To solve energy‐related environmental problems and the energy crisis, efficient electrochemical materials have been developed as alternative energy storage and conversion systems. Abundant transition metals and their sulfides are attractive electrochemical materials. Herein, we report an efficient phosphorization strategy, which improves the overall electrochemical performance of metal sulfides. In detail, CoS hexagonal bipyramids were synthesized through simple calcination combined with in situ sulfurization of a cobalt‐based metal–organic framework template, and then phosphate ion‐functionalized CoS (P‐CoS) was prepared through a phosphorization reaction. P‐CoS exhibited outstanding electrochemical activity as both supercapacitor electrode and oxygen evolution reaction (OER) catalyst. Supercapacitors based on CoS and P‐CoS as the electrodes had high specific capacitances of 304 and 442 F g−1, respectively, and remained stable for over 10 000 cycles at 5 A g−1. For OER, P‐CoS showed a current density of 10 mA cm−2 at an overpotential of 340 mV, with a small Tafel slope. In conclusion, functionalizing CoS with phosphate ions is a promising method for enhancing chemical reactivity and accelerating ion and electron transfer. [ABSTRACT FROM AUTHOR]
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