期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 51, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202212164
关键词
2-Methyltetrahydrofuran; Cleavage of C-O Bond; Niobium Sites; Pentadienes
资金
- EPSRC [EP/S023755/1]
- Royal Society
- University of Manchester
- EPSRC National EPR Facility at Manchester - EPSRC
- BBSRC
- University of Warwick - Advantage West Midlands (AWM)
- European Regional Development Fund (ERDF)
- Henry Royce Institute for Advanced Materials - EPSRC [EP/T015063/1]
- [EP/R00661X/1]
- [EP/S019367/1]
- [EP/P025021/1]
- [EP/P025498/1]
This study reports the successful conversion of 2-MTHF to pentadienes using bimetallic atomically doped mesoporous silica material. The molecular mechanism of the conversion is revealed, highlighting the potential of hetero-atomic mesoporous solids for the manufacture of renewable materials.
The production of conjugated C4-C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)-atomically doped mesoporous silica, denoted as AlNb-MCM-41, which affords quantitative conversion of 2-methyltetrahydrofuran (2-MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of Al-III and Nb-V sites into the framework of AlNb-MCM-41 has effectively tuned the nature and distribution of Lewis and Bronsted acid sites within the structure. Operando X-ray absorption, diffuse reflectance infrared and solid-state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2-MTHF over AlNb-MCM-41. Specifically, the atomically-dispersed Nb-V sites play an important role in binding 2-MTHF to drive the conversion. Overall, this study highlights the potential of hetero-atomic mesoporous solids for the manufacture of renewable materials.
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