Unlocking the Interfacial Adsorption-Intercalation Pseudocapacitive Storage Limit to Enabling All-Climate, High Energy/Power Density and Durable Zn-Ion Batteries

Sluggish storage kinetics and insufficient performance are the major challenges that restrict the transition metal dichalcogenides (TMDs) applied for zinc ion storage, especially at the extreme temperature conditions. Herein, a multiscale interface structure-integrated modulation concept was presented, to unlock the omnidirectional storage kinetics-enhanced porous VSe2-x center dot n H2O host. Theory research indicated that the co-modulation of H2O intercalation and selenium vacancy enables enhancing the interfacial zinc ion capture ability and decreasing the zinc ion diffusion barrier. Moreover, an interfacial adsorption-intercalation pseudocapacitive storage mechanism was uncovered. Such cathode displayed remarkable storage performance at the wide temperature range (-40-60 degrees C) in aqueous and solid electrolytes. In particular, it can retain a high specific capacity of 173 mAh g(-1) after 5000 cycles at 10 A g(-1), as well as a high energy density of 290 Wh kg(-1) and a power density of 15.8 kW kg(-1) at room temperature. Unexpectedly, a remarkably energy density of 465 Wh kg(-1) and power density of 21.26 kW kg(-1) at 60 degrees C also can be achieved, as well as 258 Wh kg(-1) and 10.8 kW kg(-1) at -20 degrees C. This work realizes a conceptual breakthrough for extending the interfacial storage limit of layered TMDs to construct all-climate high-performance Zn-ion batteries.

Automated summary

This study presents a multiscale interface structure-integrated modulation concept to enhance the storage kinetics of VSe2-x · n H2O host for zinc ion storage. The intercalation of H2O and the modulation of selenium vacancy can enhance the capture ability and reduce the diffusion barrier of zinc ions. It is found that the storage mechanism involves interfacial adsorption and intercalation pseudocapacitance. The cathode exhibits excellent storage performance at a wide temperature range (-40-60 degrees C) in aqueous and solid electrolytes. High specific capacity, energy density, and power density are achieved at different temperatures. This work extends the interfacial storage limit of layered TMDs and enables the construction of all-climate high-performance Zn-ion batteries.