Nanocrystalline rhenium-doped TiO2: an efficient catalyst in the one-pot conversion of carbohydrates into levulinic acid. The synergistic effect between Brønsted and Lewis acid sites

Sorin Avramescu; Cristian D. Ene; Madalina Ciobanu; Josefine Schnee; Francois Devred; Cristina Bucur; Eugeniu Vasile; Luke Colaciello; Ryan Richards; Eric M. Gaigneaux; Marian Nicolae Verziu

doi:10.1039/D1CY01450A

Nanocrystalline rhenium-doped TiO₂: an efficient catalyst in the one-pot conversion of carbohydrates into levulinic acid. The synergistic effect between Brønsted and Lewis acid sites†

Sorin Avramescu,^a Cristian D. Ene,

^b Madalina Ciobanu,^b Josefine Schnee,

^c Francois Devred,^d Cristina Bucur,^e Eugeniu Vasile,^f Luke Colaciello,^g Ryan Richards,

*^g Eric M. Gaigneaux

*^d and Marian Nicolae Verziu

*^hi

Author affiliations

* Corresponding authors

^a Department of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, Bdul Regina Elisabeta, 4-12, Bucharest 030016, Romania

^b “Ilie Murgulescu” Institute of Physical Chemistry, Romanian Academy, Splaiul Independentei 202, 060021 Bucharest, Romania

^c Normandie Université, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, Boulevard Maréchal Juin 6, 14000 Caen, France

^d Institute of Condensed Matter and Nanosciences (IMCN) – Molecular Chemistry, Materials and Catalysis (MOST) – Université Catholique de Louvain (UCLouvain), Place Louis Pasteur 1, box L4.01.09, 1348 Louvain-la-Neuve, Belgium
E-mail: eric.gaigneaux@uclouvain.be

^e National Institute of Materials Physics, Atomistilor 105b, 077125 Magurele-Ilfov, Romania

^f Faculty of Applied Chemistry and Materials Science, University Politehnica of Bucharest, 1-7 Gh Polizu Street, Bucharest, Romania

^g Colorado School of Mines, Department of Chemistry, Golden, Colorado 80401, USA
E-mail: rrichard@mines.edu

^h Institute of Organic Chemistry “C. D. Nenitescu” of Romanian Academy, 202B Spl. Independentei, P.O. Box 35-108, Bucharest, Romania

ⁱ Department of Bioresources and Polymer Science, Advanced Polymer Materials Group, Faculty of Applied Chemistry and Materials Science, University Politehnica of Bucharest, 1-7 Gh Polizu Street, Bucharest, Romania
E-mail: marian.verziu@upb.ro

Abstract

Catalytic activity of TiO₂, 2%Re–TiO₂ and 10%Re–TiO₂ in the conversion of carbohydrates into levulinic acid under autoclave conditions was evaluated. These materials were prepared by aerogel method, for the first time to the best of our knowledge, and characterized by XPS, SEM-EDX, DRIFTS, DR UV-vis, Raman, N₂ adsorption/desorption isotherms, TGA and XRD. Further, the surface acidity was probed by NH₃-TPD and pyridine-FT-IR where it was observed that increasing the amount of rhenium doped into TiO₂ led to an increase in the total number of acid sites (Lewis + Brønsted) but with an overall lower strength. The presence of both Brønsted and Lewis acid sites led to the hypothesis that these materials may be well suited for conversion of carbohydrates into levulinic acid. Indeed a levulinic acid yield of 57% was reached over 10%Re–TiO₂ for a low mass ratio catalyst to glucose (1 : 5). Moreover, the 10%Re–TiO₂ catalyst was reused in the conversion of glucose for four catalytic cycles without a significant loss of the catalytic activity.

Catalysis Science & Technology

Nanocrystalline rhenium-doped TiO₂: an efficient catalyst in the one-pot conversion of carbohydrates into levulinic acid. The synergistic effect between Brønsted and Lewis acid sites†

Abstract

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Nanocrystalline rhenium-doped TiO₂: an efficient catalyst in the one-pot conversion of carbohydrates into levulinic acid. The synergistic effect between Brønsted and Lewis acid sites

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