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

Angewandte Chemie (International ed. in English) 2022 Nov 17

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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 AlIII and NbV 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 NbV 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. © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Citation

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. Bimetallic Aluminum- and Niobium-Doped MCM-41 for Efficient Conversion of Biomass-Derived 2-Methyltetrahydrofuran to Pentadienes. Angewandte Chemie (International ed. in English). 2022 Nov 17;61(51):e202212164