典型文献
Understanding the Effect of the Exchange-Correlation Functionals on Methane and Ethane Formation over Ruthenium Catalysts
文献摘要：
Density functional theory(DFT)has been es-tablished as a powerful research tool for het-erogeneous catalysis research in obtaining key thermodynamic and/or kinetic parameters like adsorption energies,enthalpies of reaction,ac-tivation barriers,and rate constants.Un-derstanding of density functional exchange-correlation approximations is essential to re-veal the mechanism and performance of a cata-lyst.In the present work,we reported the influ-ence of six exchange-correlation density func-tionals,including PBE,RPBE,BEEF+vdW,optB86b+vdW,SCAN,and SCAN+rVV10,on the adsorption energies,reaction energies and activation barriers of carbon hydrogenation and carbon-carbon couplings during the formation of methane and ethane over Ru(0001)and Ru(10(1)1)surfaces.We found the calculated reaction energies are strongly dependent on exchange-correlation density func-tionals due to the difference in coordination number between reactants and products on sur-faces.The deviation of the calculated elementary reaction energies can be accumulated to a large value for chemical reaction involving multiple steps and vary considerably with differ-ent exchange-correlation density functionals calculations.The different exchange-correlation density functionals are found to influence considerably the selectivity of Ru(0001)surface for methane,ethylene,and ethane formation determined by the adsorption energies of interme-diates involved.However,the influence on the barriers of the elementary surface reactions and the structural sensitivity of Ru(0001)and Ru(10(1)1)are modest.Our work highlights the limitation of exchange-correlation density functionals on computational catalysis and the im-portance of choosing a proper exchange-correlation density functional in correctly evaluating the activity and selectivity of a catalyst.
文献关键词：
中图分类号：
作者姓名：
Chen Chen;Minzhen Jian;Jin-Xun Liu;Wei-Xue Li
作者机构：
Department of Chemical Physics,School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230026,China
文献出处：
引用格式：
[1]Chen Chen;Minzhen Jian;Jin-Xun Liu;Wei-Xue Li-.Understanding the Effect of the Exchange-Correlation Functionals on Methane and Ethane Formation over Ruthenium Catalysts)[J].化学物理学报（英文版）,2022(04):619-628
A类：
Functionals,tionals,RPBE,BEEF+vdW,optB86b+vdW,SCAN+rVV10
B类：
Understanding,Effect,Exchange,Correlation,Methane,Ethane,Formation,over,Ruthenium,Catalysts,Density,theory,DFT,has,been,tablished,powerful,research,tool,het,erogeneous,catalysis,obtaining,key,thermodynamic,kinetic,parameters,like,adsorption,energies,enthalpies,barriers,rate,constants,density,exchange,correlation,approximations,essential,veal,mechanism,performance,In,present,work,reported,six,including,activation,carbon,hydrogenation,couplings,during,formation,methane,surfaces,We,found,calculated,are,strongly,dependent,due,difference,coordination,number,between,reactants,products,deviation,elementary,can,accumulated,large,value,chemical,involving,multiple,steps,vary,considerably,functionals,calculations,different,influence,selectivity,ethylene,determined,by,interme,diates,involved,However,reactions,structural,sensitivity,modest,Our,highlights,limitation,computational,portance,choosing,proper,correctly,evaluating,activity,catalyst
AB值：
0.464165
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