution to the fossil energy shortage. However, the development and design of catalysts with high-performance HDO under mild reaction conditions is a significant challenge. In this paper, the defect-rich ZrO2 anchored Pd nanoparticles was investigated for selective HDO of bio-models at room temperature. The oxygen vacancies of Pd/ZrO2(x) catalysts can be regulated by the addition of template agent cetyltrimethylammonium bromide (CTAB), in which CTAB combines with OH on the support to form complex oxides and then promoting the formation of Zr3+-Ov-Zr4+ structure of the as-prepared Pd/ZrO2(x) catalysts. When the mass ratio of CTAB/ZrOSO4 is 0.5, the Pd/ZrO2(0.5) catalyst with the highest oxygen defect content exhibits excellent performance towards 99.9% yield of 2-methoxy-4-methylphenol (MMP) at 25 °C for one hour in vanillin HDO. The rich oxygen vacancies of Pd/ZrO2(x) catalysts can regulate the electronic structure of the catalyst surface metal palladium and zirconium, and promote the adsorption and hydrogenolysis of C-O in vanillin HDO. In addition, it is obviously that the catalysts had excellent versatility and stability, and the MMP selectivity of the Pd-ZrO2(0.5) catalyst slightly decreased after five consecutive reactions.
ISSN:0016-2361
1873-7153
DOI:10.1016/j.fuel.2022.123529