Abstract
Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2 reduction. The obtained Pd/UiO-66-NO2 catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2 exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.
Highlights
Introduction iationsThe value-added conversion of biomass at high efficiency has become increasingly attractive for the sustainable production of clean fuels and chemicals [1,2]
We report on the catalytic hydrogenative ring-rearrangement of FAL to CPO in an aqueous phase using Pd/UiO-66-NO2 as the catalyst
When the thermal treatment time was 7 h, the selectivity to tetrahydrofurfuryl alcohol (THFOL) decreased to 2.5%, indicating that the higher Lewis acidity accelerated the conversion of furfuryl alcohol (FOL) to the rearrangement product
Summary
Powder X-ray diffraction (XRD) patterns were collected on a Rigaku D/Max-2400 diffractometer at 40 kV and 100 mA equipped with Ni-filtered Cu-Kα radiation. N2 adsorption/desorption isotherms were measured on a Micrometritics Tristar II 3020 instrument at. The specific surface area of the sample was calculated using the BET equation from the N2 adsorption isotherms. Measurements were performed on an ESCALAB XI+ X-ray photoelectron spectrometer, using an Al-Kα source. Where U pulse is the moles of CO injected each time, n is the number of pulses, Si is the chromatographic peak-area of each pulse, Smax is the chromatographic peak-area of saturated adsorption, A is the atomic weight of Pd, ν is the stoichiometry factor, W is the weight of supported Pd, n0 is the initial moles of FAL, C is the conversion of FAL, t is the reaction time, ωcat is the catalyst mass, Uad is the total moles of CO adsorbed on the sample
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