Multi-Electron Reactions Enabled by Anion-Based Redox Chemistry for High-Energy Multivalent Rechargeable Batteries.,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Multi-Electron Reactions Enabled by Anion-Based Redox Chemistry for High-Energy Multivalent Rechargeable Batteries.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-03-27 , DOI: 10.1002/anie.202002560
Zhenyou Li ₁ , Bhaghavathi P Vinayan ₁ , Piotr Jankowski ₂ , Christian Njel ₃ , Ananyo Roy ₁ , Tejs Vegge ₂ , Julia Maibach ₃ , Juan Maria García Lastra ₂ , Maximilian Fichtner _{1,

4} , Zhirong Zhao-Karger ₁

Affiliation

The development of multivalent metal (such as Mg and Ca) based battery systems is hindered by lack of suitable cathode chemistry that shows reversible multi‐electron redox reactions. Cationic redox centres in the classical cathodes can only afford stepwise single‐electron transfer, which are not ideal for multivalent‐ion storage. The charge imbalance during multivalent ion insertion might lead to an additional kinetic barrier for ion mobility. Therefore, multivalent battery cathodes only exhibit slope‐like voltage profiles with insertion/extraction redox of less than one electron. Taking VS₄ as a model material, reversible two‐electron redox with cationic–anionic contributions is verified in both rechargeable Mg batteries (RMBs) and rechargeable Ca batteries (RCBs). The corresponding cells exhibit high capacities of >300 mAh g⁻¹ at a current density of 100 mA g⁻¹ in both RMBs and RCBs, resulting in a high energy density of >300 Wh kg⁻¹ for RMBs and >500 Wh kg⁻¹ for RCBs. Mechanistic studies reveal a unique redox activity mainly at anionic sulfides moieties and fast Mg²⁺ ion diffusion kinetics enabled by the soft structure and flexible electron configuration of VS₄.

中文翻译：

基于阴离子的氧化还原化学实现的多电子反应，用于高能多价可充电电池。

基于多价金属（如Mg和Ca）的电池系统的发展因缺乏合适的阴极化学物质而受到阻碍，该化学物质显示出可逆的多电子氧化还原反应。经典阴极中的阳离子氧化还原中心只能提供逐步的单电子转移，这对于多价离子存储而言并不理想。多价离子插入过程中的电荷不平衡可能会导致离子迁移的其他动力学障碍。因此，多价电池阴极仅表现出类似斜坡的电压分布，其插入/提取氧化还原少于一个电子。以VS ₄作为模型材料，可充电的Mg电池（RMB）和可充电的Ca电池（RCB）均已验证了具有阳离子-阴离子作用的可逆双电子氧化还原。相应的细胞表现出> 300毫安克高容量^-1在100mA g的电流密度^-1在两个人民币和RCBS，导致>为300Wh公斤的高能量密度^-1为红巴和> 500瓦时公斤^- RCB为¹。机理研究表明，VS ₄具有柔软的结构和灵活的电子构型，主要在阴离子硫化物部分具有独特的氧化还原活性，并具有快速的Mg ²⁺离子扩散动力学。

更新日期：2020-03-27

点击分享查看原文

点击收藏

公开下载

阅读更多本刊最新论文本刊介绍/投稿指南11