期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 227, 期 -, 页码 79-89出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.01.017
关键词
Heterogeneous catalysis; Biofuels; Biomass-derived materials; Self-assembly; Acid-base bifunctionality
资金
- Nanjing Agricultural University [68Q-0603]
- International Postdoctoral Exchange Fellowship Program of China [20170026]
- Postdoctoral Science Foundation of China [2016M600422]
- Jiangsu Postdoctoral Research Funding Plan [1601029A]
The use of organic chemicals derived from renewable sources to synthesize functional solid materials for heterogeneous catalysis is of great significance. Herein, a new porous and acid-base bifunctional hybrid (FDCA-Hf) was designed and prepared by simple assembly of biomass-derived 2,5-furandicarboxylic acid (FDCA) with hafnium (Hf) under template-free conditions. The resulting FDCA-Hf hybrid with mesopores centered at 6.9 nm, moderate surface area (365.8 m(2)/g) and acid-base couple sites (density: 0.51 vs 0.97 mmol/g, acid/base molar ratio: 0.53), could selectively catalyze the Meerwein-Ponndorf-Verley reduction of carbonyl compounds under mild reaction conditions (as low as 90 degrees C in a short time of 1 h), especially of ethyl levulinate to gamma-valerolactone, in quantitative yields (95-100%) and relatively higher reaction rate (e.g., turnover frequency: 2.28 h(-1)) compared to other catalysts. Moreover, the efficient simultaneous (trans)esterification of Jatropha oils with high acidic values to biodiesel (up to 98% yield) could also be achieved over FDCA-Hf with robust acid-base catalytic sites. The FDCA-Hf hybrid was highly stable due to the presence of robust metal-organic framework and could be resued with no decline in activity. Further studies demonstrated that the synergistic role of Lewis acid-base couple species (Hf4+-O2-) and Bronsted acidic species (-OH) of FDCA-Hf contributed greatly to its pronounced catalytic activity.
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