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[Display omitted] The effect of various types of electrolytes on the operation of coordination polymers based on NiII or CuII in lithium-ion batteries has been examined. Cyclic voltammetry, galvanostatic cycling and quantum chemical modeling have been used to study the processes of lithiation and delithiation. It was shown that the use of a new electrolyte based on a mixture of 1 M LiN(CF 3 SO 2) 2 in 1,3-dioxolane–1,2-dimethoxyethane and 1 M LiPF 6 in ethylene carbonate–dimethyl carbonate improved battery performance, while cycling in the range of 0.2–2.5 V increased the discharge capacity up to 177–188 mA h g−1 and stabilized the charge–discharge processes. [ABSTRACT FROM AUTHOR]