Engineering electronic structure of graphene to boost Lithium-Storage performances

Yongqi Xu; Yuxiao Chu; Tingting Zhao; Xiao-Rui Liu; Chengshuo Shen; Lei Dong; Liang Cui; Yongmiao Shen; Wei-Shi Li; Fu-Gang Zhao

doi:10.1016/j.jcis.2023.02.124

Engineering electronic structure of graphene to boost Lithium-Storage performances

J Colloid Interface Sci. 2023 Jun 15:640:383-390. doi: 10.1016/j.jcis.2023.02.124. Epub 2023 Feb 27.

Authors

Yongqi Xu¹, Yuxiao Chu¹, Tingting Zhao¹, Xiao-Rui Liu², Chengshuo Shen¹, Lei Dong³, Liang Cui¹, Yongmiao Shen⁴, Wei-Shi Li⁵, Fu-Gang Zhao⁶

Affiliations

¹ Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Department of Chemistry, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China.
² Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Department of Chemistry, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China; Key Laboratory of Excited-State Materials of Zhejiang Province, Zhejiang University, Hangzhou 310027, China.
³ State Key Laboratory of Solidification Processing, Center of Advanced Lubrication and Seal Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an 710072, China.
⁴ Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Department of Chemistry, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: shenym@zstu.edu.cn.
⁵ Key Laboratory of Synthetic and Self-Assembly Chemistry for Functional Molecules, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai 200032, China.
⁶ Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Department of Chemistry, Zhejiang Sci-Tech University, 928 Second Street, Hangzhou 310018, China. Electronic address: zhaofugang85@163.com.

PMID: 36867935
DOI: 10.1016/j.jcis.2023.02.124

Abstract

Organic functionalization of graphene framework was an effective means used to boost the storage performances of lithium, but it lacked a universal strategic guideline for introducing functional groups (electron-withdrawing and electron-donating modules are overall classified). It mainly entailed designing and synthesizing graphene derivatives, in which the interference functional groups were necessarily excluded. To this end, a unique synthetic methodology based on graphite reduction cascaded by electrophilic reaction was developed. The electron-withdrawing-type groups (Br; trifluoroacetyl: TFAc) and electron-donating-type counterparts (butyl: Bu; 4-methoxyphenyl: 4-MeOPh) were readily attached to graphene sheets at a comparable functionalization degree. As the electron density of carbon skeleton was enriched by electron-donating modules, particularly for Bu units, the lithium-storage capacity, rate capability and cyclability were appreciably boosted. For example, they had 512 and 286 mA h g^-1 at 0.5C and 2C, respectively; and 88 % of capacity retention after 500 cycles at 1C.

Keywords: Graphene electronic structure; Graphene functionalization; Graphite intercalation compounds; Lithium-ion batteries.