Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
Wubin Yan,Binbin Jin,Jiong Cheng,Xiaoyu Shi,Heng Zhong,Fangming Jin
Direct hydrogenation of CO2 (or HCO3–) into chemicals using organic waste biomass as a hydrogen donor is a promising carbon-negative strategy to alleviate the global warming caused by excessive CO2 emission. However, the reported conversion efficiencies are quite limited. In this work, a facile Ru/ZrO2 catalyst was developed to catalyze the hydrogenation of HCO3– into formate by using biodiesel-waste glycerol as the reductant. It was found that ruthenium can significantly promote the dehydrogenation of glycerol to provide in situ hydrogen for HCO3– hydrogenation according to the in situ Fourier transform infrared spectrometer analysis. Moreover, hydrogen spillover between ruthenium and ZrO2 support was also formed. Consequently, efficient hydrogen transfer could be constructed in the presence of Ru/ZrO2, achieving desirable in situ hydrogenation of HCO3– into formate eventually. The highest yield of formate up to 25.1% was obtained over Ru/ZrO2, while the formate yield was only 4.2% in the case without catalysts.
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