Integration of Fullerenes as Electron Acceptors in 3D Graphene Networks: Enhanced Charge Transfer and Stability through Molecular Design

Journal Article · Thu Jul 11 00:00:00 EDT 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.9b06681· OSTI ID:1558332

Cerón, Maira R.  ^[1]; Zhan, Cheng ^[1]; Campbell, Patrick G.  ^[1]; Freyman, Megan C. ^[1]; Santoyo, Christy ^[2]; Echegoyen, Luis  ^[2]; Wood, Brandon C. ^[1]; Biener, Juergen ^[1]; Pham, Tuan Anh  ^[1]; Biener, Monika M.  ^[1]

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1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
2. Univ. of Texas at El Paso, TX (United States)

Here, we report a concept that allows the integration of the characteristic properties of [60]fullerene in 3D graphene networks. In these systems, graphene provides high electrical conductivity and surface area while fullerenes add high electron affinity. We use molecular design to optimize the interaction between 3D graphene networks and fullerenes, specifically in the context of stability and charge transfer in an electrochemical environment. We demonstrated that the capacity of the 3D graphene network is critcally improved upon the addition of C₆₀ and C₆₀ monoadducts by providing additional acceptor states in the form of low-lying lowest unoccupied molecular orbitals of C₆₀ and its derivative. Guided by experimental results and first-principles calculations, we synthesized and tested a C₆₀ monoadduct with increased stability by strengthening the 3D graphene–C₆₀ van-der-Waals interactions. The synthesis approach and stabilization strategy presented here is expected to benefit the integration of graphene–C₆₀ hybrid materials in solar cell and charge storage applications.

• Research Organization: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
• Grant/Contract Number: AC52-07NA27344; AC02-05CH11231
• OSTI ID: 1558332
• Report Number(s): LLNL-JRNL-768044; 958302
• Journal Information: ACS Applied Materials and Interfaces, Vol. 11, Issue 32; ISSN 1944-8244
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

25 ENERGY STORAGE
77 NANOSCIENCE AND NANOTECHNOLOGY
36 MATERIALS SCIENCE
3D graphene network
[60]fullerene
charge transfer
electrochemical stability
capacity