Control of electronic properties of 2D carbides (MXenes) by manipulating their transition metal layers

Anasori, Babak; Shi, Chenyang; Moon, Eun Ju; Xie, Yu; Voigt, Cooper A.; Kent, Paul R. C.; May, Steven J.; Billinge, Simon J. L.; Barsoum, Michel W.; Gogotsi, Yury

doi:10.1039/C5NH00125K

Control of electronic properties of 2D carbides (MXenes) by manipulating their transition metal layers

Journal Article · Wed Feb 24 00:00:00 EST 2016 · Nanoscale Horizons

DOI:https://doi.org/10.1039/C5NH00125K· OSTI ID:1261289

Anasori, Babak ^[1]; Shi, Chenyang ^[2]; Moon, Eun Ju ^[1]; Xie, Yu ^[3]; Voigt, Cooper A. ^[1]; Kent, Paul R. C. ^[3]; May, Steven J. ^[1]; Billinge, Simon J. L. ^[4]; Barsoum, Michel W. ^[1]; Gogotsi, Yury ^[1]

Drexel Univ., Philadelphia, PA (United States)
Columbia Univ., New York, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

In this paper, a transition from metallic to semiconducting-like behavior has been demonstrated in two-dimensional (2D) transition metal carbides by replacing titanium with molybdenum in the outer transition metal (M) layers of M₃C₂ and M₄C₃ MXenes. The MXene structure consists of n + 1 layers of near-close packed M layers with C or N occupying the octahedral site between them in an [MX]_nM arrangement. Recently, two new families of ordered 2D double transition metal carbides MXenes were discovered, M'₂M"C₂ and M'₂M"₂C₃ – where M' and M" are two different early transition metals, such as Mo, Cr, Ta, Nb, V, and Ti. The M' atoms only occupy the outer layers and the M" atoms fill the middle layers. In other words, M' atomic layers sandwich the middle M"–C layers. Using X-ray atomic pair distribution function (PDF) analysis on Mo₂TiC₂ and Mo₂Ti₂C₃ MXenes, we present the first quantitative analysis of structures of these novel materials and experimentally confirm that Mo atoms are in the outer layers of the [MC]_nM structures. The electronic properties of these Mo-containing MXenes are compared with their Ti₃C₂ counterparts, and are found to be no longer metallic-like conductors; instead the resistance increases mildly with decreasing temperatures. Density functional theory (DFT) calculations suggest that OH terminated Mo–Ti MXenes are semiconductors with narrow band gaps. Measurements of the temperature dependencies of conductivities and magnetoresistances have confirmed that Mo₂TiC₂T_x exhibits semiconductor-like transport behavior, while Ti₃C₂T_x is a metal. Finally, this finding opens new avenues for the control of the electronic and optical applications of MXenes and for exploring new applications, in which semiconducting properties are required.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Army Research Office (United States); Drexel Univ. (United States); King Abdullah Univ. of Science and Technology (KAUST) (Saudi Arabia); National Science Foundation (NSF) (United States); USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; SC0012704

OSTI ID:: 1261289

Alternate ID(s):: OSTI ID: 1327611
OSTI ID: 1354306

Journal Information:: Nanoscale Horizons, Journal Name: Nanoscale Horizons Journal Issue: 3 Vol. 1; ISSN 2055-6756

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Control of electronic properties of 2D carbides (MXenes) by manipulating their transition metal layers

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