A new design strategy for redox-active molecular assemblies with crystalline porous structures for lithium-ion batteries†
A new design strategy for high-performance organic cathode active materials for lithium-ion batteries is presented, which involves the assembly of redox-active organic molecules with a crystalline porous structure using mixed-stacked charge-transfer (CT) complexes. Hexahydroxytriphenylene was used as a donor molecule and 1,4,5,8,9,12-hexaazatriphenylene-2,3,6,7,10,11-hexacarbonitrile as an acceptor molecule to give a new porous CT complex (PCT-1) with a pseudo-hexagonal mixed columnar structure. X-ray diffraction measurements and sorption experiments demonstrated that the intercolumnar spaces in PCT-1 can incorporate various molecules accompanied by lattice expansion. A lithium metal battery containing PCT-1 as a cathode active material exhibited a high capacity of 288 mA h g−1 at 500 mA g−1, and this performance was attributed to a combination of the redox-active units and the porous structure of PCT-1.