Carbons with Regular Pore Geometry Yield Fundamental Insights into Supercapacitor Charge Storage

Liu, Yifei Michelle; Merlet, Céline; Smit, Berend

doi:10.1021/acscentsci.9b00800

Title: Carbons with Regular Pore Geometry Yield Fundamental Insights into Supercapacitor Charge Storage

Journal Article · 15 November 2019 · ACS Central Science

DOI: https://doi.org/10.1021/acscentsci.9b00800 · OSTI ID:1591831

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Univ. of California, Berkeley, CA (United States); École polytechnique fédérale de Lausanne (EPFL), Sion (Switzerland)
Univ. de Toulouse (France); Federation de Recherche CNRS, Amiens (France)

We conduct molecular dynamics simulations of electrical double-layer capacitors (EDLCs) using a library of ordered, porous carbon electrode materials called zeolite templated carbons (ZTCs). The well-defined pore shapes of the ZTCs enable us to determine the influence of pore geometry on both charging dynamics and charge storage mechanisms in EDLCs, also referred to as supercapacitors. We show that charging dynamics are negatively correlated with the pore-limiting diameter of the electrode material and display signatures of both progressive charging and ion trapping. However, the equilibrium capacitance, unlike charging dynamics, is not strongly correlated to commonly used, purely geometric descriptors such as pore size. Instead, we find a strong correlation of capacitance to the charge compensation per carbon (CCpC), a descriptor we define in this work as the average charge of the electrode atoms within the coordination shell of a counterion. A high CCpC indicates efficient charge storage, as the strong partial charges of the electrode are able to screen counterion charge, enabling higher ion loading and thus more charge storage within the electrode at a fixed applied voltage. We determine that adsorption sites with a high CCpC tend to be found within pockets with a smaller radius of curvature, where the counterions are able to minimize their distance with multiple points on the electrode surface, and therefore induce stronger local partial charges.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; European Research Council (ERC)

Grant/Contract Number:: AC02-05CH11231; 714581

OSTI ID:: 1591831

Journal Information:: ACS Central Science, Vol. 5, Issue 11; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 42 works

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Three-Dimensionally Arrayed and Mutually Connected 1.2-nm Nanopores for High-Performance Electric Double Layer Capacitor Itoi, Hiroyuki; Nishihara, Hirotomo; Kogure, Taichi Journal of the American Chemical Society, Vol. 133, Issue 5 https://doi.org/10.1021/ja108315p	journal	February 2011
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Oscillation of Capacitance inside Nanopores Jiang, De-en; Jin, Zhehui; Wu, Jianzhong Nano Letters, Vol. 11, Issue 12 https://doi.org/10.1021/nl202952d	journal	December 2011
Complex Capacitance Scaling in Ionic Liquids-Filled Nanopores Wu, Peng; Huang, Jingsong; Meunier, Vincent ACS Nano, Vol. 5, Issue 11 https://doi.org/10.1021/nn203260w	journal	October 2011
On the Dynamics of Charging in Nanoporous Carbon-Based Supercapacitors Péan, Clarisse; Merlet, Céline; Rotenberg, Benjamin ACS Nano, Vol. 8, Issue 2 https://doi.org/10.1021/nn4058243	journal	January 2014
Lanthanum-catalysed synthesis of microporous 3D graphene-like carbons in a zeolite template Kim, Kyoungsoo; Lee, Taekyoung; Kwon, Yonghyun Nature, Vol. 535, Issue 7610 https://doi.org/10.1038/nature18284	journal	June 2016
Highly confined ions store charge more efficiently in supercapacitors Merlet, C.; Péan, C.; Rotenberg, B. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3701	journal	October 2013
Efficient storage mechanisms for building better supercapacitors Salanne, M.; Rotenberg, B.; Naoi, K. Nature Energy, Vol. 1, Issue 6 https://doi.org/10.1038/nenergy.2016.70	journal	May 2016
Accelerating charging dynamics in subnanometre pores Kondrat, Svyatoslav; Wu, Peng; Qiao, Rui Nature Materials, Vol. 13, Issue 4 https://doi.org/10.1038/nmat3916	journal	March 2014
Nanoporous carbide-derived carbon with tunable pore size Gogotsi, Yury; Nikitin, Alexei; Ye, Haihui Nature Materials, Vol. 2, Issue 9 https://doi.org/10.1038/nmat957	journal	August 2003
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Electrochemical interface between an ionic liquid and a model metallic electrode Reed, Stewart K.; Lanning, Oliver J.; Madden, Paul A. The Journal of Chemical Physics, Vol. 126, Issue 8 https://doi.org/10.1063/1.2464084	journal	February 2007
Influence of surface topology and electrostatic potential on water/electrode systems Siepmann, J. Ilja; Sprik, Michiel The Journal of Chemical Physics, Vol. 102, Issue 1 https://doi.org/10.1063/1.469429	journal	January 1995
Evaluation of the constant potential method in simulating electric double-layer capacitors Wang, Zhenxing; Yang, Yang; Olmsted, David L. The Journal of Chemical Physics, Vol. 141, Issue 18 https://doi.org/10.1063/1.4899176	journal	November 2014
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Anomalous Increase in Carbon Capacitance at Pore Sizes Less Than 1 Nanometer Chmiola, J. Science, Vol. 313, Issue 5794 https://doi.org/10.1126/science.1132195	journal	September 2006
Increasing Capacitance of Zeolite-Templated Carbons in Electric Double Layer Capacitors Moon, Jong Seok; Kim, Hyea; Lee, Dong-Chan Journal of The Electrochemical Society, Vol. 162, Issue 5 https://doi.org/10.1149/2.0131505jes	journal	January 2015
Review of Battery Systems for Electrically Powered Vehicles Ragone, D. V. Mid-Year Meeting, SAE Technical Paper Series https://doi.org/10.4271/680453	conference	May 1968

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