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Journal article
Spectroscopic signature of negative electronic compressibility from the Ti core-level of titanium carbonitride MXene
Applied physics reviews, v 8(2)
Jun 2021
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Abstract
Two-dimensional transition metal carbides, carbonitrides, and nitrides, called MXenes, exhibit high metallic conductivity, ion intercalation capability, and reversible redox activity, prompting their applications in energy storage and conversion, electromagnetic interference (EMI) shielding, and electronics, among many other fields. It has been shown that replacement of ∼50% of carbon atoms in the most popular MXene family member, titanium carbide (Ti3C2Tx), by nitrogen atoms, forming titanium carbonitride (Ti3CNTx), leads to drastically different properties. Such properties include very high negative charge in solution and extreme EMI shielding effectiveness, exceeding all known materials, even metals at comparable thicknesses. Here, by using ultraviolet photoemission spectroscopy (UPS), the electronic structures of Ti3CNTx and Ti3C2Tx are systematically investigated and compared as a function of charge carrier density. We observe that, in contrast to Ti3C2Tx, the Ti 3p core-level of Ti3CNTx exhibits a counterintuitive shift to a lower binding energy of up to ∼250 meV upon increasing the electron density, which is a spectroscopic signature of negative electronic compressibility (NEC). These experimentally measured chemical potential shifts are well captured by the density functional theory (DFT) calculation. The DFT results also further suggest that the hybridization of titanium–nitrogen bonding in Ti3CNTx helps to promote the available states of Ti atoms for receiving more electrons above the fermi level and leads to the observed NEC. Our findings explain the differences in electronic properties between the two very important and widely studied MXenes and also suggest a new strategy to apply the NEC effect of Ti3CNTx in energy and charge storage applications.
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- Title
- Spectroscopic signature of negative electronic compressibility from the Ti core-level of titanium carbonitride MXene
- Creators
- Warakorn Jindata - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyKanit Hantanasirisakul - 8Thailand Center of Excellence in Physics (ThEP), MHESI, Bangkok 10400, ThailandTanachat Eknapakul - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyJonathan D Denlinger - Advanced Light Source, Lawrence Berkeley National LaboratorySuppanut Sangphet - 8Thailand Center of Excellence in Physics (ThEP), MHESI, Bangkok 10400, ThailandSujinda Chaiyachad - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyChutchawan Jaisuk - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyAissara Rasritat - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyTanawat Sawasdee - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologyHideki Nakajima - Synchrotron Light Research InstituteArunothai Rattanachata - Synchrotron Light Research InstituteIttipon Fongkaew - School of Physics and Center of Excellence on Advanced Functional Materials, Suranaree University of TechnologySukit Limpijumnong - 8Thailand Center of Excellence in Physics (ThEP), MHESI, Bangkok 10400, ThailandYury Gogotsi - 8Thailand Center of Excellence in Physics (ThEP), MHESI, Bangkok 10400, ThailandWorawat Meevasana - 8Thailand Center of Excellence in Physics (ThEP), MHESI, Bangkok 10400, Thailand
- Publication Details
- Applied physics reviews, v 8(2)
- Publisher
- American Institute of Physics (AIP)
- Number of pages
- 9
- Grant note
- DE-SC0018618 / U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, USA B05F630108 / Program Management Unit for Human Resource & Institutional Developement, Research and Innovation DE-AC02-05CH11231 / U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, USA
- Resource Type
- Journal article
- Academic Unit
- Materials Science and Engineering
- Web of Science ID
- WOS:000637926900001
- Scopus ID
- 2-s2.0-85103909551
- Other Identifier
- 991014970024904721
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Physics, Applied