Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 3, Issue 13, Pages 1732-1737Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz300506j
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Funding
- NSF [CBET-0967175]
- Oak Ridge National Laboratory (ORNL)
- Center for Nanophase Materials Sciences
- Scientific User Facilities Division by the Office of Basic Energy Sciences, U.S. Department of Energy
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [0967175] Funding Source: National Science Foundation
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Using molecular dynamics simulations, we show that charge storage in subnanometer pores follows a distinct voltage dependent behavior. Specifically, at lower voltages, charge storage is achieved by swapping co-ions in the pore with counterions in the bulk electrolyte. As voltage increases, further charge storage is due mainly to the removal of co-ions from the pore, leading to a capacitance increase. The capacitance eventually reaches a maximum when all co-ions are expelled from the pore. At even higher electrode voltages, additional charge storage is realized by counterion insertion into the pore, accompanied by a reduction of capacitance. The molecular mechanisms of these observations are elucidated and provide useful insight for optimizing energy storage based on supercapacitors.
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