Ultrahigh energy density Li-ion batteries based on cathodes of 1D metals with –Li–N–B–N– repeating units in α-LixBN2 (1 ⩽ x ⩽ 3)

Ultrahigh energy density batteries based on α-LixBN2 (1 ⩽ x ⩽ 3) positive electrode materials are predicted using density functional theory calculations. The utilization of the reversible LiBN2 + 2 Li+ + 2 e− \documentclass[12pt]{minimal}\begin{document}$\rightleftharpoons$\end{document}⇌ Li3BN2 electrochemical cell reaction leads to a voltage of 3.62 V (vs Li/Li+), theoretical energy densities of 3251 Wh/kg and 5927 Wh/l, with capacities of 899 mAh/g and 1638 mAh/cm3, while the cell volume of α-Li3BN2 shrinks only 2.8% per two-electron transfer on charge. These values are far superior to the best existing or theoretically designed intercalation or conversion-based positive electrode materials. For comparison, the theoretical energy density of a Li–O2/peroxide battery is 3450 Wh/kg (including the weight of O2), that of a Li–S battery is 2600 Wh/kg, that of Li3Cr(BO3)(PO4) (one of the best designer intercalation materials) is 1700 Wh/kg, while already commercialized LiCoO2 allows for 568 Wh/kg. α-Li3BN2 is also known as a good Li-ion conductor with experimentally observed 3 mS/cm ionic conductivity and 78 kJ/mol (≈0.8 eV) activation energy of conduction. The attractive features of α-LixBN2 (1 ⩽ x ⩽ 3) are based on a crystal lattice of 1D conjugated polymers with –Li–N–B–N– repeating units. When some of the Li is deintercalated from α-Li3BN2 the crystal becomes a metallic electron conductor, based on the underlying 1D conjugated π electron system. Thus, α-LixBN2 (1 ⩽ x ⩽ 3) represents a new type of 1D conjugated polymers with significant potential for energy storage and other applications.