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Title: Evidence of molecular hydrogen trapped in two-dimensional layered titanium carbide-based MXene

Abstract

Two-dimensional transition metal carbides and nitrides (MXenes) are one of the largest and fastest growing families of materials. The presence of molecular hydrogen at ambient conditions in a MXene (Ti3C2Tx, where Tx represents a surface terminating species, including O, OH, and F) material is revealed here by inelastic and elastic neutron scatterings. The inelastic neutron-scattering spectrum measured at 5 K shows a peak at 14.6 meV, presenting a clear indication of the presence of parahydrogen in the MXene synthesized using 48% hydrofluoric acid and annealed at 110°C in vacuum prior to the measurement. An increase in the measurement temperature gradually reduces the peak intensity and increases the peak width due to the mobility of the molecular hydrogen in confinement. The presence of molecular hydrogen is confirmed further from the observed elastic intensity drop in a fixed energy-window scan of elastic intensity measurements in the temperature range of 10–35 K. Using milder etching conditions, ion intercalation, or an increase in the annealing temperature all result in the absence of the trapped hydrogen molecules in MXene. Here, the results of this paper can guide the development of MXene materials with desired properties and improve our understanding of the behavior of MXenes inmore » applications ranging from supercapacitors to hydrogen evolution reaction catalysis and hydrogen storage.« less

Authors:
 [1];  [1];  [2];  [3];  [1];  [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
  3. Drexel Univ., Philadelphia, PA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1376464
Alternate Identifier(s):
OSTI ID: 1371611
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 2; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Osti, Naresh C., Naguib, Michael, Tyagi, Madhusudan, Gogotsi, Yury, Kolesnikov, Alexander I., and Mamontov, Eugene. Evidence of molecular hydrogen trapped in two-dimensional layered titanium carbide-based MXene. United States: N. p., 2017. Web. doi:10.1103/PhysRevMaterials.1.024004.
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Osti, Naresh C., Naguib, Michael, Tyagi, Madhusudan, Gogotsi, Yury, Kolesnikov, Alexander I., & Mamontov, Eugene. Evidence of molecular hydrogen trapped in two-dimensional layered titanium carbide-based MXene. United States. https://doi.org/10.1103/PhysRevMaterials.1.024004
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Osti, Naresh C., Naguib, Michael, Tyagi, Madhusudan, Gogotsi, Yury, Kolesnikov, Alexander I., and Mamontov, Eugene. Mon . "Evidence of molecular hydrogen trapped in two-dimensional layered titanium carbide-based MXene". United States. https://doi.org/10.1103/PhysRevMaterials.1.024004. https://www.osti.gov/servlets/purl/1376464.
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@article{osti_1376464,
title = {Evidence of molecular hydrogen trapped in two-dimensional layered titanium carbide-based MXene},
author = {Osti, Naresh C. and Naguib, Michael and Tyagi, Madhusudan and Gogotsi, Yury and Kolesnikov, Alexander I. and Mamontov, Eugene},
abstractNote = {Two-dimensional transition metal carbides and nitrides (MXenes) are one of the largest and fastest growing families of materials. The presence of molecular hydrogen at ambient conditions in a MXene (Ti3C2Tx, where Tx represents a surface terminating species, including O, OH, and F) material is revealed here by inelastic and elastic neutron scatterings. The inelastic neutron-scattering spectrum measured at 5 K shows a peak at 14.6 meV, presenting a clear indication of the presence of parahydrogen in the MXene synthesized using 48% hydrofluoric acid and annealed at 110°C in vacuum prior to the measurement. An increase in the measurement temperature gradually reduces the peak intensity and increases the peak width due to the mobility of the molecular hydrogen in confinement. The presence of molecular hydrogen is confirmed further from the observed elastic intensity drop in a fixed energy-window scan of elastic intensity measurements in the temperature range of 10–35 K. Using milder etching conditions, ion intercalation, or an increase in the annealing temperature all result in the absence of the trapped hydrogen molecules in MXene. Here, the results of this paper can guide the development of MXene materials with desired properties and improve our understanding of the behavior of MXenes in applications ranging from supercapacitors to hydrogen evolution reaction catalysis and hydrogen storage.},
doi = {10.1103/PhysRevMaterials.1.024004},
journal = {Physical Review Materials},
number = 2,
volume = 1,
place = {United States},
year = {Mon Jul 17 00:00:00 EDT 2017},
month = {Mon Jul 17 00:00:00 EDT 2017}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1103/PhysRevMaterials.1.024004
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Cited by: 22 works
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Figures / Tables:

FIG. 1 FIG. 1: Inelastic neutron scattering spectrum of MXene synthesized using 48% HF (Ti3C2Tx) and annealed at 110 °C measured for 2 h at SEQUOIA spectrometer with Ei=50 meV, immediately after cooling the sample to T=8 K (blue circles, error bars represent one standard deviation). For comparison, the INS spectra aremore » also shown for MXenes synthesized using 48% HF (Ti3C2Tx) and annealed at 150 °C (pink squares), and synthesized using 10% HF (Ti3C2Tx-H) and annealed at 110 °C (green triangles), where the data were collected after the samples were cooled to T=8 K for 7 and 4 h, respectively.« less
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    Works referencing / citing this record:

    From the perspectives of DFT calculations, thermodynamic modeling, and kinetic Monte Carlo simulations: the interaction between hydrogen and Sc 2 C monolayers
    journal, January 2020

    • Le, Thong Nguyen-Minh; Chiu, Cheng-chau; Kuo, Jer-Lai
    • Physical Chemistry Chemical Physics, Vol. 22, Issue 8
    • DOI: 10.1039/c9cp05796j

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    • Osti, Naresh C.; Mamontov, Eugene
    • Sustainable Energy & Fuels, Vol. 4, Issue 4
    • DOI: 10.1039/c9se00829b
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