Hybrid density functional calculations of redox potentials and formation energies of transition metal compounds

V. L. Chevrier; S. P. Ong; R. Armiento; M. K. Y. Chan; G. Ceder

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Hybrid density functional calculations of redox potentials and formation energies of transition metal compounds

机译：过渡金属化合物氧化还原电势和形成能的混合密度泛函计算

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We compare the accuracy of conventional scmilocal density functional theory (DFT), the DFT+U method, and the Heyd-Scuseria-Ernzerhof (HSR06) hybrid functional for structural parameters, redox reaction energies, and formation energies of transition metal compounds. Conventional DFT functionals significantly underestimate redox potentials for these compounds. Zhou et al. [Phys. Rev. B 70. 235121 (2004)] addressed this issue with DFT+U and a linear-response scheme for calculating U values. We show that the Li intercalation potentials of prominent Li-ion intercalation battery materials, such as the layered Li_xA/O_2 (M = Co and Ni), Li_xTiS_2; olivine Li_xMPO_4 (M = Mn, Fe. Co, and Ni): and spinel-like Li_xMn_2O_4. Li_xTi_2O_4, are also well reproduced by HSE06, due to the self-interaction error correction from the patrtial inclusion of Hartree-Fock exchange. For formation energies, HSE06 performs well for transition metal compounds, which typically are not well reproduced by conventional DFT functionals but does not significantly improve the results of nontransi-tion metal oxides. Hence, we find that hybrid functionals provide a good alternative to DFT+U for transition metal applications when the large extra computational effort is compensated by the benefits of (ⅰ) avoiding species-specific adjustable parameters and (ⅱ) a more universal treatment of the self-interaction error that is not exclusive to specific atomic orbital projections on selected ions.

机译：我们比较了常规scmilocal密度泛函理论（DFT），DFT + U方法和Heyd-Scuseria-Ernzerhof（HSR06）杂合函数在结构参数，氧化还原反应能和过渡金属化合物形成能方面的准确性。传统的DFT功能明显低估了这些化合物的氧化还原电位。周等。 [物理Rev. B 70. 235121（2004）]通过DFT + U和用于计算U值的线性响应方案解决了这个问题。我们显示了突出的锂离子插层电池材料（例如层状Li_xA / O_2（M = Co和Ni），Li_xTiS_2）的Li插层势；橄榄石Li_xMPO_4（M = Mn，Fe.Co和Ni）：和尖晶石状的Li_xMn_2O_4。由于从Hartree-Fock交换的目录夹杂中进行的自交互误差校正，HSE06还很好地复制了Li_xTi_2O_4。对于形成能，HSE06对过渡金属化合物的性能很好，传统的DFT功能通常不能很好地复制这些金属，但不能显着改善非过渡金属氧化物的结果。因此，我们发现，当（ⅰ）避免使用特定于物种的可调参数，并且（ⅱ）对DFT + U进行更普遍的处理时，可以为混合金属应用提供很好的替代方法，从而替代了DFT + U。自相互作用误差，不是选定离子上特定原子轨道投影所独有的。

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来源
《Physical review》 |2010年第7期|p.075122.1-075122.11|共11页
作者
V. L. Chevrier; S. P. Ong; R. Armiento; M. K. Y. Chan; G. Ceder;
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Department of Materials Science and Engineering, Massachusetts Institute of Technology. Cambridge, Massachusetts 02139, USA;

rnDepartment of Materials Science and Engineering, Massachusetts Institute of Technology. Cambridge, Massachusetts 02139, USA;

rnDepartment of Materials Science and Engineering, Massachusetts Institute of Technology. Cambridge, Massachusetts 02139, USA;

rnDepartment of Materials Science and Engineering, Massachusetts Institute of Technology. Cambridge, Massachusetts 02139, USA;

rnDepartment of Materials Science and Engineering, Massachusetts Institute of Technology. Cambridge, Massachusetts 02139, USA;

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density functional theory, local density approximation, gradient and other corrections; total energy and cohesive energy calculations; strongly correlated electron systems; heavy fermions; lithium-ion batteries;

机译：密度泛函理论;局部密度近似;梯度和其他校正;总能量和内聚能计算;强相关电子系统;重费米子;锂离子电池;

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机译：过渡金属化合物氧化还原电势和形成能的混合密度泛函计算

Hybrid density functional calculations of redox potentials and formation energies of transition metal compounds

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