Acidic graphene organocatalyst for the superior transformation of wastes into high-added-value chemicals

Abstract

Our dependence on finite fossil fuels and the insecure energy supply chains have stimulated intensive research for sustainable technologies. Upcycling glycerol, produced from biomass fermentation and as a biodiesel formation byproduct, can substantially contribute in circular carbon economy. Here, we report glycerol’s solvent-free and room-temperature conversion to high-added-value chemicals via a reusable graphene catalyst (G-ASA), functionalized with a natural amino acid (taurine). Theoretical studies unveil that the superior performance of the catalyst (surpassing even homogeneous, industrial catalysts) is associated with the dual role of the covalently linked taurine, boosting the catalyst’s acidity and affinity for the reactants. Unlike previous catalysts, G-ASA exhibits excellent activity (7508 mmol g−1 h−1) and selectivity (99.9%) for glycerol conversion to solketal, an additive for improving fuels’ quality and a precursor of commodity and fine chemicals. Notably, the catalyst is also particularly active in converting oils to biodiesel, demonstrating its general applicability.

Efficient Synthesis of Solketal from Glycerol and Acetone Catalyzed by FeCl3 /γ‐Al2O3**

“…Meanwhile, FeCl 3 /γ‐Al 2 O 3 catalyst was recovered from the reaction system by separation, washing and calcination at 300 °C for 2 h to remove adsorbed H 2 O and organic matter. The glycerol conversion, Solketal selectivity and Yield of Solketal were gotten based on the following equations (1‐3) [31a,39] : $$$\vcenter{\openup.5em\halign{$\displaystyle{#}$\cr {\rm C}{\rm o}{\rm n}{\rm v}{\rm e}{\rm r}{\rm s}{\rm i}{\rm o}{\rm n}{\rm \ }{\rm o}{\rm f}{\rm \ }{\rm g}{\rm l}{\rm y}{\rm c}{\rm e}{\rm r}{\rm o}{\rm l}{\rm \ }\left({\rm \char37 }\right)=\hfill\cr {{{\rm G}{\rm l}{\rm y}{\rm c}{\rm e}{\rm r}{\rm o}{\rm l}{\rm \ }{\rm c}{\rm o}{\rm n}{\rm v}{\rm e}{\rm r}{\rm t}{\rm e}{\rm d}{\rm \ }\left({\rm m}{\rm o}{\rm l}\right){\rm \ }}\over{{\rm I}{\rm n}{\rm i}{\rm t}{\rm i}{\rm a}{\rm l}{\rm \ }{\rm g}{\rm l}{\rm y}{\rm c}{\rm e}{\rm r}{\rm o}{\rm l}{\rm \ }\left({\rm m}{\rm o}{\rm l}\right)}}\times 100\hskip0.17em{\rm \char37 }\hfill\cr}}$$$ …”

Advances in Biocarbon and Soft Material Assembly for Enthalpy Storage: Fundamentals, Mechanisms, and Multimodal Applications

“…Owing to their distinct chemical and physical characteristics (with a breaking strength of 42 N m −1 and Young's modulus of ≈1.0 terapascals), high electron mobility (>200 000 cm 2 (V s) −1 at low temperatures), [130] strong thermal and chemical stabilities, conductivity (≈3000 W m −1 K −1 ), and optoelectronic properties, applications of graphene and its derivatives have been extended to a much broader areas, such as energy storage, adsorption, water splitting, photocatalysis, biosensors, and biomedical. [68,[131][132][133][134][135][136] One plausible approach to harness these characteristics for applications would be to integrate graphene sheets in composite material using different design methods, such as solution mixing/impregnation, in situ polymerization, coating, and melt grinding, [135,137] as shown in Figure 13. Li et al [138] prepared graphene foam-based nanocomposite using paraffin wax.…”

Graphene oxide-catalysed carbene-transfer reaction in water: a highly “green” and selective approach to access 3,3′,3′′-trisindoles

“…30 Recently, Zbořil et al reported the transformation of wastes into high-added-value chemicals using GO as an organocatalyst. 31 With our interest towards the development of environmentally friendly synthetic methodologies, herein we revealed a highly green and efficient synthesis of 3,3′,3″-trisindoles using GO as a heterogeneous catalyst in DMSO/water medium. This is the first report on a carbene-transfer reaction using GO as a highly green and reusable catalyst (Scheme 1f ).…”

“…30 Recently, Zbořil et al reported the transformation of wastes into high-added-value chemicals using GO as an organocatalyst. 31…”