From Biomass‐Derived Furans to Aromatics with Ethanol over Zeolite

Abstract

Reaction conditions:In a typical experiment, 15 mL of the model compound 2,5-Dimethylfuran (99% Sigma-Aldrich), 8.2 mL of ethanol (99.5% Sigma-Aldrich) and 0.4 g of zeolite were used over a temperature range of 200 to 300 °C and 1.0 mL of tridecane as an internal standard. The reaction vessel was flushed with inert gas (N2). Liquid products were identified and quantified using a gas chromatograph/mass spectrometer (Agilent 6890 and Agilent MSD 5973 (N)) calibrated with pure standards. After reaction, the autoclave was cooled down to −60°C by dry ice/acetone bath. The gas products (CO, CO 2 , CH 4 ) analyzed by a Perkin Elmer Autosystem XL Arnel Gas phase GC-FID-Methanator. C 2 H 4 gas product was assumed to be mainly produced from ethanol. The solid residue was filtrated and washed with acetone and dried overnight (80 °C). Then it was analyzed by thermogravimetric analyses (TA instruments Q50), the samples were heated at 10 °C min −1 from room temperature to 900 °C under air to quantify the coke on zeolite to complete the carbon balance. The conversion was expressed in term of the molar conversion of 2,5-dimethylfuran and carbon balance was achieved at the minimum of 90-95%. Assessment of a possible diffusional controlled (mass limitations) reaction:The reaction conditions for ethylene gas or ethanol liquid placed with DMF liquid (generated pressurized vapors at 300 o C) were employed following the conditions established in reference [1]

Applications of Zeolites in Sustainable Chemistry

“…Recently, the catalytic conversion of 2,5-dimethylfuran to aromatics with ethanol over Brønsted acidic zeolites H-ZSM-5 (MFI type) and H-USY (USY type) was reported. 11 The usage of liquid ethanol instead of gaseous ethylene made the production of aromatics much simpler and renewable. More importantly, much improved reaction rates (turnover frequency up to 15 3 10 2 hr À1 ) and selectivity (up to 90%) to…”

Understanding initial zeolite oligomerization steps with first principles calculations

“…Zeolites can be synthesized with detailed control of their physiochemical properties which makes them excellent materials for applications in fields such as separations, 1,2 ion exchange, 3 and catalysis. 4,5 The ability to control the structural and chemical functionalities of a given zeolite is extremely important for its end application. For example, ZSM-5 (MFI type) is one of the most commonly used industrial catalysts in the cracking of long hydrocarbon chains to produce light olefins due to its acidic properties and (hydro)thermal stability.…”

“…Zeolites are porous aluminosilicates that are both naturally occurring and synthetically produced. Zeolites can be synthesized with detailed control of their physiochemical properties which makes them excellent materials for applications in fields such as separations, 1,2 ion exchange, 3 and catalysis 4,5 . The ability to control the structural and chemical functionalities of a given zeolite is extremely important for its end application.…”

Mononuclear gold species anchored on TS-1 framework as catalyst precursor for selective epoxidation of propylene

“…13,14 The alteration in scattering parameters of modified framework atoms by the host species enables the probing of adsorption geometries and interactions on the inner zeolitic surface. 15,16 SXRD patterns of calcined TS-1 and (NaOH)i-Au/TS-1 are presented in Figure S9. As discussed in the main text, the incorporation of Au into TS-1 did not alter the space group of TS-1; on the other hand, the relative intensities of the peaks were different for the two samples without any observable peak broadening.…”