Structure-Performance relationship guided design and strategic synthesis of lithiated oxa-graphene for high lithium storage

Zhaoxin Li; Naxing Liu; Jian Wang; Yongqi Xu; Li Bai; Long Jiang; Liang Cui; Chengshuo Shen; Xunshan Liu; Fu-Gang Zhao

doi:10.1016/j.jcis.2022.12.140

Structure-Performance relationship guided design and strategic synthesis of lithiated oxa-graphene for high lithium storage

J Colloid Interface Sci. 2023 Apr:635:543-551. doi: 10.1016/j.jcis.2022.12.140. Epub 2022 Dec 30.

Authors

Zhaoxin Li¹, Naxing Liu¹, Jian Wang¹, Yongqi Xu¹, Li Bai¹, Long Jiang¹, Liang Cui², Chengshuo Shen³, Xunshan Liu⁴, Fu-Gang Zhao⁵

Affiliations

¹ Department of Chemistry, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China.
² Department of Chemistry, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: cuiliang@hnu.edu.cn.
³ Department of Chemistry, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: shenchengshuo@zstu.edu.cn.
⁴ Department of Chemistry, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: xliu350@zstu.edu.cn.
⁵ Department of Chemistry, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: fgzhao@zstu.edu.cn.

PMID: 36603537
DOI: 10.1016/j.jcis.2022.12.140

Abstract

Graphene derivative materials are widely used as anode component in lithium-ion batteries. However, there is still a lack of reliable and foresighted guides helpful for designing high-performance graphene-based electrode materials. To this end, we strategically chose challenging graphite fluoride as starting material for the derivatization of graphene in order to exclude interference factors. As a result, graphene framework was functionalized with oxygen-containing carboxylate and sulfonate groups and oxygen-free aniline units at a similar functionalization degree. Due to the strong effect of lithiation, out-of-plane p-aminobenzoic acid blocks boosted the lithium-storage capacity of graphene matrix to 636 mAh g^-1 at 0.1 A/g, and sulfanilic acid blocks maximized this value to 873 mAh g^-1. Sadly, oxygen-free aniline functionalized graphene material only delivered a specific capacity of 88 mAh g^-1. Meanwhile, spatial lithiated carboxylate and sulfonate units endowed graphene framework with better rate capability and cycling stability. Such a structure-performance relationship established herein was beneficial for the design and preparation of high-performance graphene derivative electrode materials.

Keywords: Graphene carboxylation; Graphene functionalization; Graphene lithium storage; Graphene structure-performance relationship; Graphene sulfonation.