Abstract

Conversion of biorenewable feedstocks into transportation fuels or chemicals likely necessitates the development of novel heterogeneous catalysts with good hydrothermal stability, due to the nature of highly oxygenated biomass compounds and the prevalence of water as a processing solvent. The use of carbon-based materials, derived from sugars as catalyst precursors, can achieve hydrothermal stability while simultaneously realizing the goal of sustainability. In this work, the simultaneous pyrolysis of glucose and taurine in the presence of multi-walled carbon nanotubes (MWCNTs), to obtain versatile solid acids, has been demonstrated. Structural and textural properties of the catalysts have been characterized by TEM, TGA, and XPS. Additionally, solid state nuclear magnetic resonance (ssNMR) spectroscopy has been exploited to elucidate the chemical nature of carbon species deposited on the surface of MWCNTs. Al(OTf)3, a model Lewis acidic metal salt, has been successfully supported on sulfonic groups tethered to MWCNTs. This catalyst has been tested for C6 sugar dehydration for the production of HMF in a tetrahydrofuran (THF)/water solvent system with good recyclability.

Highlights

  • Due to the rapidly growing world energy and materials consumption, and diminishing petroleum reserves, economical and environmental concerns have risen, urging the utilization of renewable sources of carbon for liquid transportation fuels and chemicals

  • multi-walled carbon nanotubes (MWCNTs) have a relatively high surface area and relatively less microporosity, making them less likely than conventional carbon-based materials to encounter mass transport limitations when they are used as catalyst supports [6]

  • This indicates that the presence of the MWCNT during the pyrolysis reaction at 250 C does nuclei that originated in the glucose

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Summary

Introduction

Due to the rapidly growing world energy and materials consumption, and diminishing petroleum reserves, economical and environmental concerns have risen, urging the utilization of renewable sources of carbon for liquid transportation fuels and chemicals. Hydrothermal stability concerns have promoted recent research into carbon-based supports for biorenewable applications [5]. MWCNTs have a relatively high surface area and relatively less microporosity, making them less likely than conventional carbon-based materials to encounter mass transport limitations when they are used as catalyst supports [6]. It was found that glucose and taurine can be pyrolyzed together to form alkyl-linked sulfonic acids for various acid-catalyzed reactions, such as dehydration and esterification [9], and this class of materials has been thoroughly characterized by NMR [10]. In order to solve this problem, we reasoned that, in the presence of a porous support such as MWCNT, co-pyrolysis of glucose and taurine could form, ideally, a thin layer of carbonaceous material containing alkyl-linked sulfonic acid groups.

Catalyst
Solid-State NMR
13 C-taurine-labeled thevariations
MultiCP spectraofof13 C-taurine-labeled
Materials Characterization
Reaction Testing
Conclusions
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