Zinc-iodine aqueous batteries (ZIABs) are highly attractive for grid-scale energy storage due to their high theoretical capacities, environmental friendliness, and intrinsic non-flammability. However, because of the close redox potential of Zn stripping/platting and hydrogen evolution, slight overcharge of ZIABs would induce drastic side reactions, serious safety concerns, and battery failure. A novel type of stimulus-responsive zinc-iodine aqueous battery (SR-ZIAB) with fast overcharge self-protection ability is demonstrated by employing a smart pH-responsive electrolyte. Operando spectroelectrochemical characterizations reveal that the battery failure mechanism of ZIABs during overcharge arises from the increase of electrolyte pH induced by hydrogen evolution as well as the consequent irreversible formation of insulating ZnO at anode and soluble Zn(IO 3 ) 2 at cathode. Under overcharge conditions, the designed SR-ZIABs can be rapidly switched off with capacity degrading to 6% of the initial capacity, thereby avoiding continuous battery damage. Importantly, SR-ZIABs can be switched on with nearly 100% of capacity recovery by re-adjusting the electrolyte pH. This work will inspire the development of aqueous Zn batteries with smart self-protection ability in the overcharge state.Stimulus-responsive materials and devices are attracting intensive attention because of the ever-increasing demand for intelligent devices. [1][2][3][4][5][6] In particular, integrating stimulus-responsive functions into rechargeable batteries shows great potential to revolutionize electrochemical energy storage systems for future smart devices. [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24] Currently, the three most eye-catching stimulus-responsive batteries are temperature-responsive Li-ion batteries, [11,14,16,20] photo-responsive Li-ion batteries, [7,17,18] and self-healing Li-ion batteries. [8,13,15,19] Despite the availability of aforementioned stimulus-responsive batteries, the developed stimulus responses for rechargeable batteries are still sparse owing to the complexity and compatibility of battery architectures. [24] Moreover, the reported stimulus-responsive functions are mainly integrated into Li-ion batteries. [8,[13][14][15][16][17][18][19][20] However, the limited Li resources and high flammability of Li-ion batteries severely impede their commercial applications for stationary energy storage systems. Therefore, it is highly desired to explore new stimulus-responsive systems beyond Li-ion batteries.As prospective alternatives for Li-ion batteries, rechargeable zinc-iodine aqueous batteries (ZIABs) are emerging for largescale energy storage systems because of high theoretical capacities and energy densities (around 169 mAh g −1 and 220 Wh kg −1 based on the total mass of active cathode and anode materials), abundant raw materials, environmental friendliness, non-flammable aqueous electrolytes, and simplified battery packaging technology in air. [25][26][27][28][29][30][31][32][33][34] However, ZIABs su...
Among various charge-carrier ions for aqueous batteries, non-metal hydronium (H 3 O +) with small ionic size and fast diffusion kinetics empowers H 3 O +-intercalation electrodes with high rate performance and fast-charging capability. However, pure H 3 O + charge carriers for inorganic electrode materials have only been observed in corrosive acidic electrolytes, rather than in mild neutral electrolytes. Herein, we report how selective H 3 O + intercalation in a neutral ZnCl 2 electrolyte can be achieved for water-proton co-intercalated a-MoO 3 (denoted WP-MoO 3). H 2 O molecules located between MoO 3 interlayers block Zn 2+ intercalation pathways while allowing smooth H 3 O + intercalation/diffusion through a Grotthuss proton-conduction mechanism. Compared to a-MoO 3 with a Zn 2+-intercalation mechanism, WP-MoO 3 delivers the substantially enhanced specific capacity (356.8 vs. 184.0 mA h g À1), rate capability (77.5 % vs. 42.2 % from 0.4 to 4.8 A g À1), and cycling stability (83 % vs. 13 % over 1000 cycles). This work demonstrates the possibility of modulating electrochemical intercalating ions by interlayer engineering, to construct high-rate and long-life electrodes for aqueous batteries.
The advancement of flexible rechargeable Zn–MnO2 batteries largely relies on directional design and fabrication of flexible cathode materials. However, the sluggish electron transfer and inferior mass diffusion rate of MnO2 cathodes hinder their application in high‐power systems. Herein, the design of flexible 3D carbon nanotube (CNT) conductive networks as excellent electron and charge transfer substrates is reported to achieve a high‐rate MnO2 cathode. With further structural protection of conductive poly(3,4‐ethylenedioxythiophene) (PEDOT), Zn2+ storage kinetics in the composite CNT/MnO2/PEDOT (denoted as CMOP) the cathode is optimized to deliver high capacity of 306.1 mAh g−1 at 1.1 A g−1 and superior rate capability of 176.8 mAh g−1 when the current density increases by tenfold (10.8 A g−1), representing a state‐of‐the‐art of current MnO2 based cathodes. Moreover, the as‐assembled quasi‐solid‐state Zn–CMOP batteries with good mechanical properties can afford a high energy density of 379.4 Wh kg−1 (17.5 mWh cm−3) and a peak power density of 17.1 kW kg−1 (0.8 W cm−3). This innovative achievement will be a critical step forward toward next‐generation quick charging electronics.
A La–Ca co-doping strategy is employed to boost the energy density of ε-MnO2 cathode. The assembled Zn//ε-MnO2 battery can achieve an maximum energy of 401.22 W h kg−1.
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