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

DOI: 10.1038/s41563-019-0562-6 DOI Help

Authors: Longfei Lin (University of Manchester) , Alena M. Sheveleva (University of Manchester; International Tomography Centre SB RAS; Novosibirsk State University) , Ivan Da Silva (ISIS Facility) , Christopher M. A. Parlett (University of Manchester; Diamond Light Source) , Zhimou Tang (East China Normal University) , Yueming Liu (East China Normal University) , Mengtian Fan (University of Manchester) , Xue Han (University of Manchester) , Joseph H. Carter (University of Manchester) , Floriana Tuna (University of Manchester) , Eric J. L. Mcinnes (University of Manchester) , Yongqiang Cheng (Oak Ridge National Laboratory) , Luke L. Daemen (Oak Ridge National Laboratory) , Svemir Rudic (ISIS Facility) , Anibal J. Ramirez-Cuesta (Oak Ridge National Laboratory) , Chiu C. Tang (Diamond Light Source) , Sihai Yang (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Materials , VOL 19 , PAGES 86 - 93

State: Published (Approved)
Published: December 2019
Diamond Proposal Number(s): 15151 , 24726

Abstract: 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.

Journal Keywords: Catalysis; Coordination chemistry; Green chemistry; Materials chemistry; Porous materials

Diamond Keywords: Biofuel

Subject Areas: Materials, Chemistry, Environment

Instruments: B18-Core EXAFS , I11-High Resolution Powder Diffraction

Other Facilities: Oak Ridge National Laboratory (ORNL); ISIS Facility

Added On: 06/01/2020 15:29

Discipline Tags:

Zeolites Bioenergy Earth Sciences & Environment Biotechnology Sustainable Energy Systems Energy Climate Change Physical Chemistry Catalysis Chemistry Engineering & Technology

Technical Tags:

Diffraction Spectroscopy X-ray Powder Diffraction X-ray Absorption Spectroscopy (XAS)