Density Functional Theory Study On Oxidation Of CO Catalyzed By Aluminum Clusters Doped Golden And Water Gas Shift Reaction Catalyzed By Tungsten Carbonyls

In recent years,with the rapid development of industry,toxic gases CO emissions also present a rapidly increasing trend.Economic development will inevitably bring the environment pollution and destruction,but starting from the concept of sustainable development,we must follow the economic development and the management of environmental pollution.People can not to damage the environment for economic development.This requests us in the pursuit of the process of economic development,one is to effective governance of poisonous gas pollution,the second is to pursue development of new green energy,which are two important ideas embodying in my paper.The nanoparticle catalyst duo to the unique catalytic activity catches more and more attention.When choosing catalyst we consider both it’s catalytic activity and cost-effective.Starting from this line of thought,we chose a cheap aluminunm cluster doped with asmall amount of glod as a catalyst for CO oxidation.This is because Aluminum nanoclusters play important roles in chemical reactions and nanosized devices with many chemical and physical properties such as conductivity,superconductivity,and also magnetic properties.Especially,aluminum alloy clusters provide a matter of increasing interest in pure and applied aterials sciences and traditional fields of physics and chemistry.So Over the past few years,aluminum clusters doped with a metal or nonmetal atom have received much attention.Nanosized gold clusters have attracted great interest over the past few decades owing to their unusual catalytic properties not seen in bulk gold.So in this work,the CO oxidation on Aluminum-doped gold clusters Al_nAu with n=1-12 is investigated by density functional theory computations,using Perdew-Burke-Ernzerh（PBE）fuctionals along with the LANL2 DZ pseudopotential basis for Au and 6-31G（d,p）basis for aluminum,oxygen and carbon.It is shown that mixing two different metals（Al and Au）can have beneficial effects on the catalytic activities and the alloyed Al11 Au cluster with the lower energy barrier 0.36 e V is proposed as the best effective nanocatalysts.Hydrogen becomes the most popular green energy due to it’s light quality,easy storage,large burning energy and the clean production of the combustion.The Water gas shift reaction（WGSR）is to removethe CO in the process of hydrogen production,further improve the concentration of hydrogen.There are a large of reports of water gas shift reaction and the metal carbonyl compounds in the water gas shift reaction show higher catalytic activity.So in this work,A density functional theory（DFT）calculation has been carried out to investigate the mechanism of W（CO）₆and W₂（CO）₁₀catalyzed water-gas-shift reaction（WGSR）.The standard 6-31++g（d,p）basis set was used for hydrogen,oxygen and carbon and the LANL2 DZ basis set was used for Tungsten.The bimetallic catalyst(W₂（CO）₁₀)with the highest value of the calculated turnover frequence(3.62×10^-12,gas phase;8.74×10^-15,solvent phase)exhibits high catalytic activity towards water gas shift reaction and the binuclear mechanism is the best mechanism in the water gas shift reaction.