Multiscale and Multimodal Characterization of 2D Titanium Carbonitride MXene

Sun, Weiwei; Wang, Hsiu‐Wen; Vlcek, Lukas; Peng, Jing; Brady, Alexander B.; Osti, Naresh C.; Mamontov, Eugene; Tyagi, Madhusudan; Nanda, Jagjit; Greenbaum, Steven G.; Kent, Paul C.; Naguib, Michael

doi:10.1002/admi.201902207

Multiscale and Multimodal Characterization of 2D Titanium Carbonitride MXene

Journal Article · Tue Apr 28 00:00:00 EDT 2020 · Advanced Materials Interfaces

DOI:https://doi.org/10.1002/admi.201902207· OSTI ID:1761652

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Beijang Univ. (China); Hunter College of the City Univ. of New York, NY (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
Hunter College of the City Univ. of New York, NY (United States)
Tulane Univ., New Orleans, LA (United States)

Here, a comprehensive study on the prototype solid solution phase carbonitride MXene Ti₃CN is conducted using nuclear magnetic resonance, electron spin resonance, total and quasi-elastic neutron scattering, combined with density functional theory-based electronic structure and molecular dynamic calculations. The combination of experiment and theory lead toward rational atomic structural models of Ti₃CN. The remnant Al ions from the etching process significantly tune the interlayer spacing, distinct from the more typical MXene, Ti₃C₂, prepared similarly. Neutron scattering indicates the surface terminations of Ti₃CN display high oxygen and fluorine concentrations and rather low hydroxyl and hydrogen concentrations. Calculations show that the structure including both the residual Al ions and mixed surface terminations give the best agreement with the measurements. The water molecules in Ti₃CN are highly immobile, in strong contrast to those in Ti₃C₂. The analysis of the electronic structure suggests that the nitride MXene displays higher conductivity than the carbides. Finally, the absence of hydroxyl groups in terminations, the solid-solution in the anion sites, the remnants within layers, and immobile water altogether make the carbonitrides a unique series in the MXene family, implying a further exploration of their exotic properties and applications in energy storage.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures, and Transport (FIRST) Center; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1761652

Alternate ID(s):: OSTI ID: 1616483
OSTI ID: 1879978

Journal Information:: Advanced Materials Interfaces, Journal Name: Advanced Materials Interfaces Journal Issue: 11 Vol. 7; ISSN 2196-7350

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

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