4.8 Article

Niobium grafted mesoporous silica for the production of biorenewable p-xylene from concentrated 2,5-dimethylfuran

期刊

GREEN CHEMISTRY
卷 24, 期 10, 页码 4095-4107

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1gc04734e

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资金

  1. National Natural Science Foundation of China [21972024, 21773033, 22088101]
  2. Science and Technology Commission of Shanghai Municipality [19DZ2270100, 20ZR1404600]
  3. SINOPEC [X514005]

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The dispersion of NbOx on the inner surface of MCM-type mesoporous silica as a catalyst enables efficient production of PX from concentrated DMF. This catalyst exhibits excellent activity, selectivity, and stability, highlighting its importance in the conversion of DMF and related furanic compounds to aromatic products.
The Diels-Alder cycloaddition of bio-based 2,5-dimethylfuran (DMF) and ethylene and the subsequent dehydration of the cycloadduct intermediate hold promise to produce renewable p-xylene (PX) from biomass feedstocks. Developing reliable and robust catalysts for the efficient transformation of concentrated DMF to PX is highly demanded but challenging. Herein we describe an efficient approach to enable practically viable PX production from concentrated DMF (4 mol L-1), employing NbOx dispersed atomically on the interior surface of MCM-type mesoporous silica as a potent catalyst. Benefiting from its unique structural merits that lead to significant lowering of the kinetic barrier for cycloadduct intermediate formation, 8Nb/MCM exhibits excellent activity with 100% conversion and over 96% selectivity and stability (marginal activity loss after 5 cycles of reuse) toward the controlled conversion of DMF and related furanic compounds to the corresponding aromatic products using concentrated feeds. These results have important implications for the advancement of next-generation solid multifunctional catalysts by meticulously tuning the pore structure and precise location of active sites with required characteristics.

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