Multi-redox organic and organometallic electrode materials have been emerging alternatives to the widespread inorganic counterparts in advanced power sources due to their design diversity, light weight, flexibility, and environmental benignity.1 However, their electrically insulating nature, limited capacity, and poor durability should be resolved for the practical application.Here, we present a one-dimensional (1D) nanohybrid composed of a multiwalled carbon nanotube (MWCNT) core and a cobalt porphyrin shell (Figure) as a new class of electrode materials for rechargeable lithium batteries.2 Highly π-conjugated and multielectron redox-active meso-tetrakis(4-carboxyphenyl) porphyrinato cobalt (CoTCPP) shows strong noncovalent interactions with the MWCNT, leading to the successful formation of the 1D nanohybrid. The resultant nanohybrid, due to its structural uniqueness and maximal use of active areas, facilitates electron transport and electrolyte accessibility, which thus contribute to exhibiting a high specific capacity and improving redox kinetics. Furthermore, intrigued by the 1D structure of the nanohybrid, an all-fibrous nanomat electrode was fabricated through concurrent electro-spraying/-spinning processes. The nanomat electrode provides bicontinuous electron and ion conduction pathways, which eventually reveals the well-distinguishable lithiation behavior of CoTCPP and exceptional electrochemical performances with a long-term stability (ca. 226 mAh g ‒1 based on the electrode sheet weight at a current density of 5 C for over 1500 electrochemical cycles).We hope that the material design strategy described in this study offers new insight into the development of high-performance electrode materials for next-generation power sources and energy storage systems.
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