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Title: Understanding the MXene Pseudocapacitance

Abstract

MXenes have attracted great attention as next-generation capacitive energy-storage materials, but the mechanisms underlying their pseudocapacitive behavior are not well understood. Here we provide a theoretical description of the surface redox process of Ti3C2Tx (T = O, OH), a prototypical MXene, in 1 M H2SO4 electrolyte, based on joint density functional theory with an implicit solvation model and the analysis of Gibbs free energy under a constant-electrode potential. From the dependence of the O/OH ratio (or the surface H coverage) and the surface charge on the applied potential, we obtain a clear picture of the capacitive energy-storage mechanism of Ti3C2Tx that shows good agreement with previous experimental findings in terms of the integral capacitance and Ti valence change. We find a voltage-dependent redox/double-layer co-charging behavior: the capacitive mechanism is dominated by the redox process, but the electric double-layer charge works against the redox process. This new insight may be useful in improving the capacitance of MXenes.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [1]
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  1. Univ. of California, Riverside, CA (United States)
  2. Tulane Univ., New Orleans, LA (United States)
  3. Drexel Univ., Philadelphia, PA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1493989
Alternate Identifier(s):
OSTI ID: 1484259
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhan, Cheng, Naguib, Michael, Lukatskaya, Maria, Kent, Paul R. C., Gogotsi, Yury, and Jiang, De-en. Understanding the MXene Pseudocapacitance. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b00200.
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Zhan, Cheng, Naguib, Michael, Lukatskaya, Maria, Kent, Paul R. C., Gogotsi, Yury, & Jiang, De-en. Understanding the MXene Pseudocapacitance. United States. doi:10.1021/acs.jpclett.8b00200.
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Zhan, Cheng, Naguib, Michael, Lukatskaya, Maria, Kent, Paul R. C., Gogotsi, Yury, and Jiang, De-en. Tue . "Understanding the MXene Pseudocapacitance". United States. doi:10.1021/acs.jpclett.8b00200. https://www.osti.gov/servlets/purl/1493989.
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@article{osti_1493989,
title = {Understanding the MXene Pseudocapacitance},
author = {Zhan, Cheng and Naguib, Michael and Lukatskaya, Maria and Kent, Paul R. C. and Gogotsi, Yury and Jiang, De-en},
abstractNote = {MXenes have attracted great attention as next-generation capacitive energy-storage materials, but the mechanisms underlying their pseudocapacitive behavior are not well understood. Here we provide a theoretical description of the surface redox process of Ti3C2Tx (T = O, OH), a prototypical MXene, in 1 M H2SO4 electrolyte, based on joint density functional theory with an implicit solvation model and the analysis of Gibbs free energy under a constant-electrode potential. From the dependence of the O/OH ratio (or the surface H coverage) and the surface charge on the applied potential, we obtain a clear picture of the capacitive energy-storage mechanism of Ti3C2Tx that shows good agreement with previous experimental findings in terms of the integral capacitance and Ti valence change. We find a voltage-dependent redox/double-layer co-charging behavior: the capacitive mechanism is dominated by the redox process, but the electric double-layer charge works against the redox process. This new insight may be useful in improving the capacitance of MXenes.},
doi = {10.1021/acs.jpclett.8b00200},
journal = {Journal of Physical Chemistry Letters},
number = 6,
volume = 9,
place = {United States},
year = {2018},
month = {2}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI:  10.1021/acs.jpclett.8b00200
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Cited by: 59 works
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Figures / Tables:

Figure 1 Figure 1: Partially protonated Ti3C2O2 as a prototypical MXene electrode in an acidic electrolyte: side view (left) and top view (right). The 2D material has an ideal surface area (counting two sides) of ∼479 m2/g.
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Works referencing / citing this record:

High-capacitance Ti 3 C 2 T x MXene obtained by etching submicron Ti 3 AlC 2 grains grown in molten salt
journal, January 2018

  • Cui, Cong; Hu, Minmin; Zhang, Chao
  • Chemical Communications, Vol. 54, Issue 58
  • DOI: 10.1039/c8cc04350g

Electrochromic Effect in Titanium Carbide MXene Thin Films Produced by Dip‐Coating
journal, February 2019

