Nanostructured materials have shown extraordinary promise for electrochemical energy storage but are usually limited to electrodes with rather low mass loading (~1 milligram per square centimeter) because of the increasing ion diffusion limitations in thicker electrodes. We report the design of a three-dimensional (3D) holey-graphene/niobia (NbO) composite for ultrahigh-rate energy storage at practical levels of mass loading (>10 milligrams per square centimeter). The highly interconnected graphene network in the 3D architecture provides excellent electron transport properties, and its hierarchical porous structure facilitates rapid ion transport. By systematically tailoring the porosity in the holey graphene backbone, charge transport in the composite architecture is optimized to deliver high areal capacity and high-rate capability at high mass loading, which represents a critical step forward toward practical applications.

Recent attention has been focused on the synthesis and application of complex heter ostructured nanomaterials, which can have superior electrochemical performance than singlestructured materials. Here we synthesize the threedimensional (3D) multicomponent oxide, mnmoo 4 /Comoo 4 . Hierarchical heterostructures are successfully prepared on the backbone material mnmoo 4 by a simple refluxing method under mild conditions; and surface modification is achieved. We fabricate asymmetric supercapacitors based on hierarchical mnmoo 4 /Comoo 4 heterostructured nanowires, which show a specific capacitance of 187.1 F g − 1 at a current density of 1 A g − 1 , and good reversibility with a cycling efficiency of 98% after 1,000 cycles. These results further demonstrate that constructing 3D hierarchical heterostructures can improve electrochemical properties. 'oriented attachment' and 'selfassembly' crystal growth mechanisms are proposed to explain the formation of the heterostructures.

The development of manganese dioxide as the cathode for aqueous Zn-ion battery (ZIB) is limited by the rapid capacity fading and material dissolution. Here, a highly reversible aqueous ZIB using graphene scroll-coated α-MnO as the cathode is proposed. The graphene scroll is uniformly coated on the MnO nanowire with an average width of 5 nm, which increases the electrical conductivity of the MnO nanowire and relieves the dissolution of the cathode material during cycling. An energy density of 406.6 Wh kg (382.2 mA h g ) at 0.3 A g can be reached, which is the highest specific energy value among all the cathode materials for aqueous Zn-ion battery so far, and good long-term cycling stability with 94% capacity retention after 3000 cycles at 3 A g are achieved. Meanwhile, a two-step intercalation mechanism that Zn ions first insert into the layers and then the tunnels of MnO framework is proved by in situ X-ray diffraction, galvanostatic intermittent titration technique, and X-ray photoelectron spectroscopy characterizations. The graphene scroll-coated metallic oxide strategy can also bring intensive interests for other energy storage systems.

Among the aqueous rechargeable batteries, Zn 2+ -based batteries exhibit a series of unique attributes for large-scale energy storage: (i) feasibility of using low-cost Zn metal anode with a high theoretical specific capacity of 819 mA h g −1 ; (ii) replacement of the traditional alkaline electrolytes by mild neutral electrolytes, mitigating the environmental disruption and recycling costs; and (iii) low redox potential of Zn/Zn 2+ (−0.76 V vs standard hydrogen electrode) and two-electron transfer mechanism during cycling responsible for the high energy density. [6,22,23] However, the zinc system also has long-standing challenges, such as the unstable cathode and anode structures in the aqueous environment. On the cathode side, the cycling stability is related to how zinc ions and the electrolyte react with the cathode materials, which is much more complex as compared to the lithium-ion systems. An initial attempt on the hexacyanoferrate system delivered a limited capacity (≈60 mA h g −1 ), although a high operation voltage of ≈1.7 V was achieved. [23][24][25][26][27][28] Recently, Pan et al. demonstrated that the manganese oxide cathode goes through a chemical conversion reaction with the zinc species and H 2 O rather than the simple intercalation process, delivering a high capacity of ≈285 mA h g −1 and an operating voltage of ≈1.44 V. [29] Nazar's group developed a Zn 0.25 V 2 O 5 ·nH 2 O cathode material, which displayed a specific energy of ≈250 Wh kg −1 (based on cathode) and a high capacity of 220 mA h g −1 at 15 C (1 C = 300 mA g −1 ). [30] During cycling, the structural water in Zn 0.25 V 2 O 5 ·nH 2 O was revealed to exchange with Zn 2+ reversibly, thus resulting in good kinetics and rate performance. Furthermore, some other studies have also suggested the importance of H 2 O in metal ion intercalation. [23,31] During cycling, the solvating H 2 O works as a charge shield for the metal ions (Al 3+ , Mg 2+ , Li + , etc.), reducing their effective charges and hence their interactions with the host frameworks. [32,33] This strategy has been investigated to enhance the capacity and rate capability of Li + , Na + , and Mg 2+ batteries. [34][35][36][37][38][39] In this paper, we present a systematic and detailed study of the role of H 2 O in bilayer V 2 O 5 ·nH 2 O (n ≥ 1) as a prototype cathode material for zinc batteries. By coupling the electrochemical measurements, thermogravimetric/differential BatteriesLarge-scale energy storage systems are critical for the integration of renewable energy and electric energy infrastructures. [1][2][3] Among numerous candidates, lithium-ion batteries with organic electrolytes are one of the most attractive options due to their high energy density [4][5][6][7][8][9][10] and mature markets. [11,12] However, for grid scale energy storage, the cost of lithium-ion batteries is still too high, [13,14] and the use of the flammable organic electrolyte in large format batteries poses a severe safety and environmental concern. [15] As an alternative, low-cost aqueous batteries wi...

Aqueous Zn‐ion batteries (ZIBs) have received incremental attention because of their cost‐effectiveness and the materials abundance. They are a promising choice for large‐scale energy storage applications. However, developing suitable cathode materials for ZIBs remains a great challenge. In this work, pioneering work on the designing and construction of aqueous Zn//Na0.33V2O5 batteries is reported. The Na0.33V2O5 (NVO) electrode delivers a high capacity of 367.1 mA h g−1 at 0.1 A g−1, and exhibits long‐term cyclic stability with a capacity retention over 93% for 1000 cycles. The improvement of electrical conductivity, resulting from the intercalation of sodium ions between the [V4O12]n layers, is demonstrated by single nanowire device. Furthermore, the reversible intercalation reaction mechanism is confirmed by X‐ray diffraction, Raman, X‐ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy analysis. The outstanding performance can be attributed to the stable layered structure and high conductivity of NVO. This work also indicates that layered structural materials show great potential as the cathode of ZIBs, and the indigenous ions can act as pillars to stabilize the layered structure, thereby ensuring an enhanced cycling stability.