Application Of Supported Two-Dimensional Nanostructured Materials In Catalytic Reaction

Since the graphene was successfully manufactured,two–dimensional?2D?materials have been attracted and followed.Due to their distinctive physical and chemical properties,they have become a hot research topic in the field of heterogeneous catalytic materials.The continuous development of computer technology also allows us to carry out simulation by using the theoretical basis.It help us to discover the theoretical explanation of experimental phenomenaand guide the next step of the latter experiment,which greatly reduce the exploration time of the experiment.In this thesis,we study the geometric structure and stability of the 2D material and substrate.The influence of intralayer space for the adsorption of the catalytic reactants is also studied.On this basis,confined catalysis under 2D materialsappliedin the oxidation of carbon monoxide?CO?.The paper mainly includes the following contents:We calculated the lattice constant,electron distribution and band structure of single–layer C₂N and Pt?111?surfaces by first–principles.The lattice of 1×1 single–layer C₂N is 8.33?and the lattice of 3×3Pt?111?surface is 8.21?.The mismatch of the two materials is less than 1.5%,which can be well combined as C₂N@Pt?111?system.With the van der Waals correction,the binding energy of those is 2.3 eV.The system can be stably existed in room temperature.By calculating the adsorption state of the reactants and the products in the interlayer and above the layer,we found that the space above the layer is unable to adsorb the reaction molecules.But in the interlayer,the adsorption energy of CO and CO₂ is weakened comparedtothose on pure Pt?111?surface,while the O₂ and O is enhanced.These results not only helps Pt surface to prevent CO poisoning,but also benefits the release of CO₂which reduces the accumulation of the product and accelerate the reaction rate.During the catalytic reaction,the dissociation energy of O₂ is also greatly reduced,and the adsorbedsingle O atom can directly combine with the CO gas in the interlayer to form CO₂.The only barrier is the potential of the reactants and products passing through the pores.base.