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Rechargeable Li−Cl2 battery is a promising high energy density battery system. However, reasonable cycle life could only be achieved under low specific capacities due to the sluggish oxidation of LiCl to Cl2. Herein, we propose an amine‐functionalized covalent organic framework (COF) with catalytic activity, namely COF−NH2, that significantly decreases the oxidation barrier of LiCl and accelerates the oxidation kinetics of LiCl in Li−Cl2 cell. The resulting Li−Cl2 cell using COF−NH2 (Li−Cl2@COF−NH2) simultaneously exhibits low overpotential, ultrahigh discharge capacity up to 3500 mAh/g and a promoted utilization ratio of deposited LiCl at the first cycle (UR−LiCl) of 81.4 %, which is one of the highest reported values to date. Furthermore, the Li−Cl2@COF−NH2 cell could be stably cycled for over 200 cycles when operating at a capacity of 2000 mAh/g at −20 °C with a Coulombic efficiency (CE) of ≈100 % and a discharge plateau of 3.5 V. Our superior Li−Cl2 batteries enabled by organocatalyst enlighten an arena towards high‐energy storage applications. [ABSTRACT FROM AUTHOR]

Rechargeable Li−Cl2 battery is a promising high energy density battery system. However, reasonable cycle life could only be achieved under low specific capacities due to the sluggish oxidation of LiCl to Cl2. Herein, we propose an amine‐functionalized covalent organic framework (COF) with catalytic activity, namely COF−NH2, that significantly decreases the oxidation barrier of LiCl and accelerates the oxidation kinetics of LiCl in Li−Cl2 cell. The resulting Li−Cl2 cell using COF−NH2 (Li−Cl2@COF−NH2) simultaneously exhibits low overpotential, ultrahigh discharge capacity up to 3500 mAh/g and a promoted utilization ratio of deposited LiCl at the first cycle (UR−LiCl) of 81.4 %, which is one of the highest reported values to date. Furthermore, the Li−Cl2@COF−NH2 cell could be stably cycled for over 200 cycles when operating at a capacity of 2000 mAh/g at −20 °C with a Coulombic efficiency (CE) of ≈100 % and a discharge plateau of 3.5 V. Our superior Li−Cl2 batteries enabled by organocatalyst enlighten an arena towards high‐energy storage applications. [ABSTRACT FROM AUTHOR]

Metallic zinc (Zn) is considered as one of the most attractive anode materials for the post‐lithium metal battery systems owing to the high theoretical capacity, low cost, and intrinsic safety. However, the Zn dendrites and parasitic side reaction impede its application. Herein, we propose a new principle of regulating p‐band center of metal oxide protective coating to balance Zn adsorption energy and migration energy barrier for effective Zn deposition and stripping. Experimental results and theoretical calculations indicate that benefiting from the uniform zincophilic nucleation sites and fast Zn transport on indium tin oxide (ITO), highly stable and reversible Zn anode can be achieved. As a result, the I−Zn symmetrical cell achieves highly reversible Zn deposition/stripping with an extremely low overpotential of 9 mV and a superior lifespan over 4000 h. The Cu/I−Zn asymmetrical cell exhibits a long lifetime of over 4000 cycles with high average coulombic efficiency of 99.9 %. Furthermore, the assembled I−Zn/AC full cell exhibits an excellent lifetime for 70000 cycles with nearly 100 % capacity retention. This work provides a general strategy and new insight for the construction of efficient Zn anode protection layer. [ABSTRACT FROM AUTHOR]

Metallic zinc (Zn) is considered as one of the most attractive anode materials for the post‐lithium metal battery systems owing to the high theoretical capacity, low cost, and intrinsic safety. However, the Zn dendrites and parasitic side reaction impede its application. Herein, we propose a new principle of regulating p‐band center of metal oxide protective coating to balance Zn adsorption energy and migration energy barrier for effective Zn deposition and stripping. Experimental results and theoretical calculations indicate that benefiting from the uniform zincophilic nucleation sites and fast Zn transport on indium tin oxide (ITO), highly stable and reversible Zn anode can be achieved. As a result, the I−Zn symmetrical cell achieves highly reversible Zn deposition/stripping with an extremely low overpotential of 9 mV and a superior lifespan over 4000 h. The Cu/I−Zn asymmetrical cell exhibits a long lifetime of over 4000 cycles with high average coulombic efficiency of 99.9 %. Furthermore, the assembled I−Zn/AC full cell exhibits an excellent lifetime for 70000 cycles with nearly 100 % capacity retention. This work provides a general strategy and new insight for the construction of efficient Zn anode protection layer. [ABSTRACT FROM AUTHOR]

