Recent years have witnessed a booming interest in grid-scale electrochemical energy storage, where much attention has been paid to the aqueous zinc ion batteries (AZIBs). Among various cathode materials for AZIBs, manganese oxides have risen to prominence due to their high energy density and low cost. However, sluggish reaction kinetics and poor cycling stability dictate against their practical application. Herein, we demonstrate the combined use of defect engineering and interfacial optimization that can simultaneously promote rate capability and cycling stability of MnO2 cathodes. β-MnO2 with abundant oxygen vacancies (VO) and graphene oxide (GO) wrapping is synthesized, in which VO in the bulk accelerate the charge/discharge kinetics while GO on the surfaces inhibits the Mn dissolution. This electrode shows a sustained reversible capacity of ~ 129.6 mAh g−1 even after 2000 cycles at a current rate of 4C, outperforming the state-of-the-art MnO2-based cathodes. The superior performance can be rationalized by the direct interaction between surface VO and the GO coating layer, as well as the regulation of structural evolution of β-MnO2 during cycling. The combinatorial design scheme in this work offers a practical pathway for obtaining high-rate and long-life cathodes for AZIBs.

The cathode materials work as the host framework for both Li + diffusion and electron transport in Liion batteries. The Li + diffusion property is always the research focus, while the electron transport property is less studied. Herein, we propose a unique strategy to elevate the rate performance through promoting the surface electric conductivity. Specifically, a disordered rock-salt phase was coherently constructed at the surface of LiCoO 2 , promoting the surface electric conductivity by over one magnitude. It increased the effective voltage (V eff ) imposed in the bulk, thus driving more Li + extraction/insertion and making LiCoO 2 exhibit superior rate capability (154 mAh g À 1 at 10 C), and excellent cycling performance (93 % after 1000 cycles at 10 C). The universality of this strategy was confirmed by another surface design and a simulation. Our findings provide a new angle for developing high-rate cathode materials by tuning the surface electron transport property.

The spinel-type materials are promising for the cathodes in rechargeable aqueous zinc batteries. Herein, the Zn3V3O8 is synthesized via a simple solid-state reaction method. By tuning Zn(CF3SO3)2 concentration in electrolytes...

The structure instability issues of the highly delithiated LiCoO2 have significantly hindered its high‐voltage applications (≥4.55 V vs Li/Li+). Herein, for the first time, multiple modifications of Li0.9Mg0.05CoO2 (L0.9M0.05CO) via a simple one‐step sintering synthesis are reported. A combination of the bulk Li/Co antisites, a Mg‐pillar enriched surface, and a thin MgO coating layer is achieved to maintain both the bulk and surface structural stability of L0.9M0.05CO upon cycling at an upper cut‐off voltage of 4.6 V. The bulk Li/Co antisites are discovered to enhance the H1‐3 phase evolution reversibility, the Mg pillars that substitute the Li sites effectively reinforces the surface structure, and the thin MgO coating layer can effectively prevent the cathode from severe side reactions. Benefiting from the reduced but reversible H1‐3 phase transition and the reinforced surface structure, L0.9M0.05CO shows an excellent cycle stability. This work provides a new structure modulation route for developing high‐voltage LiCoO2 cathodes.

To increase the service life of rechargeable batteries, transition metal oxide hosts with high structural stability for the intercalation of carrier ions are important. Herein, we reconstruct the crystal structure of a commercial V 2 O 5 by pre-intercalating H + and H 2 O pillars using a facile hydrothermal reaction and obtain a bi-layer structured H 0.642 V 2 O 5 •0.143H 2 O (HVO) as an excellent host for aqueous Zn-ion batteries. Benefiting from the structural reconstruction, the irreversible "layer-to-amorphous" phase evolution during cycling is considerably less, resulting in ultra-high cycling stability of HVO with nearly no capacity fading even after 500 cycles at a current density of 0.5 A g −1 . Moreover, a synthetic proton and Zn 2+ intercalation mechanism in the HVO host is demonstrated. This work provides both a facile synthesis method for the preparation of V-based compounds and a new viewpoint for achieving high-performance host materials.