Article Ion Dynamics in Porous Carbon Electrodes in Supercapacitors Using in situ Infrared Spectroelectrochemistry

Ion Dynamics in Porous Carbon Electrodes in Supercapacitors Using in situ Infrared Spectroelectrochemistry

Francis W Richey , Boris Dyatkin , Yury Gogotsi ,  Yossef A Elabd

J. Am. Chem. Soc., Just Accepted Manuscript

DOI: 10.1021/ja406120e

Publication Date (Web): August 5, 2013

Abstract

Electrochemical double layer capacitors (EDLC), or supercapacitors, rely on electrosorption of ions by porous carbon electrodes and offer a higher power and a longer cyclic lifetime compared to batteries. Ionic liquid (IL) electrolytes can broaden the operating voltage window and increase the energy density of EDLCs. Herein, we present direct measurements of ion dynamics of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIm-TFSI) in an operating EDLC with electrodes composed of porous nanosized carbide-derived carbons (CDCs) and non-porous onion-like carbons (OLCs) with the use of in situ infrared spectroelectrochemistry. For CDC electrodes, IL ions (both cations and anions) were directly observed entering and exiting CDC nanopores during charging and discharging of the EDLC.

 

Ion Dynamics in Porous Carbon Electrodes in Supercapacitors Using in Situ Infrared Spectroelectrochemistry

Conversely, for OLC electrodes, IL ions were observed in close proximity to the OLC surface without any change in the bulk electrolyte concentration during charging and discharging of the EDLC. This provides experimental evidence that charge is stored on the surface of OLCs in OLC EDLCs without long-range ion transport through the bulk electrode. In addition, for CDC EDLCs with mixed electrolytes of IL and propylene carbonate (PC), the IL ions were observed entering and exiting CDC nanopores, while PC entrance into the nanopores was IL concentration dependent.

Figure S1. (a) BET analysis of CDC and OLC  particles. (b) SEM image of the gold current  collector/CDC electrode interface. (c) SEM image of electrode surface without gold. (d) Picture  of the CDC electrodes with gold current collector on surface.

This work provides direct experimental confirmation of EDLC charging mechanisms that previously were restricted to computational simulations and theories. The experimental measurements presented here also provide deep insights about the molecular level transport of IL ions in EDLC electrodes that will impact the design of electrode materials’ structure for electrical energy storage.

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