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Silicon-based material is one of the most promising substitutes for commercial graphite anodes for the next generation lithium-ion batteries due to its extremely high theoretical capacity. However, the huge volume changes during the charging and discharging processes will cause rapid capacity decay and a short cycle life. Developing novel silicon-based materials requires a fundamental understanding of their properties. However, in many cases, the present experiments are incapable of completely mimicking real battery-operation conditions, and detailed information about the electrochemical mechanisms and ion and electron kinetic transport at the electrode/electrolyte interface is still ambiguous due to their complexity. First-principles calculations have become an effective method for predicting and interpreting the characteristics of electrode materials, understanding the electrochemical mechanisms at the atomic scale and delivering rational design strategies for electrode materials. In this review, the first-principles calculations of silicon-based anode materials in recent years, based on different modification strategies, are summarized. First, we introduce the diffusion kinetics of lithium ions in silicon and the mechanism of structure changes during the lithiation process. Then, typical examples of novel Si-based anodes, including 2D nanomaterials, silicide materials and coating materials based on theoretical predictions, are presented. Finally, we provide perspectives and future directions of first-principles calculations on Si-based anodes. [ABSTRACT FROM AUTHOR]

Zinc ion batteries (ZIBs) exhibit significant promise in the next generation of grid‐scale energy storage systems owing to their safety, relatively high volumetric energy density, and low production cost. Despite substantial advancements in ZIBs, a comprehensive evaluation of critical parameters impacting their practical energy density (Epractical) and calendar life is lacking. Hence, we suggest using formulation‐based study as a scientific tool to accurately calculate the cell‐level energy density and predict the cycling life of ZIBs. By combining all key battery parameters, such as the capacity ratio of negative to positive electrode (N/P), into one formula, we assess their impact on Epractical. When all parameters are optimized, we urge to achieve the theoretical capacity for a high Epractical. Furthermore, we propose a formulation that correlates the N/P and Coulombic efficiency of ZIBs for predicting their calendar life. Finally, we offer a comprehensive overview of current advancements in ZIBs, covering cathode and anode, along with practical evaluations. This Minireview outlines specific goals, suggests future research directions, and sketches prospects for designing efficient and high‐performing ZIBs. It aims at bridging the gap from academia to industry for grid‐scale energy storage. [ABSTRACT FROM AUTHOR]

Growth in intermittent renewable sources including solar and wind has sparked increasing interest in electrical energy storage. Grid‐scale energy storage integrated with renewable sources has significant advantages in energy regulation and grid security. Aqueous zinc‐ion batteries (AZIBs) have emerged as a practically attractive option for electrical storage because of environmentally benign aqueous‐based electrolytes, high theoretical capacity of Zn anode, and significant global reserves of Zn. However, application of AZIBs at the grid‐scale is restricted by drawbacks in cathode material(s). Herein, a comprehensive summary of the features and storage mechanisms of the latest cathode materials is provided. The fundamental problems and corresponding in‐depth causes for cathode materials is critically reviewed. It is also assess practical challenges, appraise their translation to commerce and industry, and systematically summarize and discuss the potential solutions reported in recent works. It is established necessary design strategies for Zn anodes and electrolytes that are matched with cathode materials for commercializing AZIBs. Finally, it is concluded with a perspective on the practical prospects for advancing the development of future AZIBs. Findings will be of interest and benefit to a range of researchers and manufacturers in the design and application of AZIBs for grid‐scale energy storage. [ABSTRACT FROM AUTHOR]

