Unlocking the Interfacial Adsorption-Intercalation Pseudocapacitive Storage Limit to Enabling All-Climate, High...

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 VSe_2-x ⋅n H₂ O host. Theory research indicated that the co-modulation of H₂ O 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 °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 °C also can be achieved, as well as 258 Wh kg^-1 and 10.8 kW kg^-1 at -20 °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.