氧化钛110面上甲醇吸附结构的研究

Adsorption of methanol on TiO2 was studied extensively theoretically and experimentally because of its potential application in photo-catalysis, due to not only its own ability to produce hydrogen but also the promotion of hydrogen production from water. However, the structures at wide range of the coverage from submonolayer to saturate adsorption as well as its stability at different temperatures and pressures remain in debate. In this talk, we present a detailed ab initio thermodynamics and kinetic Monte Carlo (KMC) study on methanol adsorption and desorption on TiO2(110) surface. The thermodynamics analysis based on the density functional theory calculations shows that the methanol adsorption at coverage of 2/3 ML is prevailed at a very wide range of temperatures and pressures. The temperature programmed desorption (TPD) based on KMC are simulated, and a detailed microscopic picture of adsorption and desorption of methanol on TiO2(110) was mapped out for the first time, and the excellent agreement with experiment was found and shown in fig. 1. We found that the full monolayer adsorption methanol desorbs at about 150 K and the methanol dimer at coverage of 2/3 ML is stable up 250 K. With increase of temperature further, the methanol dimer becomes unstable and transit to the monomer, which desorbs from the surface at 350 K