The First-Principles Investigation Of Electrocatalytic Oxygen Evolution Reaction On FeO_x

With the development of the density functional theory,it plays a more and more important role in the design of new materials.By using computer software program implement the calculation of the specific system.The development of computer level provides an effective means to the realization of design new material.With the global population growth,we are facing more and more serious problems of' environmental pollution and energy shortage.So the development of clean energy is an important challenging issue.Most notably,electrochemical reactions can be achieved by decomposing water into hydrogen and oxygen to store energy,and the products can provide the clean energy with zero pollutant emissions.Therefore,the electrochemical method has become a long-term sustainable development of the application methods which can reduce greenhouse gas emissions.However,the kinetics of electrochemical reactions hampered the application efficiency of this technology.In order to promote the development of this technology and renewable energy,the high activity and cost-effective catalysts play an important role in the electrochemical reaction.In this paper,according to the first-principles theory,the catalytic activities of Fe₂O₃?0001?surface,Fe₂O₃ cluster and Fe₄O cluster are studied for the oxygen evolution reaction.And we analyze the effects of the Ni and Co doped the catalysts.The details are as follows:In the first chapter,we mainly introduce the density functional theory.Some approximations and development of density functional theory are briefly introduced.We can get the ground state density and energy of the original interaction system by solving the equation,and we calculate the properties of the exact multi-body particle system by using the non-interacting independent particle system method.Then,the application of density functional theory method is implemented through the computer program.The development of the commercial software package also provides an effective means for the realization of the calculation.And we also introduce some of the software programs in this paper.In the second chapter,we mainly introduce the reaction mechanism of oxygen evolution reaction.Currently,the reaction mechanism of the oxygen evolution reaction is the four proton-coupled electron transfer mechanism.On the basis of the four proton-coupled electron transfer mechanism of the oxygen evolution reaction,we calculate the reaction free energy of each reaction step.The catalytic performance was estimated by magnitude of the potential-determining step and over-potential.We also give some detail information,such as bond length,binding energy and charges.In the third chapter,based on the first-principles theory and the reaction mechanism of oxygen evolution reaction,we studied the catalytic activity of the Fe₂O₃?0001?surface.Then,a Fe atom of the top layer of surface is replaced by one Ni atom or Co atom.We researched the effects of' doped atoms on the catalytic activity for the oxygen evolution reaction.It is found that the potential-determining step of the oxygen evolution reaction of these catalysts is the step of the formation^*O from^*OH.And we also find that the doping of Ni and Co can improve the catalytic activity of the surface.The Co atom on the Co-doped surface as the adsorption site,it has the lowest theoretical over-potential?0.63V?.In the fourth chapter,according to the first-principles theory and the reaction mechanism of oxygen evolution reaction,we studied the catalytic activities of the Fe₂O₃ cluster and Fe₄O₆ cluster,respectively.Similarly,we researched the effects of doping atoms on the catalytic activity for the oxygen evolution reaction.It is found that the potential-determining step of the oxygen evolution reaction of these catalysts is the step of the formation^*O from^*OH.And we also find that the doping of Co can improve the catalytic activity of the Fe₂O₃ cluster.The Co atom of the Co-doped cluster as the adsorption site,it has the lowest theoretical over-potential?0.67V?.In addition,we find that the doping of Ni can improve the catalytic activity of the Fe₄O cluster.The Fe atom of the Ni-doped cluster as the adsorption site,it has the lowest theoretical over-potential?0.55V?.