Highly tunable selectivity to benzaldehyde over Pd/ZrO2 catalysts in Oppenauer oxidation of benzyl alcohol using acetone as H-acceptor

被引:12
作者
Akinnawo, Christianah Aarinola [1 ]
Maheso, Dimakatso Jeannett [1 ]
Bingwa, Ndzondelelo [1 ]
Meijboom, Reinout [1 ]
机构
[1] Univ Johannesburg, Res Ctr Synth & Catalysis, Dept Chem Sci, POB 524,Auckland Pk, ZA-2006 Johannesburg, South Africa
基金
新加坡国家研究基金会; 芬兰科学院;
关键词
Mesoporous zirconia; Pd nanoparticles; Oppenauer oxidation; Acid-base sites; Selectivity; Aldol condensation; SOLVENT-FREE OXIDATION; ZRO2; ALDEHYDES; GREEN; NANOPARTICLES; ZEOLITE; OXIDES; SITES;
D O I
10.1016/j.apcata.2021.118022
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The development of novel bifunctional catalysts with high selectivity is the key to achieving the goals of sustainable chemical synthesis. Here, we report the synthesis of mesoporous zirconia and transition metal-doped zirconia by inverse micelle approach. Also, meso-zirconia supported Pd nanocatalysts via the deposition-precipitation method. Highly crystalline Pd/ZrO2 nanoparticles were formed, as evidenced in the pXRD and TEM analyses. The acid-base quantification was investigated using TPD-NH3 and TPD-CO2. Interestingly, the integration of the intrinsic chemical properties of the multi-component catalyst is significant in tailoring the catalytic activities. Interactions between the adsorbates and the moderate acid-base pair sites rather than a single dominating acid or base site mediate the higher selectivity for the aldehyde product. The 100 % chemoselectivity to benzaldehyde is ascribed to the strong synergy between Pd-Zr, which generated the moderate acid-base property. The Pd/ZrO2 is reusable, with selectivity retained after ten cycles.
引用
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页数:11
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