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

• Published in: Journal of colloid and interface science Vol. 635; pp. 543 - 551
• Main Authors: Li, Zhaoxin, Liu, Naxing, Wang, Jian, Xu, Yongqi, Bai, Li, Jiang, Long, Cui, Liang, Shen, Chengshuo, Liu, Xunshan, Zhao, Fu-Gang
• Format: Journal Article
• Language: English
• Published: United States Elsevier Inc 01.04.2023
• Subjects: Graphene carboxylation; Graphene functionalization; Graphene lithium storage; Graphene structure-performance relationship; Graphene sulfonation; Graphene functionalization; Graphene sulfonation; Graphene lithium storage; Graphene carboxylation; Graphene structure-performance relationship
• ISSN: 0021-9797; 1095-7103
• DOI: 10.1016/j.jcis.2022.12.140

To elucidate how different spatial oxygen-containing groups influenced lithium-storage performance of graphene matrix, and further establish a clear structure-performance relationship, graphene framework was strategically functionalized with carboxylate and sulfonate groups and oxygen-free aniline ones as a reference. Due to maximum lithiation effect, spatially sulfonate functionalized graphene delivered the best electrochemical performances in lithium-ion batteries. [Display omitted] 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.