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 Jl Mcinnes, Luke L Keenan, Daniel Lee, Martin P Attfield, Sihai Yang

Research output: Contribution to journalArticlepeer-review

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.
Original languageEnglish
Article numbere202212164
JournalAngewandte Chemie International Edition
Volume61
Issue number51
Early online date14 Oct 2022
DOIs
Publication statusPublished - 19 Dec 2022

Research Beacons, Institutes and Platforms

  • Henry Royce Institute
  • Dalton Nuclear Institute

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