Bond modulation of MoSe2+x driving combined intercalation and conversion reactions for high-performance K cathodes

Abstract

The urgent demand for large-scale global energy storage systems and portable electronic devices is driving the need for considerable energy density and stable batteries. Here, Se atoms are introduced between MoSe₂ layers (denoted as MoSe_2+x) by bond modulation to produce a high-performance cathode for potassium-ion batteries. The introduced Se atoms form covalent Se–Se bonds with the Se in MoSe₂, and the advantages of bond modulation are as follows: (i) the interlayer spacing is enlarged which increases the storage space of K⁺; (ii) the system possesses a dual reaction mechanism, and the introduced Se can provide an additional conversion reaction when discharged to 0.5 V, which improves the capacity further; (iii) the Se atoms confined between MoSe₂ layers do not give rise to the shuttle effect. MoSe_2+x is compounded with rGO (MoSe_2+x-rGO) as a cathode for potassium-ion batteries and displays an ultrahigh capacity (235 mA h g⁻¹ at 100 mA g⁻¹), a long cycle life (300 cycles at 100 mA g⁻¹) and an extraordinary rate performance (135 mA h g⁻¹ at 1000 mA g⁻¹ and 89 mA h g⁻¹ at 2000 mA g⁻¹). Pairing the MoSe_2+x-rGO cathode with graphite, the full cell delivers considerable energy density compared to other K cathode materials. The MoSe_2+x-rGO cathode also exhibits excellent electrochemical performance for lithium-ion batteries. This study on bond modulation driving combined intercalation and conversion reactions offers new insights into the design of high-performance K cathodes.