Journal
ACS APPLIED NANO MATERIALS
Volume 4, Issue 3, Pages 3232-3240Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c00412
Keywords
functionalized graphene oxide; amine functionalized graphene oxide; ethylene diamine; stitched graphene oxide sheets; thermal reduction; graphene oxide; reduced graphene oxide; density functional theory
Funding
- Australian Research Council [DP190100831]
- National Health and Medical Research Council (NHMRC), Australia [GNT1139060]
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Functionalization of graphene oxide with ethylene diamine can improve the performance of lithium-ion batteries, but there is still a lack of detailed understanding of stitching and reduction processes.
Diamine functionalization of GO continues to draw significant research attention because of the ability to manipulate the interlayer spacing between GO sheets. Control over the GO interlayer spacing has resulted in profound improvements in the capacitance and cyclic stability in lithium-ion batteries. The reaction of ethylene diamine (EDA) with GO has previously been reported to cause simultaneous stitching/crosslinking, reduction, and functionalization of GO. However, detailed understanding of stitching and reduction is still lacking. In the present work, we have used combinatorial experimental and computational approaches to determine the reactivity of EDA toward main oxygen-containing functional groups of GO (epoxy, hydroxyl, and carboxylic acid). Using excess EDA, we observed experimental predominant evidence of stitching, which was further corroborated with DFT calculations. However, no clear experimental evidence of reduction of GO as a result of reaction of EDA with GO was observed. DFT calculations revealed that the first step of EDA functionalization exhibits similar reaction energies for hydroxyl and epoxy groups. However, in regard to stitching, hydroxyl and carboxyl groups were energetically comparable. The present results have implications in regard to energy storage applications of these materials.
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