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Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite.
Nature Materials ( IF 41.2 ) Pub Date : 2019-12-16 , DOI: 10.1038/s41563-019-0562-6
Longfei Lin 1 , Alena M Sheveleva 1, 2 , Ivan da Silva 3 , Christopher M A Parlett 4, 5, 6 , Zhimou Tang 7 , Yueming Liu 7 , Mengtian Fan 1 , Xue Han 1 , Joseph H Carter 1 , Floriana Tuna 1 , Eric J L McInnes 1 , Yongqiang Cheng 8 , Luke L Daemen 8 , Svemir Rudić 3 , Anibal J Ramirez-Cuesta 8 , Chiu C Tang 6 , Sihai Yang 1
Affiliation  

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.

中文翻译:

杂原子MFI沸石催化从生物质衍生的γ-戊内酯定量生产丁烯。

由可再生生物质有效生产轻质烯烃是实现未来可持续化学过程的重要且具有挑战性的目标。在这里,我们报告了一种杂原子MFI型沸石(NbAlS-1),从生物质衍生的碳水化合物中获得的γ-戊内酯(GVL)水溶液可以定量转化为丁烯,其收率> 99%连续流动条件下的环境压力。NbAlS-1同时将铌(V)和铝(III)中心并入骨架中,因此具有理想强度的路易斯和布朗斯台德酸中心分布。同步X射线衍射和吸收光谱表明,在GVL的有限吸附下,Nb(V)与布朗斯台德酸位之间存在协同作用,而受限的GVL转化为丁烯的催化机理是通过原位非弹性中子散射和建模来揭示的。这项研究为丁烯作为生产可再生材料的平台化学品的可持续生产提供了前景。
更新日期:2019-12-17
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