One-Dimensional Transition-Metal-Based Metal–Organic Assembly Engineered for Enhanced Lithium Storage

Metal–organic assemblies (MOAs), with multiple active sites and well-defined lithium transport pathways, are considered ideal electrode materials for lithium-ion batteries. However, their further development is impeded by poor structural stability and limited electronic conductivity. In this study, two isostructural one-dimensional MOAs, namely, [M(pyzdc)(H2O)2]n (M-1D, M = Co and Ni; H2pyzdc = pyrazine-2,3-dicarboxylic acid) were synthesized for lithium storage. The chain structure formed by multiple hydrogen bond interactions constitutes a three-dimensional supramolecular architecture. This unique hydrogen bond network not only enhances structural stability but also facilitates efficient electron transfer. When tested as anode materials, Co-1D and Ni-1D exhibited reversible capacities of 1003.3 and 841.3 mAh g–1 at 100 mA g–1 after 100 cycles, respectively. Theoretical calculations and kinetic analyses have elucidated the impact of electronic configuration on lithium-ion adsorption and diffusion in these MOAs, highlighting the intricate relationship between the electronic structure of MOAs and lithium storage behavior.