  • Salles, Pol; Pinto, David; Hantanasirisakul, Kanit
  • Advanced Functional Materials, Vol. 29, Issue 17
  • DOI: 10.1002/adfm.201809223

Revealing the Pseudo‐Intercalation Charge Storage Mechanism of MXenes in Acidic Electrolyte
journal, May 2019

  • Mu, Xinpeng; Wang, Dashuai; Du, Fei
  • Advanced Functional Materials, Vol. 29, Issue 29
  • DOI: 10.1002/adfm.201902953

MXene‐Based Composites: Synthesis and Applications in Rechargeable Batteries and Supercapacitors
journal, February 2019

  • Yang, Jian; Bao, Weizhai; Jaumaux, Pauline
  • Advanced Materials Interfaces, Vol. 6, Issue 8
  • DOI: 10.1002/admi.201802004

MXene-Conducting Polymer Asymmetric Pseudocapacitors
journal, December 2018

Electrochemical Behavior of Ti 3 C 2 T x MXene in Environmentally Friendly Methanesulfonic Acid Electrolyte
journal, August 2019

  • Zhao, Xin; Dall'Agnese, Chunxiang; Chu, Xue‐Feng
  • ChemSusChem, Vol. 12, Issue 19
  • DOI: 10.1002/cssc.201901746

Automated Scalpel Patterning of Solution Processed Thin Films for Fabrication of Transparent MXene Microsupercapacitors
journal, October 2018

Highly Conductive Ti 3 C 2 T x MXene Hybrid Fibers for Flexible and Elastic Fiber-Shaped Supercapacitors
journal, January 2019

Highly Enhanced Pseudocapacitive Performance of Vanadium‐Doped MXenes in Neutral Electrolytes
journal, August 2019

Delaminating Vanadium Carbides for Zinc‐Ion Storage: Hydrate Precipitation and H + /Zn 2+ Co‐Action Mechanism
journal, August 2019

Layer-by-layer self-assembly of pillared two-dimensional multilayers
journal, June 2019

Applications of 2D MXenes in energy conversion and storage systems
journal, January 2019

  • Pang, Jinbo; Mendes, Rafael G.; Bachmatiuk, Alicja
  • Chemical Society Reviews, Vol. 48, Issue 1
  • DOI: 10.1039/c8cs00324f

Two-dimensional transitional metal dihydride crystals with anisotropic and spin-polarized Fermi Dirac cones
journal, January 2018

  • Lv, Haifeng; Wu, Daoxiong; Li, Xiuling
  • Journal of Materials Chemistry C, Vol. 6, Issue 42
  • DOI: 10.1039/c8tc03489c

A first-principles roadmap and limits to design efficient supercapacitor electrode materials
journal, January 2019

  • Ali, Basant A.; Allam, Nageh K.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 32
  • DOI: 10.1039/c9cp02614b

Origin of theoretical pseudocapacitance of two-dimensional supercapacitor electrodes Ti 3 C 2 T 2 (T = bare, O, S)
journal, January 2019

  • Wang, Lijing; Wang, Jin; Zhang, Zhenzhou
  • Journal of Materials Chemistry A, Vol. 7, Issue 27
  • DOI: 10.1039/c9ta03529j

Superfast high-energy storage hybrid device composed of MXene and Chevrel-phase electrodes operated in saturated LiCl electrolyte solution
journal, January 2019

  • Malchik, Fyodor; Shpigel, Netanel; Levi, Mikhael D.
  • Journal of Materials Chemistry A, Vol. 7, Issue 34
  • DOI: 10.1039/c9ta08066j

The development of 2D materials for electrochemical energy applications: A mechanistic approach
journal, March 2019

  • Hynek, David J.; Pondick, Joshua V.; Cha, Judy J.
  • APL Materials, Vol. 7, Issue 3
  • DOI: 10.1063/1.5085187

Distinguishing electronic contributions of surface and sub-surface transition metal atoms in Ti-based MXenes
journal, February 2020

Interfacial and electronic properties of heterostructures of MXene and graphene
journal, February 2019

Probing the pseudocapacitance and energy-storage performance of RuO 2 facets from first principles
journal, August 2019

Review on Carbon/Polyaniline Hybrids: Design and Synthesis for Supercapacitor
journal, June 2019

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