Construction of a mechanistic model of Fischer–Tropsch synthesis on Ni(1 1 1) and Co(0 0 0 1) surfaces

摘要: Abstract Tools for computer generation of reaction mechanisms were extended to handle heterogeneous catalytic reactions. Development these generic capabilities was carried out by constructing a detailed kinetic model Fischer–Tropsch synthesis on Ni(1 1 1) and Co(0 0 0 1) surfaces. To estimate rate constants during automatic mechanism reactions, linear free energy relationships applied using heat as the reactivity index, theoretical approaches used activation energies preexponential factors. Calculation heats involving surface species presented special challenges due unknown adsorption many adsorbates. This problem addressed estimating phenomenological approach which relates chemisorption multiatomic that adatoms. provide basis set values adsorbed surfaces, binding key intermediates calculated an ab initio method developed periodic systems. The energetics obtained in automatically constructed describing via carbene polymerization. predictions surfaces successfully captured product selectivities observed experimentally over nickel cobalt catalysts.