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Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite.

Longfei LinAlena M ShevelevaFabian HesseChristopher M A ParlettZhimou TangYueming LiuMengtian FanXue HanJoseph H CarterFloriana TunaEric J L McInnesYongqiang ChengLuke L DaemenSvemir RudićAnibal J Ramirez-CuestaChiu C TangSihai Yang
Published in: Nature materials (2019)
The efficient production of light olefins from renewable biomass is a vital and challenging target to achieve future sustainable chemical processes. Here we report a hetero-atomic MFI-type zeolite (NbAlS-1), over which aqueous solutions of γ-valerolactone (GVL), obtained from biomass-derived carbohydrates, can be quantitatively converted into butenes with a yield of >99% at ambient pressure under continuous flow conditions. NbAlS-1 incorporates simultaneously niobium(V) and aluminium(III) centres into the framework and thus has a desirable distribution of Lewis and Brønsted acid sites with optimal strength. Synchrotron X-ray diffraction and absorption spectroscopy show that there is cooperativity between Nb(V) and the Brønsted acid sites on the confined adsorption of GVL, whereas the catalytic mechanism for the conversion of the confined GVL into butenes is revealed by in situ inelastic neutron scattering, coupled with modelling. This study offers a prospect for the sustainable production of butene as a platform chemical for the manufacture of renewable materials.
Keyphrases
  • high resolution
  • wastewater treatment
  • electron microscopy
  • anaerobic digestion
  • current status
  • air pollution
  • high throughput
  • magnetic resonance imaging
  • single molecule