Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities,where the migration barrier(Em)is the governing factor.Here,we assess the accuracy and c...Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities,where the migration barrier(Em)is the governing factor.Here,we assess the accuracy and computational performance of generalized gradient approximation(GGA),the strongly constrained and appropriately normed(SCAN),and their Hubbard U corrections,GGA+U and SCAN+U,within the density functional theory-nudged elastic band framework,in the prediction of Em as benchmarked against experimental data.Importantly,we observe SCAN to be more accurate than other frameworks,on average,albeit with higher computational costs and convergence difficulties,while GGA is a feasible choice for“quick”and“qualitative”Em predictions.Further,we quantify the sensitivity of Em with adding uniform background charge and/or the climbing image approximation in solid electrolytes,and the Hubbard U correction in electrodes.Our findings will improve the quality of Em predictions which will enable identifying better materials for energy storage applications.展开更多
基金G.S.G.acknowledges financially support from the Indian Institute of Science(IISc)Seed Grant,SG/MHRD/20/0020 and SR/MHRD/20/0013 and the Science and Engineering Research Board(SERB)of the Department of Science and Technology,Government of India,under sanction number SRG/2021/000201R.D.thanks the Ministry of Human Resource Development,Government of India,for financial assistance+2 种基金B.S.and P.C.acknowledge funding from the National Research Foundation under the NRF Fellowship NRFF12-2020-0012P.C.acknowledges support from the Singapore Ministry of Education Academic Fund Tier 1(R-284-000-186-133)G.S.G.thanks the International Travel Support scheme of SERB,under sanction number ITS/2022/000391,and the Indian Institute of Metals for travel support.
文摘Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities,where the migration barrier(Em)is the governing factor.Here,we assess the accuracy and computational performance of generalized gradient approximation(GGA),the strongly constrained and appropriately normed(SCAN),and their Hubbard U corrections,GGA+U and SCAN+U,within the density functional theory-nudged elastic band framework,in the prediction of Em as benchmarked against experimental data.Importantly,we observe SCAN to be more accurate than other frameworks,on average,albeit with higher computational costs and convergence difficulties,while GGA is a feasible choice for“quick”and“qualitative”Em predictions.Further,we quantify the sensitivity of Em with adding uniform background charge and/or the climbing image approximation in solid electrolytes,and the Hubbard U correction in electrodes.Our findings will improve the quality of Em predictions which will enable identifying better materials for energy storage applications.
