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    28 November 2022, Volume 28 Issue 11
    Special Issue:In Honor of Professor Yu-Sheng Yang on the Occasion of His 90th Birthday
    Table of Contents
    2022, 28(11):  0-0. 
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    Insight into the Effects of Cation Disorder and Surface Chemical Residues on the Initial Coulombic Efficiency of Layered Oxide Cathode
    Jin-Li Liu, Han-Feng Wu, Zhi-Bei Liu, Ying-Qiang Wu, Li Wang, Feng-Li Bei, Xiang-Ming He
    2022, 28(11):  2219001.  doi:10.13208/j.electrochem.2219001
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    Lithium layered oxide LiNi0.6Co0.2Mn0.2O2 (NCM622) is one of the most promising cathode materials in high-energy lithium-ion batteries for electric vehicles. However, one drawback for NCM622 is that its initial coulombic efficiency (ICE) is only about 87%, which is at least 6% lower than that of LiCoO2 or LiFePO4. In this work, we investigated the effects of surface chemical residues (e.g., LiOH and Li2CO3) and Li/Ni cation disorder resulted during the sintering on the ICE. We found that the ICE of the as-prepared samples could be boosted from 80.80% to 86.68% as the sintering temperatures were increased from 825 to 900 oC. The corresponding Li/Ni cation disorder and surface chemical residues were also reduced with the increasing sintering temperatures. Furthermore, the ICE of the sample sintered at 825 oC could be enhanced by 3.57% after washing with HNO3 solution to remove the surface residues despite the Li/Ni cation disorder being increased. These results demonstrate that minimizing the amount of surface residuals and the degree of Li/Ni cation disorder through an appropriate sintering process and post-treatment technology is critical to achieve a high ICE and improve the electrochemical performances of NCM622.

    Oligomeric Ionic Liquids: Bulk, Interface and Electrochemical Application in Energy Storage
    Dan-Dan Li, Xiang-Yu Ji, Ming Chen, Yan-Ru Yang, Xiao-Dong Wang, Guang Feng
    2022, 28(11):  2219002.  doi:10.13208/j.electrochem.2219002
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    Over recent years, oligomer ionic liquids (OILs), a novel class of ionic liquids, are becoming preferential electrolytes for high-performance energy-storage devices, such as supercapacitors with enhanced energy density and non-flammable lithium-ion batteries (LIBs). Herein, structures, properties, and their associations of the up-to-the-minute formulated OILs are systematically summarized and elaborately interpreted, especially for dicationic ionic liquids and tricationic ionic liquids. The physicochemical and electrochemical properties of OIL-based electrolytes are presented and analyzed, which are vitally important for supercapacitors and LIBs. Subsequently, the applications of OILs as electrolytes for supercapacitors and LIBs are summarized, with the comparisons of the energy-storage mechanisms and performance between OILs and MILs electrolytes in supercapacitors. Meanwhile, the optimization of the dynamic performance of OILs electrolytes is provided. Finally, the main difficulties and probable perspectives of OIL-based electrolytes are presented for future work. This review would contribute to a deep understanding of OILs and design optimized OIL-based electrolytes for energy storage systems.

    Review on Oxygen-Free Vanadium-Based Cathodes for Aqueous Zinc-Ion Batteries
    Xiao-Ru Yun, Yu-Fang Chen, Pei-Tao Xiao, Chun-Man Zheng
    2022, 28(11):  2219004.  doi:10.13208/j.electrochem.2219004
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    Aqueous zinc-ion batteries (AZIBs) are considered as one of the most promising next-generation electrochemical energy storage systems owing to their high-power density, environmental benign, intrinsic safety, and the low cost of the abundant zinc resources. However, their further development is still plagued by the inferior electrochemical performance of cathode materials. Though extensive research has been conducted to investigate various cathode materials (including manganese oxides, vanadium oxides, Prussian blues analogy, and organic materials), design of high-performance cathodes with satisfying capacity and long-term cycling stability still faces great challenges. Oxygen-free vanadium-based compounds, owing to their better conductivity, larger interlayer spacing, lower ion diffusion barrier and higher theoretical specific capacity than those of vanadium oxides, have gained increasing attention recently. In this review, we summarize the recent development about the emerging oxygen-free vanadium-based compounds in AZIBs, emphasizing the methods to design electrode materials with desired structures, effective strategies to improve their electrochemical performance, and the fundamental electrochemical mechanisms. Finally, the current challenges and outlooks of oxygen-free vanadium-based compounds are proposed, providing a novel perspective and useful guidance for the design of high-performance vanadium-based cathode materials for AZIBs.

