An Overall Understanding of Sodium Storage Behaviors in Hard Carbons by an "Adsorption-Intercalation/Filling" Hybrid Mechanism

被引：373

作者：

Chen, Xiaoyang ^{[1
]}

Tian, Jiyu ^{[1
]}

Li, Peng ^{[1
]}

Fang, Youlong ^{[1
]}

Fang, Yongjin ^{[1
]}

Liang, Xinmiao ^{[2
]}

Feng, Jiwen ^{[2
]}

Dong, Jiao ^{[3
]}

Ai, Xinping ^{[1
]}

Yang, Hanxi ^{[1
]}

Cao, Yuliang ^{[1
]}

机构：

[1] Wuhan Univ, Engn Res Ctr Organosilicon Cpds & Mat, Minist Educ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China

[2] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Key Lab Magnet Resonance Biol Syst,Innovat Acad P, Wuhan 430071, Peoples R China

[3] Contemporary Amperex Technol Co Ltd, Ningde 352100, Peoples R China

来源：

ADVANCED ENERGY MATERIALS | 2022年 / 12卷 / 24期

关键词：

anode; hard carbon; interlayer intercalation; pore filling; sodium-ion batteries; sodium storage mechanism; MAGNETIC-RESONANCE OBSERVATION; LITHIUM-ION BATTERIES; ELECTROCHEMICAL INTERCALATION; INTERMITTENT TITRATION; RAMAN-SPECTROSCOPY; INSERTION; ELECTRODES; GRAPHITE; INSIGHTS; SUPERCAPACITORS;

D O I：

10.1002/aenm.202200886

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Hard carbon has the potential to serve as a high-capacity anode material for sodium-ion batteries (SIBs), however, its Na+ storage mechanism, particularly on the low potential plateau, remains controversial. To overcome this issue, two types of hard carbons with different microstructures are employed and the relationship between the microstructures and Na+ storage behaviors is evaluated. By the combination of operando X-ray diffraction, ex situ Raman spectroscopy, NMR, and theoretical calculation, it is found that the sodium storage capacities of the hard carbons in the low potential plateau region contain the concurrent contributions from both interlayer intercalation and micropores filling, and the ratio of the two contributors greatly depends on the microstructure of hard carbon materials. Moreover, an electrochemical pointer (potential inflection point at the end of the discharge curve) is found to distinguish the dominance of interlayer intercalation and the micropores filling processes of sodium ions in the low potential plateau region. Based on this new finding, a microstructure-dependent mechanism ("adsorption-intercalation/filling" hybrid mechanism) is proposed to achieve an overall understanding of the sodium storage behaviors in different hard carbon materials, which may provide deep insight into the rational design of hard carbon structures as high-performance anode materials for advanced SIBs.

引用

页数：13