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Title: Electrocatalytic and Optoelectronic Characteristics of the Two-Dimensional Titanium Nitride Ti 4N 3T x MXene

Abstract

A relatively new class of two-dimensional (2D) materials called MXenes have garnered tremendous interest in the field of energy storage and conversion. Thus far nearly all MXenes reported experimentally have been described as metals, with a lone report of a mixed-metal carbide phase exhibiting semiconducting character. Here, we report the optical, electrocatalytic, and electrical properties of the 2D Ti 4N 3T x MXene (Tx = basal plane surface terminating groups) and show that this material exhbits both metallic and semiconducting behaviors. We provide complete structural characterization of exfoliated Ti 4N 3T x MXene and assign T x = O and/or OH and find that this material is susceptible to surface oxidation. Optical experiments indicate that the exfoliated Ti 4N 3T x MXene forms a hybrid with a thin surface oxide layer resulting in visible light absorbtion at energies greater than ~2.0 eV and an excitation wavelength-dependent defect-state emission over a broad range centered at ~2.9 eV. As an electrocatalyst for the hydrogen evolution reaction, the exfoliated Ti 4N 3T x shows an overpotential of ~300 mV at -10 mA cm -2 and a Tafel slope of ~190 mV dec -1. Finally, we observe semiconducting behavior at temperatures below ~90 Kmore » from temperature-dependent transport measurements under 5 T magnetic field likely resulting from the thin oxide layer. These results unveil the intriguing optical, electrocatalytic, and electrical properties of this 2D Ti 4N 3T x MXene that expands the potential of these new 2D materials into electrocatalysis and (opto)electronic applications.« less

Authors:
 [1];  [1];  [1];  [1];  [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:
1506614
Report Number(s):
NREL/JA-5900-71662
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 12; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 2D materials; energy conversion; nitride MXenes; semiconductors; water splitting

Citation Formats

Djire, Abdoulaye, Zhang, Hanyu, Liu, Jun, Miller, Elisa M., and Neale, Nathan R. Electrocatalytic and Optoelectronic Characteristics of the Two-Dimensional Titanium Nitride Ti4N3Tx MXene. United States: N. p., 2019. Web. doi:10.1021/acsami.9b01150.
Djire, Abdoulaye, Zhang, Hanyu, Liu, Jun, Miller, Elisa M., & Neale, Nathan R. Electrocatalytic and Optoelectronic Characteristics of the Two-Dimensional Titanium Nitride Ti4N3Tx MXene. United States. doi:10.1021/acsami.9b01150.
Djire, Abdoulaye, Zhang, Hanyu, Liu, Jun, Miller, Elisa M., and Neale, Nathan R. Mon . "Electrocatalytic and Optoelectronic Characteristics of the Two-Dimensional Titanium Nitride Ti4N3Tx MXene". United States. doi:10.1021/acsami.9b01150.
@article{osti_1506614,
title = {Electrocatalytic and Optoelectronic Characteristics of the Two-Dimensional Titanium Nitride Ti4N3Tx MXene},
author = {Djire, Abdoulaye and Zhang, Hanyu and Liu, Jun and Miller, Elisa M. and Neale, Nathan R.},
abstractNote = {A relatively new class of two-dimensional (2D) materials called MXenes have garnered tremendous interest in the field of energy storage and conversion. Thus far nearly all MXenes reported experimentally have been described as metals, with a lone report of a mixed-metal carbide phase exhibiting semiconducting character. Here, we report the optical, electrocatalytic, and electrical properties of the 2D Ti4N3Tx MXene (Tx = basal plane surface terminating groups) and show that this material exhbits both metallic and semiconducting behaviors. We provide complete structural characterization of exfoliated Ti4N3Tx MXene and assign Tx = O and/or OH and find that this material is susceptible to surface oxidation. Optical experiments indicate that the exfoliated Ti4N3Tx MXene forms a hybrid with a thin surface oxide layer resulting in visible light absorbtion at energies greater than ~2.0 eV and an excitation wavelength-dependent defect-state emission over a broad range centered at ~2.9 eV. As an electrocatalyst for the hydrogen evolution reaction, the exfoliated Ti4N3Tx shows an overpotential of ~300 mV at -10 mA cm-2 and a Tafel slope of ~190 mV dec-1. Finally, we observe semiconducting behavior at temperatures below ~90 K from temperature-dependent transport measurements under 5 T magnetic field likely resulting from the thin oxide layer. These results unveil the intriguing optical, electrocatalytic, and electrical properties of this 2D Ti4N3Tx MXene that expands the potential of these new 2D materials into electrocatalysis and (opto)electronic applications.},
doi = {10.1021/acsami.9b01150},
journal = {ACS Applied Materials and Interfaces},
number = 12,
volume = 11,
place = {United States},
year = {2019},
month = {3}
}

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