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Aqueous batteries with high safety and cost efficiency usually employ metallic cations as charge carriers. Recently, ammonium (NH4+) ion batteries using the nonmetal NH4+ as a charge carrier exhibit distinct electrochemical features from conventional aqueous batteries. Herein, the electrochemical performances of a bimetallic hydroxide material are systematically studied with different charge carriers in the electrolytes, including NH4+, as well as the conventional monovalent metallic cations K+ and Na+, respectively. Electrochemical results indicate that the charge storage process using NH4+ as the working ions exhibits a higher discharge plateau, smaller electrochemical polarization, and larger discharge capacity than that using conventional metallic charge carriers. Experimental characterizations and theoretical calculations suggest that the strong interaction between NH4+ and the electrode material, as well as the low NH4+‐ion diffusion barrier lead to these superior electrochemical features. The assembled NH4+‐ion battery exhibits a good energy density of 123 Wh kg(cathode+anode)−1 at the power density of 480 W kg(cathode+anode)−1. These fundamental findings are important for developing good safety, low‐cost, and high‐energy aqueous batteries with sustainable NH4+ charge carriers. [ABSTRACT FROM AUTHOR]

The limited choice of anode materials always challenges the development of high performance aqueous ammonium-ion batteries (AAIBs). Herein, we fabricate amorphous molybdenum oxide (MoOx) materials and study the NH4+ storage performances. The results indicate that the optimized electrode exhibits high gravimetric/areal capacities of 175 mA h g−1/1.30 mA h cm−2, outperforming state-of-the-art anode materials for AAIBs. Our findings indicate that the valence state of Mo and the Mo–O–H content in MoOx synergistically control the NH4+ storage performances, offering new understanding for rational design of MoOx materials for energy storage applications. [ABSTRACT FROM AUTHOR]

Manganese (Mn) oxides are promising cathode materials for rechargeable aqueous Zn‐ion batteries. However, the Mn dissolution in weakly acidic electrolytes always hinders the development of better aqueous Zn–Mn batteries. Herein, a hydroxylated manganese oxide cathode material (H‐MnO2) is fabricated using an electrochemical method for stable aqueous Zn–Mn batteries without relying on the Mn2+ electrolyte additives. The partial hydroxylation of the oxides leads to charge redistribution of the material, changing the reaction thermodynamics and kinetics. Theoretical simulation suggests that the hydroxylation of manganese oxide promotes both Zn2+ adsorption thermodynamics and diffusion kinetics on the surface of H‐MnO2 but weakens the interaction between H+ and the electrode. Therefore, Zn2+ ions can be more reactive with the hydroxylated manganese oxide than H+ ions. Experimental results show that the Zn2+ insertion mechanism dominates the charge storage process of H‐MnO2, and the H+‐induced Mn dissolution reaction is effectively alleviated. Importantly, H‐MnO2 exhibits good cycling stability with 95% capacity retention over 5000 cycles at the current density of 3.8 A g−1 in the ZnSO4 electrolyte, outperforming the state‐of‐the‐art aqueous Zn–Mn batteries, even those with Mn2+ electrolyte additives. The findings provide new insights for designing stable manganese oxide cathodes in aqueous Zn–Mn batteries. [ABSTRACT FROM AUTHOR]

There has been a growing interest in developing catalysts to enable the reversible iodine conversion reaction for high-performance aqueous zinc-iodine batteries (AZIBs). While diatomic catalysts (DACs) have demonstrated superior performance in various catalytic reactions due to their ability to facilitate synergistic charge interactions, their application in AZIBs remains unexplored. Herein, we present, for the first time, a DAC comprising Mn-Zn dual atoms anchored on a nitrogen-doped carbon matrix (MnZn-NC) for iodine loading, resulting in a high-performance AZIB with a capacity of 224 mAh g-1 at 1 A g-1 and remarkable cycling stability over 320,000 cycles. The electron hopping along the Mn-N-Zn bridge is stimulated via a spin exchange mechanism. This process broadens the Mn 3dxy band width and enhances the metallic character of the catalyst, thus facilitating charge transfer between the catalysts and reaction intermediates. Additionally, the increased electron occupancy within the d-orbital of Zn elevates Zn's d-band center, thereby enhancing chemical interactions between MnZn-NC and I-based species. Furthermore, our mechanism demonstrates potential applicability to other Metal-Zn-NC DACs with spin-polarized atoms. Our work elucidates a clear mechanistic understanding of diatomic catalysts and provides new insights into catalyst design for AZIBs., (© 2024 Wiley‐VCH GmbH.)

Rechargeable aqueous Zn-VO x batteries are attracting attention in large scale energy storage applications. Yet, the sluggish Zn 2+ diffusion kinetics and ambiguous structure-property relationship are always challenging to fulfil the great potential of the batteries. Here we electrodeposit vanadium oxide nanobelts (VO-E) with highly disordered structure. The electrode achieves high capacities (e.g., ≈5 mAh cm -2 , 516 mAh g -1 ), good rate and cycling performances. Detailed structure analysis indicates VO-E is composed of integrated amorphous-crystalline nanoscale domains, forming an efficient heterointerface network in the bulk electrode, which accounts for the good electrochemical properties. Theoretical calculations indicate that the amorphous-crystalline heterostructure exhibits the favorable cation adsorption and lower ion diffusion energy barriers compared to the amorphous and crystalline counterparts, thus accelerating charge carrier mobility and electrochemical activity of the electrode., (© 2023 Wiley-VCH GmbH.)

The limited choice of anode materials always challenges the development of high performance aqueous ammonium-ion batteries (AAIBs). Herein, we fabricate amorphous molybdenum oxide (MoO x ) materials and study the NH 4 + storage performances. The results indicate that the optimized electrode exhibits high gravimetric/areal capacities of 175 mA h g -1 /1.30 mA h cm -2 , outperforming state-of-the-art anode materials for AAIBs. Our findings indicate that the valence state of Mo and the Mo-O-H content in MoO x synergistically control the NH 4 + storage performances, offering new understanding for rational design of MoO x materials for energy storage applications.