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

Zhan, Cheng; Pham, Tuan Anh; Cerón, Maira R.; Campbell, Patrick G.; Vedharathinam, Vedasri; Otani, Minoru; Jiang, De-en; Biener, Juergen; Wood, Brandon C.; Biener, Monika

doi:10.1021/acsami.8b10349

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

Journal Article · Mon Oct 08 00:00:00 EDT 2018 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.8b10349· OSTI ID:1512603

Zhan, Cheng ^[1]; ^[2]; Cerón, Maira R. ^[2]; Campbell, Patrick G. ^[2]; Vedharathinam, Vedasri ^[2]; Otani, Minoru ^[3]; ^[4]; Biener, Juergen ^[2]; ^[2]; Biener, Monika ^[2]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of California, Riverside, CA (United States). Dept. of Chemistry
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (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, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 43 Vol. 10; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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