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Creators/Authors contains: "Ji, Xiulei"

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  1. There is a growing interest in anionic redox chemistry to improve the energy densities of rechargeable batteries, and the reversible chlorine/chloride reactions are a promising option for low-temperature applications. As such, understanding Cl adsorption on the cathode surfaces is important in revealing the intimate connection between catalysis and charge storage via the reversible surface Cl2/Cl− redox chemistry. In this work, we investigate the adsorption of Cl on various SrBO3 perovskites, with B being 3d transition metals, by using density functional theory calculations and interpretable machine learning. We identify the electronic structure descriptors crucial for Cl adsorption. Our findings reveal that SrCoO3 exhibits optimal Cl adsorption at the top of the volcano curve for Cl2 evolution, suggesting its potential as a catalyst to enable a low-temperature, liquid Cl2 electrode. 
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  2. The PEG addition into aqueous electrolytes has an opposite effect on an Fe metal anode compared to a Zn metal anode. 
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  3. While NH4+ions dominate bulk insertion within the electrode lattice, interfacial proton-coupled electron transfer takes place at the beginning and end of charge and discharge processes. 
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  4. Abstract The narrow electrochemical stability window of water poses a challenge to the development of aqueous electrolytes. In contrast to non‐aqueous electrolytes, the products of water electrolysis do not contribute to the formation of a passivation layer on electrodes. As a result, aqueous electrolytes require the reactions of additional components, such as additives and co‐solvents, to facilitate the formation of the desired solid electrolyte interphase (SEI) on the anode and cathode electrolyte interphase (CEI) on the cathode. This review highlights the fundamental principles and recent advancements in generating electrolyte interphases in aqueous batteries. 
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  5. Abstract Iron is a promising candidate for a cost‐effective anode for large‐scale energy storage systems due to its natural abundance and well‐established mass production. Recently, Fe‐ion batteries (FeIBs) that use ferrous ions as the charge carrier have emerged as a potential storage solution. The electrolytes in FeIBs are necessarily acidic to render the ferrous ions more anodically stable, allowing a wide operation voltage window. However, the iron anode suffers severe hydrogen evolution reaction with a low Coulombic efficiency (CE) in an acidic environment, shortening the battery cycle life. Herein, a hybrid aqueous electrolyte that forms a solid‐electrolyte interphase (SEI) layer on the Fe anode surface is introduced. The electrolyte mainly comprises FeCl2and ZnCl2as cosalts, where the Zn‐Cl anionic complex species of the concentrated ZnCl2allows dimethyl carbonate (DMC) to be miscible with the aqueous ferrous electrolyte. SEI derived from DMC's decomposition passivates the iron surface, which leads to an average CE of 98.3% and much‐improved cycling stability. This advancement shows the promise of efficient and durable FeIBs. 
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  6. Abstract The electrochemical stability window of water is known to vary with the type and concentration of dissolved salts. However, the underlying influence of ions on the thermodynamic stability of aqueous solutions has not been fully understood. Here, we investigated the electrolytic behaviors of aqueous electrolytes as a function of different ions. Our findings indicate that ions with high ionic potentials, i.e., charge density, promote the formation of their respective hydration structures, enhancing electrolytic reactions via an inductive effect, particularly for small cations. Conversely, ions with lower ionic potentials increase the proportion of free water molecules—those not engaged in hydration shells or hydrogen‐bonding networks—leading to greater electrolytic stability. Furthermore, we observe that the chemical environment created by bulky ions with lower ionic potentials impedes electrolytic reactions by frustrating the solvation of protons and hydroxide ions, the products of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively. We found that the solvation of protons plays a more substantial role than that of hydroxide, which explains a greater shift for OER than for HER, a puzzle that cannot be rationalized by the notion of varying O−H bond strengths of water. These insights will help the design of aqueous systems. 
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  7. Abstract Li2MnO3has been contemplated as a high‐capacity cathode candidate for Li‐ion batteries; however, it evolves oxygen during battery charging under ambient conditions, which hinders a reversible reaction. However, it is unclear if this irreversible process still holds under subambient conditions. Here, the low‐temperature electrochemical properties of Li2MnO3in an aqueous LiCl electrolyte are evaluated and a reversible discharge capacity of 302 mAh g−1at a potential of 1.0 V versus Ag/AgCl at −78 °C with good rate capability and stable cycling performance, in sharp contrast to the findings in a typical Li2MnO3cell cycled at room temperature, is observed. However, the results reveal that the capacity does not originate from the reversible oxygen oxidation in Li2MnO3but the reversible Cl2(l)/Cl(aq.) redox from the electrolyte. The results demonstrate the good catalytic properties of Li2MnO3to promote the Cl2/Clredox at low temperatures. 
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