Alkali cation stabilization of defects in 2D MXenes at ambient and elevated temperatures

Brian C. Wyatt, Matthew G. Boebinger, Zachary D. Hood, Shiba Adhikari, Paweł Piotr Michałowski, Srinivasa Kartik Nemani, Murali Gopal Muraleedharan, Annabelle Bedford, Wyatt J. Highland, Paul R.C. Kent, Raymond R. Unocic, Babak Anasori

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Transition metal carbides have been adopted in energy storage, conversion, and extreme environment applications. Advancements in their 2D counterparts, known as MXenes, enable the design of unique structures at the ~1 nm thickness scale. Alkali cations have been essential in MXenes manufacturing processing, storage, and applications, however, exact interactions of these cations with MXenes are not fully understood. In this study, using Ti3C2Tx, Mo2TiC2Tx, and Mo2Ti2C3Tx MXenes, we present how transition metal vacancy sites are occupied by alkali cations, and their effect on MXene structure stabilization to control MXene’s phase transition. We examine this behavior using in situ high-temperature x-ray diffraction and scanning transmission electron microscopy, ex situ techniques such as atomic-layer resolution secondary ion mass spectrometry, and density functional theory simulations. In MXenes, this represents an advance in fundamentals of cation interactions on their 2D basal planes for MXenes stabilization and applications. Broadly, this study demonstrates a potential new tool for ideal phase-property relationships of ceramics at the atomic scale.

Original languageEnglish
Article number6353
JournalNature Communications
Volume15
Issue number1
DOIs
StatePublished - Dec 2024

Funding

B.C.W., S.K.N., A.B., W.J.H., and B.A. thank the Office of Naval Research (ONR) for funding this research under award number N0 0 014-21-1-2799. B.C.W. acknowledges financial support from the National Defense Engineering & Science Graduate (NDSEG) Fellowship Program. All STEM-EELS characterization was conducted at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy (DOE), Office of Science User Facility. Z.D.H. and S.P.A. were supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. P.P.M. was supported by the National Science Center (Project No. 2018/31/D/ST5/00399) and the National Center for Research and Development (Project No. LIDER/8/0055/L-12/20/NCBR/2021). Computational work performed by M.G.M. and P.R.C.K. at ORNL was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences.\u00A0We thank the Purdue University Libraries Open Access Publishing Fund for partially supporting the open-access publication of this article. We also\u00A0thank the Integrated Nanosystems Development Institute of Indiana University\u00A0Indianapolis as well as the\u00A0National Science Foundation Major Research Instrumentation Program for the use of their SEM and XRD equipment\u00A0(Award 1229514 for SEM and Award 1429241 for XRD). B.C.W., S.K.N., A.B., W.J.H., and B.A. thank the Office of Naval Research (ONR) for funding this research under award number N0 0 014-21-1-2799. B.C.W. acknowledges financial support from the National Defense Engineering & Science Graduate (NDSEG) Fellowship Program. All STEM-EELS characterization was conducted at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy (DOE), Office of Science User Facility. Z.D.H. and S.P.A. were supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. P.P.M. was supported by the National Science Center (Project No. 2018/31/D/ST5/00399) and the National Center for Research and Development (Project No. LIDER/8/0055/L-12/20/NCBR/2021). Computational work performed by M.G.M. and P.R.C.K. at ORNL was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. We thank the Purdue University Libraries Open Access Publishing Fund for partially supporting the open-access publication of this article. We also thank the Integrated Nanosystems Development Institute of Indiana University Indianapolis as well as the National Science Foundation Major Research Instrumentation Program for the use of their SEM and XRD equipment (Award 1229514 for SEM and Award 1429241 for XRD).

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