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

Longfei Lin; Alena Sheveleva; Ivan da Silva; Christopher Parlett; Zhimou Tang; Yueming Liu; Mengtian Fan; Xue Han; Joseph Carter; Floriana Tuna; Eric Mcinnes; Yongqiang Cheng; Luke L  Daemen; Svemir Rudic; Anibal J Ramirez-Cuesta; Chiu C Tang; Sihai Yang

doi:10.1038/s41563-019-0562-6

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

Longfei Lin, Alena Sheveleva, Ivan da Silva, Christopher Parlett, Zhimou Tang, Yueming Liu, Mengtian Fan, Xue Han, Joseph Carter, Floriana Tuna, Eric Mcinnes, Yongqiang Cheng, Luke L Daemen, Svemir Rudic, Anibal J Ramirez-Cuesta, Chiu C Tang, Sihai Yang

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Abstract

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 to 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 Brønsted acid sites on confined adsorption of GVL, while the catalytic mechanism for conversion of confined GVL to 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.

Original language	English
Pages (from-to)	86-93
Journal	Nature Materials
Volume	19
DOIs	https://doi.org/10.1038/s41563-019-0562-6
Publication status	Published - 16 Dec 2019

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Lin, L., Sheveleva, A., Silva, I. D., Parlett, C., Tang, Z., Liu, Y., Fan, M., Han, X., Carter, J., Tuna, F., Mcinnes, E., Cheng, Y., Daemen, L. L., Rudic, S., Ramirez-Cuesta, A. J., Tang, C. C., & Yang, S. (2019). Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite. Nature Materials, 19, 86-93. https://doi.org/10.1038/s41563-019-0562-6

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

abstract = "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 to 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 Br{\o}nsted acid sites with optimal strength. Synchrotron X-ray diffraction and absorption spectroscopy show that there is cooperativity between Nb(V) and Br{\o}nsted acid sites on confined adsorption of GVL, while the catalytic mechanism for conversion of confined GVL to 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. ",

author = "Longfei Lin and Alena Sheveleva and Silva, {Ivan da} and Christopher Parlett and Zhimou Tang and Yueming Liu and Mengtian Fan and Xue Han and Joseph Carter and Floriana Tuna and Eric Mcinnes and Yongqiang Cheng and Daemen, {Luke L} and Svemir Rudic and Ramirez-Cuesta, {Anibal J} and Tang, {Chiu C} and Sihai Yang",

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doi = "10.1038/s41563-019-0562-6",

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journal = "Nature Materials",

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publisher = "Springer Nature",

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Lin, L, Sheveleva, A, Silva, ID, Parlett, C, Tang, Z, Liu, Y, Fan, M, Han, X, Carter, J, Tuna, F , Mcinnes, E, Cheng, Y, Daemen, LL, Rudic, S, Ramirez-Cuesta, AJ, Tang, CC & Yang, S 2019, 'Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite', Nature Materials, vol. 19, pp. 86-93. https://doi.org/10.1038/s41563-019-0562-6

TY - JOUR

T1 - Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite

AU - Lin, Longfei

AU - Sheveleva, Alena

AU - Silva, Ivan da

AU - Parlett, Christopher

AU - Tang, Zhimou

AU - Liu, Yueming

AU - Fan, Mengtian

AU - Han, Xue

AU - Carter, Joseph

AU - Tuna, Floriana

AU - Mcinnes, Eric

AU - Cheng, Yongqiang

AU - Daemen, Luke L

AU - Rudic, Svemir

AU - Ramirez-Cuesta, Anibal J

AU - Tang, Chiu C

AU - Yang, Sihai

PY - 2019/12/16

Y1 - 2019/12/16

N2 - 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 to 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 Brønsted acid sites on confined adsorption of GVL, while the catalytic mechanism for conversion of confined GVL to 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.

AB - 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 to 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 Brønsted acid sites on confined adsorption of GVL, while the catalytic mechanism for conversion of confined GVL to 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.

U2 - 10.1038/s41563-019-0562-6

DO - 10.1038/s41563-019-0562-6

M3 - Article

SN - 1476-1122

VL - 19

SP - 86

EP - 93

JO - Nature Materials

JF - Nature Materials

ER -

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

Abstract

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