Replacement of chromium by non-toxic metals in lewis-acid MOFs: Assessment of stability as glucose conversion catalysts

Ralentri Pertiwi; Ryan Oozeerally; David L. Burnett; Thomas W. Chamberlain; Nikolay Cherkasov; Marc Walker; Reza J. Kashtiban; Yuni K. Krisnandi; Volkan Degirmenci; Richard I. Walton

doi:10.3390/catal9050437

Replacement of chromium by non-toxic metals in lewis-acid MOFs: Assessment of stability as glucose conversion catalysts

Ralentri Pertiwi, Ryan Oozeerally, David L. Burnett, Thomas W. Chamberlain, Nikolay Cherkasov, Marc Walker, Reza J. Kashtiban, Yuni K. Krisnandi, Volkan Degirmenci, Richard I. Walton

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

37 Citations (Scopus)

Abstract

The metal-organic framework MIL-101(Cr) is known as a solid-acid catalyst for the solution conversion of biomass-derived glucose to 5-hydroxymethyl furfural (5-HMF). We study the substitution of Cr³⁺ by Fe³⁺ and Sc³⁺ in the MIL-101 structure in order to prepare more environmentally benign catalysts. MIL-101(Fe) can be prepared, and the inclusion of Sc is possible at low levels (10% of Fe replaced). On extended synthesis times the polymorphic MIL-88B structure instead forms.Increasing the amount of Sc also only yields MIL-88B, even at short crystallisation times. The MIL-88B structure is unstable under hydrothermal conditions, but in dimethylsulfoxide solvent, it provides 5-HMF from glucose as the major product. The optimum material is a bimetallic (Fe,Sc) form of MIL-88B, which provides ~70% conversion of glucose with 35% selectivity towards 5-HMF after 3 hours at 140 °C: this offers high conversion compared to other heterogeneous catalysts reported in the same solvent.

Original language	English
Article number	437
Journal	Catalysts
Volume	9
Issue number	5
DOIs	https://doi.org/10.3390/catal9050437
Publication status	Published - 1 May 2019

Keywords

5-hydroxymethyl furfural
Biomass
Fructose
Lewis acid
Metal-organic framework

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title = "Replacement of chromium by non-toxic metals in lewis-acid MOFs: Assessment of stability as glucose conversion catalysts",

abstract = "The metal-organic framework MIL-101(Cr) is known as a solid-acid catalyst for the solution conversion of biomass-derived glucose to 5-hydroxymethyl furfural (5-HMF). We study the substitution of Cr3+ by Fe3+ and Sc3+ in the MIL-101 structure in order to prepare more environmentally benign catalysts. MIL-101(Fe) can be prepared, and the inclusion of Sc is possible at low levels (10% of Fe replaced). On extended synthesis times the polymorphic MIL-88B structure instead forms.Increasing the amount of Sc also only yields MIL-88B, even at short crystallisation times. The MIL-88B structure is unstable under hydrothermal conditions, but in dimethylsulfoxide solvent, it provides 5-HMF from glucose as the major product. The optimum material is a bimetallic (Fe,Sc) form of MIL-88B, which provides ~70% conversion of glucose with 35% selectivity towards 5-HMF after 3 hours at 140 °C: this offers high conversion compared to other heterogeneous catalysts reported in the same solvent.",

keywords = "5-hydroxymethyl furfural, Biomass, Fructose, Lewis acid, Metal-organic framework",

author = "Ralentri Pertiwi and Ryan Oozeerally and Burnett, {David L.} and Chamberlain, {Thomas W.} and Nikolay Cherkasov and Marc Walker and Kashtiban, {Reza J.} and Krisnandi, {Yuni K.} and Volkan Degirmenci and Walton, {Richard I.}",

year = "2019",

month = may,

day = "1",

doi = "10.3390/catal9050437",

language = "English",

volume = "9",

journal = "Catalysts",

issn = "2073-4344",

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TY - JOUR

T1 - Replacement of chromium by non-toxic metals in lewis-acid MOFs

T2 - Assessment of stability as glucose conversion catalysts

AU - Pertiwi, Ralentri

AU - Oozeerally, Ryan

AU - Burnett, David L.

AU - Chamberlain, Thomas W.

AU - Cherkasov, Nikolay

AU - Walker, Marc

AU - Kashtiban, Reza J.

AU - Krisnandi, Yuni K.

AU - Degirmenci, Volkan

AU - Walton, Richard I.

PY - 2019/5/1

Y1 - 2019/5/1

N2 - The metal-organic framework MIL-101(Cr) is known as a solid-acid catalyst for the solution conversion of biomass-derived glucose to 5-hydroxymethyl furfural (5-HMF). We study the substitution of Cr3+ by Fe3+ and Sc3+ in the MIL-101 structure in order to prepare more environmentally benign catalysts. MIL-101(Fe) can be prepared, and the inclusion of Sc is possible at low levels (10% of Fe replaced). On extended synthesis times the polymorphic MIL-88B structure instead forms.Increasing the amount of Sc also only yields MIL-88B, even at short crystallisation times. The MIL-88B structure is unstable under hydrothermal conditions, but in dimethylsulfoxide solvent, it provides 5-HMF from glucose as the major product. The optimum material is a bimetallic (Fe,Sc) form of MIL-88B, which provides ~70% conversion of glucose with 35% selectivity towards 5-HMF after 3 hours at 140 °C: this offers high conversion compared to other heterogeneous catalysts reported in the same solvent.

AB - The metal-organic framework MIL-101(Cr) is known as a solid-acid catalyst for the solution conversion of biomass-derived glucose to 5-hydroxymethyl furfural (5-HMF). We study the substitution of Cr3+ by Fe3+ and Sc3+ in the MIL-101 structure in order to prepare more environmentally benign catalysts. MIL-101(Fe) can be prepared, and the inclusion of Sc is possible at low levels (10% of Fe replaced). On extended synthesis times the polymorphic MIL-88B structure instead forms.Increasing the amount of Sc also only yields MIL-88B, even at short crystallisation times. The MIL-88B structure is unstable under hydrothermal conditions, but in dimethylsulfoxide solvent, it provides 5-HMF from glucose as the major product. The optimum material is a bimetallic (Fe,Sc) form of MIL-88B, which provides ~70% conversion of glucose with 35% selectivity towards 5-HMF after 3 hours at 140 °C: this offers high conversion compared to other heterogeneous catalysts reported in the same solvent.

KW - 5-hydroxymethyl furfural

KW - Biomass

KW - Fructose

KW - Lewis acid

KW - Metal-organic framework

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U2 - 10.3390/catal9050437

DO - 10.3390/catal9050437

M3 - Article

AN - SCOPUS:85067002472

SN - 2073-4344

VL - 9

JO - Catalysts

JF - Catalysts

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M1 - 437

ER -

Replacement of chromium by non-toxic metals in lewis-acid MOFs: Assessment of stability as glucose conversion catalysts

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Keywords

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