Reconstructing Vanadium Oxide with Anisotropic Pathways for a Durable and Fast Aqueous K-Ion Battery

Abstract

Aqueous potassium-ion batteries are long-term pursued, due to their excellent performance and intrinsic superiority in safe, low-cost storage for portable and grid-scale applications. However, the notorious issues of K-ion battery chemistry are the inferior cycling stability and poor rate performance, due to the inevitably destabilization of the crystal structure caused by K-ions with pronouncedly large ionic radius. Here, we resolve such issues by reconstructing commercial vanadium oxide (α-V2O5) into the bronze form, i.e., δ-K0.5V2O5 (KVO) nanobelts, as cathode materials with layered structure of enlarged space and anisotropic pathways for K-ion storage. Specifically, it can deliver a high capacity as 116 mAh g–1 at the 1 C-rate, an outstanding rate capacity of 65 mAh g–1 at 50 C, and a robust cyclic stability with 88.2% capacity retention after 1,000 cycles at 1 C. When coupled with organic anode in a full-cell configuration, the KVO electrodes can output 95 mAh g–1 at 1 C and cyclic stability with 77.3% capacity retention after 20,000 cycles at 10 C. According to experimental and calculational results, the ultradurable cyclic performance is assigned to the robust structural reversibility of the KVO electrode, and the ultrahigh-rate capability is attributed to the anisotropic pathways with improved electrical conductivity in KVO nanobelts. In addition, applying a 22 M KCF3SO3 water-in-salt electrolyte can impede the dissolving issues of the KVO electrode and further stabilize the battery cyclic performance. Lastly, the as-designed AKIBs can operate with superior low-temperature adaptivity even at −30 °C. Overall, the KVO electrode can serve as a paradigm toward developing more suitable electrode materials for high-performance AKIBs.

Aqueous organic anode//iodine cascadable battery with ultra-long lifespan, high energy and power density

“…Conversely, the intensity of K 2p peaks at the fully discharged state declined sharply and almost vanished when compared with that at the fully charged state, verifying the reversible de-intercalation of K + from PTCDI. 31,34,42,44 Distinct from the pristine state, a new peak (532.6 eV) corresponding to the C − O species at the fully charged state was clearly observed, verifying the conversion of C = O to C − O species (Fig. 3e).…”

“…As shown in Fig. 2i, the demonstrated rate capability of the full cell surpasses all reported I 2 -based cathode batteries 3, 5, 6, 16-21, 47, 49-54 and ARKFBs 38, [40][41][42] , representing the highest level thus far. As presented in Fig.…”

“…Clearly, PTCDI (3,4,9,10-Perylenetetracarboxylic diimide) displays the lowest redox potential and highest speci c capacity, thus holding a great promise as anode in the aqueous KCl electrolyte. 34,42 X − ray diffraction (XRD) and Fourier transform infrared (FT-IR) spectroscopy were performed to determine the crystal structure and functional groups of PTCDI (Fig. S2).…”

“…2, 3, 5 As for the PTCDI anode, the anodic and cathodic peaks correspond to the stepwise intercalation and de-intercalation of K + . 34,42,44 The typical galvanostatic charge/discharge (GCD) curve displays a major plateau at 1.90 V during the discharge process (Fig. 2d).…”

“…2d). Impressively, the voltage plateau of the PTCDI//I 2 full cell is of considerable superiority to that of all reported aqueous rechargeable Zn//I 2 , 3,5,6,[18][19][20][21]47 Fe//I 2 16 , Al//I 2 , 17 H 2 //I 2 , 48 and most aqueous rechargeable K + full battery systems (ARKFBs), [38][39][40][41][42] making it a promising prospect for high-energy output (Fig. 2e).…”