Adsorption behavior of CO, CO2, H2, H2O, NO, and O2 on pristine and defective 2D monolayer ferromagnetic Fe3GeTe2

Recently, 2D ferromagnets have emerged as a hot research topic, especially after the exfoliation of monolayer ferromagnetic Fe3GeTe2 from its bulk structure (Nature 2018, 563, 94; Nat. Mater. 2018, 17, 778). In this work, we systematically report the adsorption behavior of CO, CO2, H2, H2O, NO, and O2 on the pristine and Te-deficient Fe3GeTe2 (FGT and d-FGT) monolayer using hybrid density functional theory. We find that the toxic gas molecules (CO and NO) and O2 molecular are chemically anchored at the surface of the pristine FGT, while the H2O, CO2, and H2 are physically associated with FGT. Interestingly, the introduction of Te deficiency would significantly enhance the covalent interactions between the substrate and the gas molecules, especially for CO2 and H2O, whose adsorption type has evolved from physisorption to chemisorption. Furthermore, the adsorption capacity of (d-)FGT to gas molecules is found to be stronger than that of the two well-studied 2D materials: MoS2 and MXenes. Meanwhile, the adsorption changes the electronic structure of (d-)FGT but does not change the metallicity of FGT. This work provides a valuable reference for the application of 2D metallic ferromagnetic materials in the field of catalysis, sensors, gas storage, and environmental remediation.