To sustainably satisfy the growing demand for energy, organic carbonyl compounds (OCCs) are being widely studied as electrode active materials for batteries owing to their high capacity, flexible structure, low cost, environmental friendliness, renewability, and universal applicability. However, their high solubility in electrolytes, limited active sites, and low conductivity are obstacles in increasing their usage. Here, the nucleophilic addition reaction of aromatic carbonyl compounds (ACCs) is first used to explain the electrochemical behavior of carbonyl compounds during charge–discharge, and the relationship of the molecular structure and electrochemical properties of ACCs are discussed. Strategies for molecular structure modifications to improve the performance of ACCs, i.e., the capacity density, cycle life, rate performance, and voltage of the discharge platform, are also elaborated. ACCs, as electrode active materials in aqueous solutions, will become a future research hotspot. ACCs will inevitably become sustainable green materials for batteries with high capacity density and high power density.
In recent years, due to their structural diversity, adjustability, versatility, and excellent electrochemical properties, organic compounds with nitrogen‐containing groups (OCNs) have become some of the most promising organic electrode materials. The nitrogen‐containing groups acting as electrochemical active sites include carbon–nitrogen groups, nitrogen–nitrogen groups, nitrogen–oxygen groups in OCNs, and nitrogen‐containing groups in covalent organic frameworks. The molecular structure regulation of OCNs with nitrogen‐containing groups acting as electrochemical active centers can suppress dissolution in electrolytes, increase electronic conductivity, and improve the kinetics of redox reactions. The kinetics behavior and electrochemical characteristics of OCN electrode materials in alkali metal rechargeable batteries with organic electrolytes are reviewed, and the related relationships between the structure and electrochemical properties of OCNs are the core of this review. Herein, the electrochemical reaction mechanisms and the strategies to improve the electrochemical activity of nitrogen‐containing groups in OCNs are clarified, and the conjugate molecular structure of OCNs is shown to be an important direction for improvement. These results will have implications for research on electrode materials and provide more choices for rechargeable batteries. Moreover, this work will guide the study of more efficient OCNs that can be used as electrode materials.
Aqueous Zn − I batteries hold great potential for high-safety and sustainable energy storage. However, the iodide shuttling effect and the hydrogen evolution reaction that occur in the aqueous electrolyte remain the main obstacles for their further development. Herein, we present the design of a cathode/electrolyte mutualistic aqueous (CEMA) Zn − I battery based on the inherent oxidation ability of trifluoromethanesulfonate ([OTf]−) based aqueous electrolyte towards triiodide species. This results in the formation of iodine sediment particles assembled by fine iodine nanocrystals (approximately 10 nm). An iodine host cathode with high areal iodine loading was realized via a spontaneous absorption process that enriched redox-active iodine and iodide species from aqueous electrolyte onto nanoporous carbon based current collector. By tuning iodide redox process and suppressing competitive hydrogen evolution reaction, the assembled CEMA Zn − I batteries demonstrated a remarkable capacity retention of 76.9% over 1000 cycles, retaining a capacity ranging from 141 to 112 mAh g− 1 at a current density of 0.5 mA cm− 2. Moreover, they exhibited a notable rate capability, with a capacity retention of 74.6% when the current density was increased from 0.5 to 5.0 mA cm− 2, resulting in a capacity retention range of 130 to 97 mAh g− 1. This study demonstrates the feasibility of using the oxidation effect to repel redox-active species from the electrolyte to the cathode, paving a new avenue for high-performance aqueous Zn − I batteries.
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