Aqueous Zn‐Iodine (I2) batteries are attractive for large‐scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode "shuttle" of polyiodines. Here we report a class of N‐containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition of pyridine /imidazole regulates electrolyte pH, and inhibits HER and anode corrosion. In addition, pyridine and imidazole preferentially absorb on Zn metal, regulating non‐dendritic Zn plating /stripping, and achieving a high Coulombic efficiency of 99.6 % and long‐term cycling stability of 3200 h at 2 mA cm−2, 2 mAh cm−2. It is also confirmed that pyridine inhibits polyiodines shuttling and boosts conversion kinetics for I−/I2. As a result, the Zn‐I2 full battery exhibits long cycle stability of >25 000 cycles and high specific capacity of 105.5 mAh g−1 at 10 A g−1. We conclude organic pH buffer engineering is practical for dendrite‐free and shuttle‐free Zn‐I2 batteries. [ABSTRACT FROM AUTHOR]

Zinc metal battery (ZMB) is promising as the next generation of energy storage system, but challenges relating to dendrites and corrosion of the zinc anode are restricting its practical application. Here, to stabilize Zn anode, we report a controlled electrolytic method for a monolithic solid‐electrolyte interphase (SEI) via a high dipole moment solvent dimethyl methylphosphonate (DMMP). The DMMP‐based electrolytes can generate a homogeneous and robust phosphate SEI (Zn3(PO4)2 and ZnP2O6). Benefiting from the protecting impact of this in situ monolithic SEI, the zinc electrode exhibits long‐term cycling of 4700 h and a high Coulombic efficiency 99.89 % in Zn|Zn and Zn|Cu cell, respectively. The full V2O5|Zn battery with DMMP‐H2O hybrid electrolyte exhibits a high capacity retention of 82.2 % following 4000 cycles under 5 A g−1. The first success in constructing the monolithic phosphate SEI will open a new avenue in electrolyte design for highly reversible and stable Zn metal anodes. [ABSTRACT FROM AUTHOR]

Highlights: First report of a lithium-ion battery cathode as a deionization electrode for desalination. A novel approach to suppress manganese dissolution by exposing the (111) facet is proposed. Excellent desalination performance by the LiMn2O4/C cathode. The material achieves an ultrahigh desalination capacity of 117.3 mg g−1 at 1.0 V and a longer cycle life (200 cycles without capacity decay) with minor manganese dissolution during the cycling test in 10 mM aqueous LiCl solution. Battery materials as emerging capacitive deionization electrodes for desalination have better salt removal capacities than traditional carbon-based materials. LiMn2O4, a widely used cathode material, is difficult to utilize as a deionization electrode due to its structural instability upon cycling and Mn dissolution in aqueous-based electrolytes. Herein, a facile and low-cost ball-milling routine was proposed to prepare a LiMn2O4 material with highly exposed (111) facets. The prepared electrode exhibited relatively low dissolution of Mn during cycling, which shows its long cycle stability. In the hybrid capacitive deionization system, the LiMn2O4/C electrode delivered a high desalination capacity of 117.3 mg g−1 without obvious capacity decay at a voltage of 1.0 V with a 20 mM initial salt concentration. In addition, the exposed (111) facets significantly alleviated Mn ion dissolution, which also enhanced the structural steadiness. [ABSTRACT FROM AUTHOR]

Metal phosphides are regarded as promising anode candidates for high‐energy‐density potassium‐ion batteries (PIBs) due to their high theoretical capacity and relatively low operation voltage. The failure mechanism of the metal phosphides originates from the large volume variation during cycling, which leads to fast capacity degradation. Herein, concentrated electrolyte is used to achieve impressive cycling stability for K‐metal and K‐ion batteries over their more dilute counterparts, mainly benefiting from the anion‐derived robust and uniform solid–electrolyte interphase layer, which is helpful in maintaining the electrode integrity, avoiding excessive side reactions, and suppressing electrolyte decomposition. Further investigations also reveal the synergistic advantages of the superior chemical compatibility of concentrated electrolyte to potassium metal, as well as its remarkable electrochemical stability and enhanced safety compared to conventional dilute electrolytes. This work provides a feasible strategy to mitigate the degradation of metal phosphides to build high‐energy‐density PIBs. [ABSTRACT FROM AUTHOR]