    Advances and Atomistic Insights of Electrolytes for Lithium-Ion Batteries and Beyond
    Tingzheng Hou, Xiang Chen, Lu Jiang, Cheng Tang
    2022, 28(11):  2219007.  doi:10.13208/j.electrochem.2219007
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    Electrolytes and the associated electrode-electrolyte interfaces are crucial for the development and application of high-capacity energy storage systems. Specifically, a variety of electrolyte properties, ranging from mechanical (compressibility, viscosity), thermal (heat conductivity and capacity), to chemical (solubility, activity, reactivity), transport, and electrochemical (interfacial and interphasial), are correlated to the performance of the resultant full energy storage device. In order to facilitate the operation of novel electrode materials, extensive experimental efforts have been devoted to improving these electrolyte properties by tuning the physical design and/or chemical composition. Meanwhile, the recent development of theoretical modeling methods is providing atomistic understandings of the electrolyte’s role in regulating the ion transport and enabling a functional interface. In this regard, we stand at a new frontier to take advantage of the revealed mechanistic insights into rationally design novel electrolyte systems. In this review, we first summarize the composition, solvation structure, and transport properties of conventional electrolytes as well as the formation mechanism of the electrode-electrolyte interphase. Moreover, some of the promising energy storage systems are briefly introduced. Further, approaches to stabilize the electrode-electrolyte interphase using novel electrolyte design, including electrolyte additives, high-concentration electrolytes, and solid-state electrolytes, are discussed. Some recent advances in the atomistic modeling of these aspects are particularly focused to provide a fundamental understanding of electrolytes and a comprehensive guide for future electrolyte design. Finally, we highlight the prospects of theoretical screening of novel electrolytes.

    Efficient Interface Enabled by Nano-Hydroxyapatite@Porous Carbon for Lithium-Sulfur Batteries
    Jia-Yu Wang, Xue-Feng Tong, Qi-Fan Peng, Yue-Peng Guan, Wei-Kun Wang, An-Bang Wang, Nai-Qiang Liu, Ya-Qin Huang
    2022, 28(11):  2219008.  doi:10.13208/j.electrochem.2219008
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    The dissolution and “shuttle effect” of lithium polysulfides (LiPSs) hinder the application of lithium-sulfur (Li-S) batteries. To solve those problems, inspired by natural materials, a nano-hydroxyapatite@porous carbon derived from chicken cartilage (nano-HA@CCPC) was fabricated by employing a simple pre-carbonization and carbonization method, and applied in Li-S batteries. The nano-HA@CCPC would provide a reactive interface that allows efficient LiPSs reduction. With a strong affinity for LiPSs and an excellent electronic conductive path for converting LiPSs, the shuttle effect of LiPSs was confined and the redox kinetics of LiPSs was substantially enhanced. Li-S batteries employing nano-HA@CCPC-modified separators exhibited long cycle life and improved rate capability. At 0.5 C after 325 cycles, a specific capacity of 815 mAh·g-1 and a low capacity fading rate of 0.051% were obtained. The superior properties, sustainable raw materials, and facile preparation process make nano-HA@CCPC a promising additive material for practical Li-S batteries.

    Which Factor Dominates Battery Performance: Metal Ion Solvation Structure-Derived Interfacial Behavior or Solid Electrolyte Interphase Layer?
    Hao-Ran Cheng, Zheng Ma, Ying-Jun Guo, Chun-Sheng Sun, Qian Li, Jun Ming
    2022, 28(11):  2219012.  doi:10.13208/j.electrochem.2219012
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    Solid-electrolyte interphase (SEI) layer formed on the electrode by electrolyte decomposition has been considered to be one of the most important factors affecting the battery performance. We discover that the metal ion solvation structure can also influence the performance, particularly, it can elucidate many phenomena that the SEI cannot. In this review, we summarize the importance of the metal ion solvation structure and the derived metal ion de-solvation behaviors, by which we can build an interfacial model to show the relationship between the interfacial behavior and electrode performance, and then apply to different electrode and battery systems. We emphasize the influences of ionic and molecular interactions on electrode surface that differ from previous SEI-based interpretations. This review provides a new view angle to understand the battery performance and guide the electrolyte design.