The goal of limiting global warming to 1.5 °C requires a drastic reduction in CO2 emissions across many sectors of the world economy. Batteries are vital to this endeavor, whether used in electric vehicles, to store renewable electricity, or in aviation. Present lithium-ion technologies are preparing the public for this inevitable change, but their maximum theoretical specific capacity presents a limitation. Their high cost is another concern for commercial viability. Metal-air batteries have the highest theoretical energy density of all possible secondary battery technologies and could yield step changes in energy storage, if their practical difficulties could be overcome. The scope of this review is to provide an objective, comprehensive, and authoritative assessment of the intensive work invested in nonaqueous rechargeable metal-air batteries over the past few years, which identified the key problems and guides directions to solve them. We focus primarily on the challenges and outlook for Li-O2 cells but include Na-O2, K-O2, and Mg-O2 cells for comparison. Our review highlights the interdisciplinary nature of this field that involves a combination of materials chemistry, electrochemistry, computation, microscopy, spectroscopy, and surface science. The mechanisms of O2 reduction and evolution are considered in the light of recent findings, along with developments in positive and negative electrodes, electrolytes, electrocatalysis on surfaces and in solution, and the degradative effect of singlet oxygen, which is typically formed in Li-O2 cells.

/pdf/lithium-oxygen-batteries-and-related-systems-potential-1kvfepaqwx.pdf

Lithium-Oxygen Batteries and Related Systems: Potential, Status, and Future

The development of low-cost and high-safety zinc-ion batteries (ZIBs) has been extensively discussed and reviewed in recent years, but the work on the comprehensive discussion and perspectives in developing zinc-ion electrolytes is still relatively lacking. Faced with critical challenges and bottlenecks practically, the viability of ZIBs critically depends on the development of suitable electrolytes and their practical considerations. In this review, a systematic summary with regard to the basic characteristics of zinc-ion electrolytes facing different issues from optimization strategies to the fundamental science of electrolyte/electrode interfaces (EEIs), particularly in the feasible modifications and advanced characterizations of EEIs, has been put forward. Due to the lack of consideration of the practical issues in major academic studies, we have particularly highlighted aspects that mainly focus on the choice of the electrolyte system, dosage of liquid and fluid electrolytes, status of gel and all-solid electrolytes, together with other concerns related to the electrolytes. The final section proposes significant perspectives to guide and promote the development of zinc-ion electrolytes.

Fundamentals and perspectives in developing zinc-ion battery electrolytes: a comprehensive review

Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector. Four types of ion-conducting, inorganic solid electrolytes are tested: Amorphous 70/30 mol% Li2S-P2S5, polycrystalline β-Li3PS4, and polycrystalline and single-crystalline Li6La3ZrTaO12 garnet. The nature of lithium plating depends on the proximity of the current collector to defects such as surface cracks and on the current density. Lithium plating penetrates/infiltrates at defects, but only above a critical current density. Eventually, infiltration results in a short circuit between the current collector and the Li-source (anode). These results do not depend on the electrolytes shear modulus and are thus not consistent with the Monroe–Newman model for “dendrites.” The observations suggest that Li-plating in pre-existing flaws produces crack-tip stresses which drive crack propagation, and an electrochemomechanical model of plating-induced Li infiltration is proposed. Lithium short-circuits through solid electrolytes occurs through a fundamentally different process than through liquid electrolytes. The onset of Li infiltration depends on solid-state electrolyte surface morphology, in particular the defect size and density.

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Nonaqueous lithium–air batteries have garnered considerable research interest over the past decade due to their extremely high theoretical energy densities and potentially low cost. Significant adv...

Current challenges and routes forward for nonaqueous lithium–air batteries

Prussian blue analogues (PBAs) have attracted wide attention for their application in the energy storage and conversion field due to their low cost, facile synthesis, and appreciable electrochemical performance. At the present stage, most research on PBAs is focused on their material-level optimization, whereas their properties in practical battery systems are seldom considered. This review aims to first provide an overview of the history and parameters of PBA materials and analyze the fundamental principles toward rational design of PBAs, and then evaluate the prospects and challenges for PBAs for practical sodium-ion batteries, hoping to bridge the gap between laboratory research and commercial reality. 

Prussian Blue Analogues for Sodium‐Ion Batteries: Past, Present, and Future

Recent Progress on Advanced Imaging Techniques for Lithium-Ion Batteries

A Li–Al–O Solid-State Electrolyte with High Ionic Conductivity and Good Capability to Protect Li Anode

Ether-based electrolytes are commonly used in Li-O2 batteries (LOBs) because of their relatively high stability. But they are still prone to be attacked by superoxides or singlet oxygen via hydrogen abstract reactions, which leads to performance decaying during long-term operation. Herein we propose a methylated cyclic ether, 2,2,4,4,5,5-hexamethyl-1,3-dioxolane (HMD), as a stable electrolyte solvent for LOBs. Such a compound does not contain any hydrogen atoms on the alpha-carbon of the ether, and thus avoids hydrogen abstraction reactions. As the result, this solvent exhibits excellent stability with the presence of superoxide or singlet oxygen. In addition the CO2 evolution during charge process is prohibited. The LOB with HMD-based electrolyte was able to run up to 157 cycles, 4 times more than with 1,3-dioxolane (DOL) or 1,2-dimethoxyethane (DME) based electrolytes.

A Stable Lithium-Oxygen Battery Electrolyte Based on Fully Methylated Cyclic Ether.

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Boosting the cyclability of tetracyanoquinodimethane (TCNQ) as cathode material in aqueous battery with high valent cation

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