Computational insight into the capacitive performance of graphene edge planes

Zhan, Cheng; Zhang, Yu; Cummings, Peter T.; Jiang, De-en

doi:10.1016/j.carbon.2017.01.104

Computational insight into the capacitive performance of graphene edge planes

Journal Article · Tue Jan 31 23:00:00 EST 2017 · Carbon

DOI:https://doi.org/10.1016/j.carbon.2017.01.104· OSTI ID:1399371

Zhan, Cheng ^[1]; Zhang, Yu ^[2]; Cummings, Peter T. ^[2]; ^[1]

Univ. of California, Riverside, CA (United States)
Vanderbilt Univ., Nashville, TN (United States)

Recent experiments have shown that electric double-layer capacitors utilizing electrodes consisting of graphene edge plane exhibit higher capacitance than graphene basal plane. However, theoretical understanding of this capacitance enhancement is still limited. Here we applied a self-consistent joint density functional theory calculation on the electrode/electrolyte interface and found that the capacitance of graphene edge plane depends on the edge type: zigzag edge has higher capacitance than armchair edge due to the difference in their electronic structures. We further examined the quantum, dielectric, and electric double-layer (EDL) contributions to the total capacitance of the edge-plane electrodes. Classical molecular dynamics simulation found that the edge planes have higher EDL capacitance than the basal plane due to better adsorption of counter-ions and higher solvent accessible surface area. Finally, our work therefore has elucidated the capacitive energy storage in graphene edge planes that take into account both the electrode's electronic structure and the EDL structure.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1399371

Alternate ID(s):: OSTI ID: 1396886

Journal Information:: Carbon, Journal Name: Carbon Journal Issue: C Vol. 116; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
capacitance
classical molecular dynamics
electric double-layer
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joint density functional theory

Computational insight into the capacitive performance of graphene edge planes

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