Unraveling the energy storage mechanism in graphene-based nonaqueous electrochemical capacitors by gap-enhanced Raman spectroscopy

Xiao-Ting Yin, En-Ming You, Ru-Yu Zhou, Li-Hong Zhu, Wei-Wei Wang, Kai-Xuan Li, Wu De-Yin, Yu Gu (), Jian-Feng Li (), Bing-Wei Mao and Jia-Wei Yan ()
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Xiao-Ting Yin: Xiamen University
En-Ming You: Jimei University
Ru-Yu Zhou: Xiamen University
Li-Hong Zhu: Xiamen University
Wei-Wei Wang: Xiamen University
Kai-Xuan Li: Xiamen University
Wu De-Yin: Xiamen University
Yu Gu: Xiamen University
Jian-Feng Li: Xiamen University
Bing-Wei Mao: Xiamen University
Jia-Wei Yan: Xiamen University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Graphene has been extensively utilized as an electrode material for nonaqueous electrochemical capacitors. However, a comprehensive understanding of the charging mechanism and ion arrangement at the graphene/electrolyte interface remain elusive. Herein, a gap-enhanced Raman spectroscopic strategy is designed to characterize the dynamic interfacial process of graphene with an adjustable number of layers, which is based on synergistic enhancement of localized surface plasmons from shell-isolated nanoparticles and a metal substrate. By employing such a strategy combined with complementary characterization techniques, we study the potential-dependent configuration of adsorbed ions and capacitance curves for graphene based on the number of layers. As the number of layers increases, the properties of graphene transform from a metalloid nature to graphite-like behavior. The charging mechanism shifts from co-ion desorption in single-layer graphene to ion exchange domination in few-layer graphene. The increase in area specific capacitance from 64 to 145 µF cm–2 is attributed to the influence on ion packing, thereby impacting the electrochemical performance. Furthermore, the potential-dependent coordination structure of lithium bis(fluorosulfonyl) imide in tetraglyme ([Li(G4)][FSI]) at graphene/electrolyte interface is revealed. This work adds to the understanding of graphene interfaces with distinct properties, offering insights for optimization of electrochemical capacitors.

Date: 2024
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DOI: 10.1038/s41467-024-49973-9

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