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Title: Pseudocapacitive Storage in Nanolayered Ti2NTx MXene Using Mg-Ion Electrolyte

Abstract

Electrochemical supercapacitors are hybrids of a capacitor and battery that rely on materials capable of storing charges via pseudocapacitive reactions in addition to conventional electrostatic double-layer charge storage. MXenes, a relatively new class of two-dimensional (2D) transition metal carbides and nitrides, are ideal candidates for supercapacitors due to their high electronic conductivity, high surface area, and ability to store charges via pseudocapacitive mechanisms. Nitride MXenes such as Ti2NTx are predicted to have higher pseudocapacitance than carbide MXenes but have not been explored experimentally. Here, we report on the synthesis, characterization, and pseudocapacitive charge storage mechanism in the Ti2NTx nitride MXene. Successful formation of nanolayered Ti2NTx MXene is characterized by XRD, SEM, and N2 physisorption analyses. The identity of the surface terminating groups Tx are assigned to primarily O and/or OH based on Raman, FTIR, and STEM-EELS. When tested in various electrolytes, the nanolayered Ti2NTx MXene exhibits pronounced reversible redox peaks and high areal capacitances (~1350 uF cm-2 in 1 M MgSO4 aqueous electrolyte) well exceeding that expected from a double-layer charge storage (~50 uF cm-2) showing that charge is stored in the Ti2NTx MXene via a pseudocapacitive mechanism. We report a trend in the capacitance as a function of cationmore » as follows: Mg2+ > Al3+ > H+ > Li+ > Na+ > K+, that matches theoretical predictions. Remarkably, nanolayered Ti2NTx MXene exhibits >200 F g-1 capacitance over a 1.0 V range in the Mg-ion electrolyte, and the capacitance increases to 160% of its initial value after 1000 cycles owing to the 2 e- process and the distinctive multilayer adsorption characteristic of the Mg2+ cation on the Ti2NTx MXene. Furthermore, these findings identify Ti2NTx MXene as a new pseudocapacitive material that possesses high capacitance and wide working voltage in a safe and environmentally friendly Mg-ion electrolyte.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1527333
Report Number(s):
NREL/JA-5900-73444
Journal ID: ISSN 2574-0970
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 5; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; energy storage; supercapacitor; 2D MXene; transition-metal nitride; pseudocapacitance

Citation Formats

Djire, Abdoulaye, Bos, Andre, Liu, Jun, Zhang, Hanyu, Miller, Elisa M., and Neale, Nathan R. Pseudocapacitive Storage in Nanolayered Ti2NTx MXene Using Mg-Ion Electrolyte. United States: N. p., 2019. Web. doi:10.1021/acsanm.9b00289.
Djire, Abdoulaye, Bos, Andre, Liu, Jun, Zhang, Hanyu, Miller, Elisa M., & Neale, Nathan R. Pseudocapacitive Storage in Nanolayered Ti2NTx MXene Using Mg-Ion Electrolyte. United States. doi:10.1021/acsanm.9b00289.
Djire, Abdoulaye, Bos, Andre, Liu, Jun, Zhang, Hanyu, Miller, Elisa M., and Neale, Nathan R. Mon . "Pseudocapacitive Storage in Nanolayered Ti2NTx MXene Using Mg-Ion Electrolyte". United States. doi:10.1021/acsanm.9b00289. https://www.osti.gov/servlets/purl/1527333.
@article{osti_1527333,
title = {Pseudocapacitive Storage in Nanolayered Ti2NTx MXene Using Mg-Ion Electrolyte},
author = {Djire, Abdoulaye and Bos, Andre and Liu, Jun and Zhang, Hanyu and Miller, Elisa M. and Neale, Nathan R.},
abstractNote = {Electrochemical supercapacitors are hybrids of a capacitor and battery that rely on materials capable of storing charges via pseudocapacitive reactions in addition to conventional electrostatic double-layer charge storage. MXenes, a relatively new class of two-dimensional (2D) transition metal carbides and nitrides, are ideal candidates for supercapacitors due to their high electronic conductivity, high surface area, and ability to store charges via pseudocapacitive mechanisms. Nitride MXenes such as Ti2NTx are predicted to have higher pseudocapacitance than carbide MXenes but have not been explored experimentally. Here, we report on the synthesis, characterization, and pseudocapacitive charge storage mechanism in the Ti2NTx nitride MXene. Successful formation of nanolayered Ti2NTx MXene is characterized by XRD, SEM, and N2 physisorption analyses. The identity of the surface terminating groups Tx are assigned to primarily O and/or OH based on Raman, FTIR, and STEM-EELS. When tested in various electrolytes, the nanolayered Ti2NTx MXene exhibits pronounced reversible redox peaks and high areal capacitances (~1350 uF cm-2 in 1 M MgSO4 aqueous electrolyte) well exceeding that expected from a double-layer charge storage (~50 uF cm-2) showing that charge is stored in the Ti2NTx MXene via a pseudocapacitive mechanism. We report a trend in the capacitance as a function of cation as follows: Mg2+ > Al3+ > H+ > Li+ > Na+ > K+, that matches theoretical predictions. Remarkably, nanolayered Ti2NTx MXene exhibits >200 F g-1 capacitance over a 1.0 V range in the Mg-ion electrolyte, and the capacitance increases to 160% of its initial value after 1000 cycles owing to the 2 e- process and the distinctive multilayer adsorption characteristic of the Mg2+ cation on the Ti2NTx MXene. Furthermore, these findings identify Ti2NTx MXene as a new pseudocapacitive material that possesses high capacitance and wide working voltage in a safe and environmentally friendly Mg-ion electrolyte.},
doi = {10.1021/acsanm.9b00289},
journal = {ACS Applied Nano Materials},
number = 5,
volume = 2,
place = {United States},
year = {2019},
month = {5}
}

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