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Title: Origins and Implications of Interfacial Capacitance Enhancements in C60-Modified Graphene Supercapacitors

Journal Article · · ACS Applied Materials and Interfaces
 [1]; ORCiD logo [2];  [2];  [2];  [2];  [3]; ORCiD logo [4];  [2]; ORCiD logo [2];  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
  4. Univ. of California, Riverside, CA (United States). Dept. of Chemistry

Understanding and controlling the electrical response at a complex electrode–electrolyte interface is key to the development of next-generation supercapacitors and other electrochemical devices. In this work, we apply a theoretical framework based on the effective screening medium and reference interaction site model to explore the role of electrical double-layer (EDL) formation and its interplay with quantum capacitance in graphene-based supercapacitors. In addition to pristine graphene, we investigate a novel C60-modified graphene supercapacitor material, which promises higher charge-storage capacity. Beyond the expected enhancement in the quantum capacitance, we find that the introduction of C60 molecules significantly alters the EDL response. These changes in EDL are traced to the interplay between surface morphology and charge localization character and ultimately dominate the overall capacitive improvement in the hybrid system. Our study highlights a complex interplay among surface morphology, electronic structure, and interfacial capacitance, suggesting general improvement strategies for optimizing carbon-based supercapacitor materials.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1512603
Report Number(s):
LLNL-JRNL-754189; 940742
Journal Information:
ACS Applied Materials and Interfaces, Vol. 10, Issue 43; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

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Cited By (4)

Specific ion effects at graphitic interfaces journal October 2019
Investigating the asymmetry in the EDL response of C 60 /graphene supercapacitors journal January 2019
Progress in supercapacitors: roles of two dimensional nanotubular materials journal January 2020
A first-principles roadmap and limits to design efficient supercapacitor electrode materials journal January 2019

Figures / Tables (4)