To meet the challenges of poor cycling performance and low specific capacity of organic electrode materials, an example of a three-dimensional manganese-based coordination polymer [Mn 2 (pztc)(H 2 O) 2 ] n (Mn-3D) was synthesized by a simple hydrothermal reaction using a redox-active organic moiety pyrazine-2,3,5,6-tetracarboxylic acid (H 4 pztc) as the linker. The Mn-3D anode material exhibited excellent lithium storage capacity to store 14 lithium ions, with a high theoretical specific capacity of 942 mA h g −1 based on density functional theory. Owing to the coordination bonds between the redox-active ligand and the metal center, Mn-3D delivered high electrolyte stability and electrical conductivity and thus the anode material could exhibit superior cycling performance with a superior reversible capacity of 692 mA h g −1 after 160 cycles at 100 mA g −1 . Experimental and theoretical analyses revealed the reversibility of the lithium storage active sites in Mn-3D during cycling. This work highlights the significance of the design of redox-active metal−organic materials as high-performance anodes of lithium-ion batteries.
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