Research output: Contribution to journal › Article › peer-review
Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite. / Lin, Longfei; Sheveleva, Alena M.; da Silva, Ivan et al.
In: Nature Materials, Vol. 19, No. 1, 01.01.2020, p. 86-93.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite
AU - Lin, Longfei
AU - Sheveleva, Alena M.
AU - da Silva, Ivan
AU - Parlett, Christopher M.A.
AU - Tang, Zhimou
AU - Liu, Yueming
AU - Fan, Mengtian
AU - Han, Xue
AU - Carter, Joseph H.
AU - Tuna, Floriana
AU - McInnes, Eric J.L.
AU - Cheng, Yongqiang
AU - Daemen, Luke L.
AU - Rudić, Svemir
AU - Ramirez-Cuesta, Anibal J.
AU - Tang, Chiu C.
AU - Yang, Sihai
PY - 2020/1/1
Y1 - 2020/1/1
N2 - 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.
AB - 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.
KW - INELASTIC NEUTRON-SCATTERING
KW - LEWIS-ACID SITES
KW - NIOBIUM PHOSPHATE
KW - SOLID ACID
KW - CONVERSION
KW - DECARBOXYLATION
KW - DEHYDRATION
KW - LOCATION
KW - FRUCTOSE
KW - ZSM-5
UR - http://www.scopus.com/inward/record.url?scp=85076925594&partnerID=8YFLogxK
U2 - 10.1038/s41563-019-0562-6
DO - 10.1038/s41563-019-0562-6
M3 - Article
C2 - 31844281
AN - SCOPUS:85076925594
VL - 19
SP - 86
EP - 93
JO - Nature Materials
JF - Nature Materials
SN - 1476-1122
IS - 1
ER -
ID: 23094033