Density functional theory was used to study the NH3 behavior on Ni monolayer covered Pt（111） and WC（001）. The electronic structure of the surfaces, and the adsorption and decomposition of NH3 were calculated and c...Density functional theory was used to study the NH3 behavior on Ni monolayer covered Pt（111） and WC（001）. The electronic structure of the surfaces, and the adsorption and decomposition of NH3 were calculated and compared. Ni atoms in the monolayer behave different from that in Ni（111）. More dz2 electrons of Ni in monolayer covered systems were shifted to other regions compared to Ni（111）, charge density depletion on this orbital is crucial to NH3 adsorption. NH3 binds more stable on Ni/Pt（lll） and Ni/WC（001） than on Ni（111）, the energy barriers of the first N-H bond scission were evidently lower on Ni/Pt（111） and Ni/WC（001） than on Ni（111）, these are significant to NH3 decomposition. N recombination is the rate-limiting step, high reaction barrier implies that N2 is produced only at high temperatures. Although WC has similar properties to Pt, differences of the electronic structure and catalytic activities are observed for Ni/Pt（111） and Ni/WC （001）, the energy barrier for the rate-determined step increases on Ni/WC（001） instead of decreasing on Ni/Pt（lll） when compared to Ni（111）. the N recombination barrier by modifying To design cheaper and better catalysts, reducing Ni/WC（001） is a critical question to be solved.展开更多
文摘Density functional theory was used to study the NH3 behavior on Ni monolayer covered Pt（111） and WC（001）. The electronic structure of the surfaces, and the adsorption and decomposition of NH3 were calculated and compared. Ni atoms in the monolayer behave different from that in Ni（111）. More dz2 electrons of Ni in monolayer covered systems were shifted to other regions compared to Ni（111）, charge density depletion on this orbital is crucial to NH3 adsorption. NH3 binds more stable on Ni/Pt（lll） and Ni/WC（001） than on Ni（111）, the energy barriers of the first N-H bond scission were evidently lower on Ni/Pt（111） and Ni/WC（001） than on Ni（111）, these are significant to NH3 decomposition. N recombination is the rate-limiting step, high reaction barrier implies that N2 is produced only at high temperatures. Although WC has similar properties to Pt, differences of the electronic structure and catalytic activities are observed for Ni/Pt（111） and Ni/WC （001）, the energy barrier for the rate-determined step increases on Ni/WC（001） instead of decreasing on Ni/Pt（lll） when compared to Ni（111）. the N recombination barrier by modifying To design cheaper and better catalysts, reducing Ni/WC（001） is a critical question to be solved.
