Construction of CoNi2S4/Co9S8@Co4S3 nanocubes derived from Ni-Co prussian blue analogues@cobalt carbonate hydroxide core–shell heterostructure for asymmetric supercapacitor

Construction of Prussian blue analogues (PBAs) with heterostructure is beneficial to preparing PBAs derivatives with superior electrochemical performance. In this work, the core–shell nanostructured nanocubes composed of nickel hexacyanocobalt PBA (NiCo-PBA)@cobalt carbonate hydroxide (CCH) are synthesized through an in-situ epitaxial growth strategy, and the formation mechanisms of coating are carefully validated and specifically discussed. Then, the precursors are successfully transformed into hierarchical CoNi2S4/Co9S8@Co4S3 via the gas-phase vulcanization method. Benefiting from the intriguing heterostructure and multicomponent sulfides, the CoNi2S4/Co9S8@Co4S3-80 electrode exhibits a high specific capacity of 799 ± 16C/g (specific capacitance of 1595 ± 31F/g) at 1 A/g, ultra-high capacity retention of 80 % at a high current density of 20 A/g. The assembled asymmetric supercapacitor (ASC) device delivers a high energy density of 43.3 Wh kg−1 at a power density of 899 W kg−1 and exhibits superior cycling stability with the capacity retention of 88 % after 5,000 cycles. Subsequently, the fabricated all-solid-state ASC device shows an excellent energy density of 36.4 Wh kg−1 with a power density of 824 W kg−1. This work proposing rational design of combining multicomponent sulfides and core–shell heterostructure based on PBA nanocubes opens up a novel route for developing asymmetric supercapacitor electrode materials with superior performance.