Journal
CHEMCATCHEM
Volume 12, Issue 1, Pages 350-359Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201901435
Keywords
Heterogeneous catalyst; Amphoteric oxide; Lewis acid-base pair; Biomass conversion
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Funding
- Advanced Low Carbon Technology Research and Development Program (ALCA) [JPMJAL1507]
- Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials in Network Joint Research Center for Materials and Devices
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Amphoteric YNbO4 was synthesized by the simple coprecipitation using (NH4)(3)[Nb(O-2)(4)] and Y(NO3)(3), and examined as a new solid acid-base bifunctional catalyst for various reactions including aqueous-phase conversion of glucose to lactic acid. After drying the white precipitate at 353 K for 3 h, the resultant oxide is an amorphous YNbO4 with high densities of Lewis acid sites (0.18 mmol g(-1)) and base sites (0.38 mmol g(-1)). Negatively-charged lattice oxygen of amorphous YNbO4 functioned as Lewis base sites that promote a Claisen-Schmidt-type condensation reaction with acetylacetone and benzaldehyde with comparable activity to reference catalysts. Amorphous YNbO4 can also be applicable to the production of lactic acid from glucose in water, which gives relatively high yields (19.6 %) compared with other reference catalysts. Mechanistic studies using glucose-1-d and H-2 nuclear magnetic resonance spectroscopy (NMR) revealed that YNbO4 first converts glucose to two carbohydrates (glyceraldehyde and pyruvaldehyde) through dehydration via the formation of 3-deoxyglucosone and subsequent retro-aldolization, and these intermediates are then converted to lactic acid by both dehydration and isomerization through hydride transfer.
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