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Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes

Mengtian Fan, Shaojun Xu, Bing An, Alena M. Sheveleva, Alexander Betts, Joseph Hurd, Zhaodong Zhu, Meng He, Dinu Iuga, Longfei Lin, Xinchen Kang, Christopher M. A. Parlett, Floriana Tuna, Eric J. L. McInnes, Luke L. Keenan, Daniel Lee, Martin P. Attfield, Sihai Yang⧫

2022Angewandte Chemie International Edition20 citationsDOIOpen Access PDF

Abstract

Abstract 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 Brønsted 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.

Topics & Concepts

Bimetallic stripMesoporous materialConjugated systemBifunctionalLewis acids and basesMaterials scienceDopingNiobiumBiomass (ecology)CatalysisInfrared spectroscopyChemical engineeringChemistryNanotechnologyOrganic chemistryPolymerGeologyEngineeringOptoelectronicsOceanographyCatalysis for Biomass ConversionMesoporous Materials and CatalysisCatalysis and Hydrodesulfurization Studies
Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes | Litcius