Tracking ion intercalation into layered Ti3C2 MXene films across length scales
Abstract
Enhancing the energy stored and power delivered by layered materials relies strongly on improved understanding of the intricate interplay of electrolyte ions, solvents, and electrode interactions as well as the role of confinement. Here we report a highly integrated study with multiscale theory/modelling and experiments to track the intercalation of aqueous Li+, Na+, K+, Cs+, and Mg2+ ions into Ti3C2 MXene. The integrated analysis of experiments assisted by theory/modelling allows for a deep understanding of energy storage processes highlighting the importance of the dynamics of cations, their positionings between MXene sheets, their effects on mechanical properties and capacitive energy storage. Computational simulations and operando calorimetry measurements prove the processes involving cation dehydration and H+ rehydration, showing a good correlation for heat variations between experiments and theory. Operando liquid AFM mapped energy dissipation of ions appears non-uniformly across the MXene surface, indicating heterogeneities of ions inside the MXene and confirming partially the ion behaviour obtained in theory. We directly demonstrate that the average distance between the cation and MXene surface follows a modified two-sided Helmholtz model when plotted versus the open circuit potential capacitance, revealing a different electrical double layer mechanism in confinement. This new fundamental understanding lays the foundation formore »
- Authors:
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[1];
[2];
[3];
[4];
[5];
[3];
[1];
[1];
[5];
[1];
[1]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Southeast Univ., Nanjing (China). SEU-FEI Nano-Pico Center, Key Lab. of MEMS
- Georgia State Univ., Atlanta, GA (United States)
- Univ. of Aveiro (Portugal). CICECO-Aveiro Inst. of Materials
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Tulane Univ., New Orleans, LA (United States)
- Drexel Univ., Philadelphia, PA (United States). Drexel Nanomaterials Inst.
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1657925
- Alternate Identifier(s):
- OSTI ID: 1638523
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy & Environmental Science
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 8; Journal ID: ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Gao, Qiang, Sun, Weiwei, Ilani-Kashkouli, Poorandokht, Tselev, Alexander, Kent, Paul C., Kabengi, Nadine, Naguib, Michael, Alhabeb, Mohamed, Tsai, Wan-Yu, Baddorf, Arthur P., Huang, Jingsong, Jesse, Stephen, Gogotsi, Yury, and Balke, Nina. Tracking ion intercalation into layered Ti3C2 MXene films across length scales. United States: N. p., 2020.
Web. doi:10.1039/d0ee01580f.
Gao, Qiang, Sun, Weiwei, Ilani-Kashkouli, Poorandokht, Tselev, Alexander, Kent, Paul C., Kabengi, Nadine, Naguib, Michael, Alhabeb, Mohamed, Tsai, Wan-Yu, Baddorf, Arthur P., Huang, Jingsong, Jesse, Stephen, Gogotsi, Yury, & Balke, Nina. Tracking ion intercalation into layered Ti3C2 MXene films across length scales. United States. https://doi.org/10.1039/d0ee01580f
Gao, Qiang, Sun, Weiwei, Ilani-Kashkouli, Poorandokht, Tselev, Alexander, Kent, Paul C., Kabengi, Nadine, Naguib, Michael, Alhabeb, Mohamed, Tsai, Wan-Yu, Baddorf, Arthur P., Huang, Jingsong, Jesse, Stephen, Gogotsi, Yury, and Balke, Nina. Wed .
"Tracking ion intercalation into layered Ti3C2 MXene films across length scales". United States. https://doi.org/10.1039/d0ee01580f. https://www.osti.gov/servlets/purl/1657925.
@article{osti_1657925,
title = {Tracking ion intercalation into layered Ti3C2 MXene films across length scales},
author = {Gao, Qiang and Sun, Weiwei and Ilani-Kashkouli, Poorandokht and Tselev, Alexander and Kent, Paul C. and Kabengi, Nadine and Naguib, Michael and Alhabeb, Mohamed and Tsai, Wan-Yu and Baddorf, Arthur P. and Huang, Jingsong and Jesse, Stephen and Gogotsi, Yury and Balke, Nina},
abstractNote = {Enhancing the energy stored and power delivered by layered materials relies strongly on improved understanding of the intricate interplay of electrolyte ions, solvents, and electrode interactions as well as the role of confinement. Here we report a highly integrated study with multiscale theory/modelling and experiments to track the intercalation of aqueous Li+, Na+, K+, Cs+, and Mg2+ ions into Ti3C2 MXene. The integrated analysis of experiments assisted by theory/modelling allows for a deep understanding of energy storage processes highlighting the importance of the dynamics of cations, their positionings between MXene sheets, their effects on mechanical properties and capacitive energy storage. Computational simulations and operando calorimetry measurements prove the processes involving cation dehydration and H+ rehydration, showing a good correlation for heat variations between experiments and theory. Operando liquid AFM mapped energy dissipation of ions appears non-uniformly across the MXene surface, indicating heterogeneities of ions inside the MXene and confirming partially the ion behaviour obtained in theory. We directly demonstrate that the average distance between the cation and MXene surface follows a modified two-sided Helmholtz model when plotted versus the open circuit potential capacitance, revealing a different electrical double layer mechanism in confinement. This new fundamental understanding lays the foundation for improved functional devices utilizing electrodes and membranes made of two-dimensional materials.},
doi = {10.1039/d0ee01580f},
journal = {Energy & Environmental Science},
number = 8,
volume = 13,
place = {United States},
year = {Wed Jul 08 00:00:00 EDT 2020},
month = {Wed Jul 08 00:00:00 EDT 2020}
}
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