The construction of iron-based catalysts encapsulated by graphite for CO2 hydrogenation to light olefins

Abstract

Developing efficient catalytic materials and unveiling the active factors are significant for selective hydrogenation of CO2 to light olefins (C2–4=). Herein, Fe3O4-FeCx nanoparticles coated by graphite without other doped elements were synthesized successfully. The optimal catalyst exhibited CO2 conversion of 48.0 %, C2–4= space–time yield of 29.0 mmol·g−1·h−1, and a stability of 100 h (3.0 MPa, 320 °C, and GHSV = 12000 mL·g−1·h−1). The core–shell structure derived from the strong interaction between the phenolic hydroxyl group of resin and iron ions, as well as the encapsulation of the copolymer P123. The characterization results revealed that the size of core–shell particles and thickness of graphite layers could be regulated by P123, which affected the conversion of CO2 and products distribution significantly. Moreover, the combined results of quasi in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and Raman spectra suggested small particle size and thin graphite shell strengthen the adsorption and conversion of CO2, playing an important role in the formation of light olefins. This work proposes a simple and feasible synthesis strategy to construct Fe3O4-FeCx particles encapsulated by graphite shell, which provides insights into catalysts design and the reaction mechanism of CO2 conversion to light olefins.