Theoretical Study On Novel Two-dimensional ZrSiSe Monolayer Structure And Its High Efficiency Catalytic Performance For Oxygen Reduction Reaction

With the rapid development of global industrialization,the massive consumption of fossil energy fuels and the destruction of the environment by combustion products are becoming more and more severe,the exploitation of sustainable and clean new energy has attracted great attention.Among them,hydrogen energy stands out because of its high energy density and zero carbon emissions.At the same time,advanced and efficient energy conversion devices such as hydrogen-oxygen fuel cells have gradually become a research hotspot.However,the oxygen reduction reaction（ORR）occurring at the cathode of fuel cells greatly limits the conversion efficiency due to the slow kinetics.Therefore,it is very important to develop new ORR catalysts with low cost and high catalytic activity.Owing to the increasing perfection of theoretical computational chemistry,density functional theory（DFT）combined with high-performance computer technology is playing an important role in the search for novel catalysts.In this work,we systematically investigate the structure,stability and ORR catalytic activity of 2D non-noble metal Zr Si Se monolayer based on DFT calculations.It is found that two-dimensional Zr Si Se monolayer can be obtained by exfoliation from bulk structure with layered stacking.It has excellent kinetic,thermodynamic,mechanical stability and good electrical conductivity,which are very beneficial to the ORR catalytic performance of the material.Further studies show that the system can exhibit excellent ORR catalytic performance with an overpotential of only 0.33 V and good four-electron selectivity.In addition,doping transition metal atoms not only keeps the low overpotential of the system,but also effectively improves the ability to capture oxygen,and further improves the selectivity of the four-electron reduction pathway in the reaction process,which can more effectively prevents the formation of by-product H₂O₂.In conclusion,this work can provide valuable theoretical basis for the design and subsequent experimental studies of novel inexpensive and efficient ORR electrocatalysts based on 2D nanosystems.