Metal–organic frameworks (MOFs)
have attracted noticeable
attention as promising candidates for electrochemical energy storage.
However, the lack of electrical conductivity and the weak stability
of most MOFs result in poor electrochemical performances. Here, a
tetrathiafulvalene (TTF)-based complex, formulated as [(CuCN)2(TTF(py)4)] (1) (TTF-(py)4 = tetra(4-pyridyl)-TTF), is assembled by in situ generation of coordinated
CN– from a nontoxic source. Single-crystal X-ray
diffraction analysis reveals that compound 1 possesses
a two-dimensional layered planar structure, which is further stacked
in parallel to form a three-dimensional supramolecular framework.
The planar coordination environment of 1 is the first
example of a TTF-based MOF. Attributed to the unique structure and
redox TTF ligand, the electrical conductivity of 1 is
significantly increased by 5 orders of magnitude upon iodine treatment.
The iodine-treated 1 (1-ox) electrode displays
typical battery-type behavior through electrochemical characterizations.
The supercapattery based on the 1-ox positrode and AC
negatrode presents a high specific capacity of 266.5 C g–1 at a specific current of 1 A g–1 with a remarkable
specific energy of 62.9 Wh kg–1 at a specific power
of 1.1 kW kg–1. The excellent electrochemical performance
of 1-ox is one of the best among those reported supercapatteries,
demonstrating a new strategy for developing MOF-based electrode materials.