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Quantitative predictions of the Li intercalation voltage and of theelectronic properties of rechargeable battery cathode materials are asubstantial challenge for first-principles theory due to the possibility of (1)strong correlations associated with localized transition metal $d$ electronsand (2) significant van der Waals (vdW) interactions in layered systems, bothof which are not accurately captured by standard approximations to densityfunctional theory (DFT). Here, we perform a systematic benchmark of electronicstructure methods based on the widely-used generalized gradient approximationof Perdew, Burke, and Ernzerhof (PBE) and the new strongly constrained andappropriately normed (SCAN) meta-generalized gradient approximation for batterycathode materials. Studying layered Li$_x$TiS$_2$, Li$_x$NiO$_2$, andLi$_x$CoO$_2$, olivine Li$_x$FePO$_4$, and spinel Li$_x$Mn$_2$O$_4$, we computethe voltage, crystal structure, and electronic structure with and withoutextensions to incorporate on-site Hubbard interactions and vdW interactions.Within pure DFT (i.e., without corrections for on-site Hubbard interactions),SCAN is a significant improvement over PBE for describing cathode materials,decreasing the mean absolute voltage error by more than 50%. Although explicitvdW interactions are not critical and in cases even detrimental when applied inconjunction with SCAN, Hubbard $U$ corrections are still in general necessaryto achieve reasonable agreement with experiment. We show that no single methodconsidered here can accurately describe the voltage and overall structural,electronic, and magnetic properties (i.e., errors no more than 5% for voltage,volume, band gap, and magnetic moments) of battery cathode materials,motivating a strong need for improved electronic structure approaches for suchsystems.

physical review materials

Prediction of Li intercalation voltages in rechargeable battery cathode  materials: effects of exchange-correlation functional, van der Waals  interactions, and Hubbard $U$