Carboxyl‐Dominant Oxygen Rich Carbon for Improved Sodium Ion Storage: Synergistic Enhancement of Adsorption and Intercalation Mechanisms,Advanced Energy Materials

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Carboxyl‐Dominant Oxygen Rich Carbon for Improved Sodium Ion Storage: Synergistic Enhancement of Adsorption and Intercalation Mechanisms
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-11-20 , DOI: 10.1002/aenm.202002981
Fei Sun _{1,

2} , Hua Wang ₁ , Zhibin Qu ₁ , Kunfang Wang ₁ , Lijie Wang ₁ , Jihui Gao ₁ , Jianmin Gao ₁ , Shaoqin Liu ₂ , Yunfeng Lu ₃

Affiliation

Oxygen‐containing groups in carbon materials have been shown to affect the carbon anode performance of sodium ion batteries; however, precise identification of the correlation between specific oxygen specie and Na⁺ storage behavior still remains challenging as various oxygen groups coexist in the carbon framework. Herein, a postengineering method via a mechanochemistry process is developed to achieve accurate doping of (20.12 at%) carboxyl groups in a carbon framework. The constructed carbon anode delivers all‐round improvements in Na⁺ storage properties in terms of a large reversible capacity (382 mAg⁻¹ at 30 mA g⁻¹), an excellent rate capability (153 mAg⁻¹ at 2 A g⁻¹) as well as good cycling stability (141 mAg⁻¹ after 2000 cycles at 1.5 A g⁻¹). Control experiments, kinetic analysis, density functional theory calculations, and operando measurements collectively demonstrate that carboxyl groups not only act as active sites for Na⁺ capacitive adsorption through suitable electrostatic interactions, but also gradually expand d‐spacing by inducing a repulsive force between carbon layers with Na⁺ preadsorbed, and hence facilitate diffusion‐controlled Na⁺ insertion process. This work provides a new insight in the rational tunning of oxygen‐containing groups in carbon for boosting reversible Na⁺ storage through a synergy of adsorption and intercalation processes.

中文翻译：

羧基占主导地位的富氧碳，用于改善钠离子存储：吸附和嵌入机制的协同增强

研究表明，碳材料中的含氧基团会影响钠离子电池的碳阳极性能。然而，由于碳框架中同时存在各种氧基团，因此精确鉴定特定氧种类与Na ⁺储存行为之间的相关性仍然具有挑战性。本文中，开发了一种通过机械化学过程的后工程方法，以实现碳骨架中（20.12 at％）羧基的准确掺杂。所构造的碳阳极提供以Na全方位改进⁺储存性质在一个较大的可逆容量（382 MAG方面^-1在30mA克^-1），优异的倍率性能（153 MAG ^-1以2A克^-1），以及良好的循环稳定性（141 MAG ^-1在1.5 A克2000次循环之后^-1）。控制实验，动力学分析，密度泛函理论计算和操作测量共同表明，羧基不仅通过适当的静电相互作用充当Na ⁺电容吸附的活性位，而且通过诱导碳层之间的排斥力逐渐扩大d间距预先吸附了Na ⁺，因此有助于扩散控制的Na ⁺插入过程。这项工作为合理修饰碳中的含氧基团以增加可逆的Na ⁺提供了新的见解。通过吸附和嵌入过程的协同作用进行存储。

更新日期：2021-01-07

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