With the low redox potential of -3.04 V (vs SHE) and ultrahigh theoretical capacity of 3862 mAh g-1 , lithium metal has been considered as promising anode material. However, lithium metal battery has ever suffered a trough in the past few decades due to its safety issues. Over the years, the limited energy density of the lithium-ion battery cannot meet the growing demands of the advanced energy storage devices. Therefore, lithium metal anodes receive renewed attention, which have the potential to achieve high-energy batteries. In this review, the history of the lithium anode is reviewed first. Then the failure mechanism of the lithium anode is analyzed, including dendrite, dead lithium, corrosion, and volume expansion of the lithium anode. Further, the strategies to alleviate the lithium anode issues in recent years are discussed emphatically. Eventually, remaining challenges of these strategies and possible research directions of lithium-anode modification are presented to inspire innovation of lithium anode.

Confronting the Challenges in Lithium Anodes for Lithium Metal Batteries.

Organic batteries for a greener rechargeable world

Aqueous zinc-ion batteries (ZIBs) are promising for next-generation energy storage. However, the reported electrode materials for ZIBs are facing the shortcomings including low capacity and unsatisfactory cycling stability etc. Herein, hexaazatrinaphthalene-quione (HATNQ) is reported for aqueous ZIBs. The HATNQ electrodes delivered an ultrahigh capacity (482.5 mAh g -1 at 0.2 A g -1 ) and outstanding cyclability of >10000 cycles at 5 A g -1 . The capacity sets new record for organic cathodes in aqueous ZIBs. The high performances are ascribed to the rich C=O and C=N groups that endowed HATNQ with 2D layered supramolecular structure by multiple hydrogen bonds in plane with π-π interactions out of plane, leading to enhanced charge transfer, insolubility, and rapid ion transport for fast-charge and -discharge batteries. Moreover, the 2D supramolecular structure boosted the storage of Zn 2+ /H + , particularly the storage of Zn 2+ , due to the more favorable O···Zn···N coordination in HATNQ.

Two-dimensional Organic Supramolecule via Hydrogen Bonding and π-π Stacking for Ultrahigh Capacity and Long-Life Aqueous Zinc-Organic Batteries.

With the rapid growth in energy consumption, renewable energy is a promising solution. However, renewable energy (e.g., wind, solar, and tidal) is discontinuous and irregular by nature, which poses new challenges to the new generation of large-scale energy storage devices. Rechargeable batteries using aqueous electrolyte and multivalent ion charge are considered more suitable candidates compared to lithium-ion and lead-acid batteries, owing to their low cost, ease of manufacture, good safety, and environmentally benign characteristics. However, some substantial challenges hinder the development of aqueous rechargeable multivalent ion batteries (AMVIBs), including the narrow stable electrochemical window of water (≈1.23 V), sluggish ion diffusion kinetics, and stability issues of electrode materials. To address these challenges, a range of encouraging strategies has been developed in recent years, in the aspects of electrolyte optimization, material structure engineering and theoretical investigations. To inspire new research directions, this review focuses on the latest advances in cathode materials for aqueous batteries based on the multivalent ions (Zn2+, Mg2+, Ca2+, Al3+), their common challenges, and promising strategies for improvement. In addition, further suggestions for development directions and a comparison of the different AMVIBs are covered.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/adfm.202010445

Cathode Design for Aqueous Rechargeable Multivalent Ion Batteries: Challenges and Opportunities

Lithium metal batteries (LMBs) are considered promising candidates for next‐generation battery systems due to their high energy density. However, commercialized carbonate electrolytes cannot be used in LMBs due to their poor compatibility with lithium metal anodes. While increasing cut‐off voltage is an effective way to boost the energy density of LMBs, conventional ethylene carbonate‐based electrolytes undergo a number of side reactions at high voltages. It is therefore critical to upgrade conventional carbonate electrolytes, the performance of which is highly influenced by the solvation structure of lithium ions (Li+). This review provides a comprehensive overview of the strategies to regulate the solvation structure of Li+ in carbonate electrolytes for LMBs by better understanding the science behind the Li+ solvation structure and Li+ behavior. Different strategies are systematically compared to help select better electrolytes for specific applications. The remaining scientific and technical problems are pointed out, and directions for future research on carbonate electrolytes for LMBs are proposed.

A Review on Regulating Li+ Solvation Structures in Carbonate Electrolytes for Lithium Metal Batteries

Due to the low cost and abundance of multivalent metallic resources (Mg/Al/Zn/Ca), multivalent rechargeable batteries (MRBs) are promising alternatives to Li-ion and Pb-acid batteries for grid-scale stationary energy storage applications. However, the high performance of inorganic electrode materials in Li-ion batteries does not extend to MRBs, because the high charge density of multivalent cations dramatically reduces their diffusivity in the crystal lattice of inorganic materials. To achieve high-performance MRBs, organic electrode materials (OEMs) with abundant structural diversity and high structural tunability offer opportunities. This review presents an overview of the state-of-the-art OEMs in MRBs, including non-aqueous rechargeable Mg/Al/Zn and aqueous rechargeable Mg/Al/Zn/Ca batteries. The advantages, challenges, development, mechanism, structure, and performance of OEMs in MRBs are discussed in detail. To provide a comprehensive and thorough understanding of OEMs in MRBs, the correlation between molecular structure and electrochemical behavior is also summarized and discussed. This review offers insights for the rational structure design and performance optimization of advanced OEMs in MRBs.

Recent advances in developing organic electrode materials for multivalent rechargeable batteries

Strategies in Structure and Electrolyte Design for High‐Performance Lithium Metal Batteries

Na-ion batteries (NIBs) are promising alternatives to Li-ion batteries (LIBs) due to the low cost, abundance, and high sustainability of sodium resources. However, the high performance of inorganic electrode materials in LIBs does not extend to NIBs because of the larger ion size of Na+ than Li+ and more complicated electrochemistry. Therefore, it is vital to search for high-performance electrode materials for NIBs. Organic electrode materials (OEMs) with the advantages of high structural tunability and abundant structural diversity show great promise in developing high-performance NIBs. To achieve advanced OEMs for NIBs, a fundamental understanding of the structure–performance correlation is desired for rational structure design and performance optimization. In this review, recent advances in developing OEMs for non-aqueous, aqueous, and all-solid-state NIBs are presented. The challenges, advantages, mechanisms, development, and applications of advanced OEMs in NIBs are also discussed. Perspectives for the innovation of structure design principle and future research direction of OEMs in non-aqueous, aqueous, and all-solid-state NIBs are provided.

/pdf/organic-electrode-materials-for-non-aqueous-aqueous-and-all-1x4y91g3w6.pdf

Organic electrode materials for non-aqueous, aqueous, and all-solid-state Na-ion batteries

A conjugated tetracarboxylate anode for stable and sustainable Na-ion batteries

Redox flow batteries (RFBs) are promising for the large-scale storage of renewable energies. Nonaqueous RFBs can achieve higher voltages and are more suitable for extreme environments than their aqueous counterparts. In this work, the first nonaqueous Mg flow battery with a polymer catholyte is reported, by integrating a Mg foil anode, and a porous membrane, with a polymer solution catholyte. The battery can deliver a voltage of 1.74 V, a capacity of 250 mAh/L, and a cycle life of 50 cycles. This work demonstrates the feasibility of Mg flow batteries and provides a unique direction for flow battery research. 

Nonaqueous Mg Flow Battery with a Polymer Catholyte

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