An amine‐functionalized covalent organic framework with catalytic activity is demonstrated to significantly decrease the oxidation barrier and accelerate the oxidation kinetics of LiCl in a rechargeable Li‐Cl2 battery. The developed battery exhibits low overpotential and ultrahigh discharge capacity with good stability in a wide temperature range, as reported by Wei Chen, Shenxiang Zhang et al. in their Research Article (e202315931)...By Yan Xu; Mingming Wang; Muhammad Sajid; Yahan Meng; Zehui Xie; Lidong Sun; Jian Jin; Wei Chen and Shenxiang ZhangReported by Author; Author; Author; Author; Author; Author; Author; Author; Author [Extracted from the article]

Aqueous zinc–chlorine battery with high discharge voltage and attractive theoretical energy density is expected to become an important technology for large‐scale energy storage. However, the practical application of Zn–Cl2 batteries has been restricted due to the Cl2 cathode with sluggish kinetics and low Coulombic efficiency (CE). Here, an aqueous Zn–Cl2 battery using an inexpensive and effective MnO2 redox adsorbent (referred to Zn‐Cl2@MnO2 battery) to modulate the electrochemical performance of the Cl2 cathode is developed. Density functional theory calculations reveal that the existence of the intermediate state Clads free radical catalyzed by MnO2 on the Cl2 cathode contributes to the charge storage capacity, which is the key to modulate the electrode and improve the electrochemical performance. Further analysis of the Cl2 cathode kinetics discloses the adsorption and catalytic roles of the MnO2 redox adsorbent. The Zn–Cl2@MnO2 battery displays an enhanced discharge voltage of 2.0 V at a current density of 2.5 mA cm−2, and stable 1000 cycles with an average CE of 91.6%, much superior to the conventional Zn–Cl2 battery with an average CE of only 66.8%. The regulation strategy to the Cl2 cathode provides opportunities for the future development of aqueous Zn‐Cl2 batteries. [ABSTRACT FROM AUTHOR]

Mg batteries utilizing divalent Mg2+ as charge carriers have been attracting significant attention for energy storage owing to their uniqueness in terms of low cost, high safety, and high energy density. However, the short cycling life arising from the accumulation of a passivation layer on the Mg anode prohibits their further development. Here, a new strategy to suppress the accumulation of the passivation layer is presented, thus stabilizing the Mg anode by constructing a robust interfacial layer using organic solvent‐in‐water electrolytes. The organic solvents decompose on the Mg anode to form a MgO, polyether Mg enriched organic‐inorganic hybrid interfacial layer, preventing free water attack to the Mg anode. In addition, the organic solvent forms an H‐bond with H2O to suppress the water activity and therefore protecting the Mg anode. As an illustration to benefits of the solvent‐in‐water electrolytes, a Mg‐MnO2 battery that is coupled by a MnO2 cathode in Mn2+/MnO2 chemistry with the Mg anode is developed. The Mg‐MnO2 battery exhibits a well‐maintained discharge plateau at ≈2.5 V and a discharging capacity of ≈500 mAh g−1 over 1000 cycles. This result highlights the feasibility to stabilize the Mg anode by interface engineering through the solvent‐in‐water electrolyte design. [ABSTRACT FROM AUTHOR]

Aqueous rechargeable hydrogen gas batteries have low cost and high safety, which are expected to be used in large-scale energy storage. Here, we design a novel static vanadium-hydrogen gas (V-H) battery by pairing V3+/VO 2 + liquid redox cathode with the hydrogen gas anode. The two-electron reactions between V3+ and VO 2 + in static hydrogen gas batteries is reported for the first time. The V-H battery has a volumetric capacity of 18.1 Ah/L and an energy efficiency of 61 % at a high current density of 500 mA/cm2. Moreover, it achieves a high capacity retention of 80 % after 900 cycles and an energy density of 22.6 Wh/L at 300 mA/cm2. Finite element simulation proves excellent reversibility of the anode HER/HOR reactions and cathode V3+/VO 2 + redox reactions. This study sheds light on the development of cost-effective, high-energy density, long cycle life, liquid-phase cathode hydrogen batteries for large-scale energy storage applications. [Display omitted] [ABSTRACT FROM AUTHOR]