A theoretical investigation of the effect of Ga alloying on thermodynamic stability, electronic-structure, and oxidation resistance of Ti2AlC MAX phase

Sauceda, Daniel; Singh, Prashant; Arroyave, Raymundo

doi:10.1038/s41598-022-17365-y

A theoretical investigation of the effect of Ga alloying on thermodynamic stability, electronic-structure, and oxidation resistance of Ti₂AlC MAX phase

Journal Article · Fri Jul 29 00:00:00 EDT 2022 · Scientific Reports

DOI:https://doi.org/10.1038/s41598-022-17365-y· OSTI ID:1881903

Sauceda, Daniel ^[1]; Singh, Prashant ^[2]; Arroyave, Raymundo ^[1]

Texas A & M Univ., College Station, TX (United States)
Texas A & M Univ., College Station, TX (United States); Ames Lab., and Iowa State Univ., Ames, IA (United States)

We present a systematic investigation of thermodynamic stability, phase-reaction, and chemical activity of Al containing disordered Ti₂(Al-Ga)C MAX phases using machine-learning driven high-throughput framework to understand the oxidation resistance behavior with increasing temperature and exposure to static oxygen. The A-site (at Al) disordering of Ti₂AlC with Ga shows significant change in the chemical activity of Al with increasing temperature and exposure to static oxygen, which is expected to enable surface segregation of Al, thereby, the formation of Al₂O₃ and improved oxidation resistance. We performed in-depth convex hull analysis of ternary Ti-Al-C, Ti-Ga-C, and Ti-Al-Ga-C based MAX phase, and provide detailed contribution arising from electronic, chemical and vibrational entropies. The thermodynamic analysis shows change in the Gibbs formation enthalpy (ΔG_form) at higher temperatures, which implies an interplay of temperature-dependent enthalpy and entropic contributions in oxidation resistance Ga doped Ti₂AlC MAX phases. A detailed electronic structure and chemical bonding analysis using crystal orbital Hamilton population method reveal the origin of change in phases stability and in oxidation resistance in disorder Ti2(Al_1-xGa_x)C MAX phases. Our electronic structure analysis correlate well with the change in oxidation resistance of Ga doped MAX phases. We believe our study provides a useful guideline to understand to role of alloying on electronic, thermodynamic, and oxidation related mechanisms of bulk MAX phases, which can work as a precursor to understand oxidation behavior of twodimensional MAX phases, i.e., MXenes (transition metal carbides, carbonitrides and nitrides).

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Texas A & M Univ., College Station, TX (United States)

Sponsoring Organization:: National Science Foundation (NSF); Qatar National Research Fund (QNRF); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-07CH11358; AR0001427

OSTI ID:: 1881903

Alternate ID(s):: OSTI ID: 1894255

Report Number(s):: IS-J-10,863

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 12; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (67)

Computational Chemistry of Solid State Materials Dronskowski, Richard https://doi.org/10.1002/9783527612277	book	November 2005
First-Principles Determination of Multicomponent Hydride Phase Diagrams: Application to the Li-Mg-N-H System R. Akbarzadeh, A.; Ozoliņš, V.; Wolverton, C. Advanced Materials, Vol. 19, Issue 20 https://doi.org/10.1002/adma.200700843	journal	September 2007
Interface Atomic-Scale Structure and its Impact on Quantum Electron Transport Wang, Zhongchang; Saito, Mitsuhiro; Tsukimoto, Susumu Advanced Materials, Vol. 21, Issue 48 https://doi.org/10.1002/adma.200900877	journal	September 2009
Analytic projection from plane-wave and PAW wavefunctions and application to chemical-bonding analysis in solids Maintz, Stefan; Deringer, Volker L.; Tchougréeff, Andrei L. Journal of Computational Chemistry, Vol. 34, Issue 29 https://doi.org/10.1002/jcc.23424	journal	September 2013
LOBSTER: A tool to extract chemical bonding from plane-wave based DFT: Tool to Extract Chemical Bonding Maintz, Stefan; Deringer, Volker L.; Tchougréeff, Andrei L. Journal of Computational Chemistry, Vol. 37, Issue 11 https://doi.org/10.1002/jcc.24300	journal	February 2016
The formation of aluminum oxide scales on high-temperature alloys Prescott, R.; Graham, M. J. Oxidation of Metals, Vol. 38, Issue 3-4 https://doi.org/10.1007/BF00666913	journal	October 1992
The Ti-Si-C system (Titanium-Silicon-Carbon) Bandyopadhyay, Debashis Journal of Phase Equilibria and Diffusion, Vol. 25, Issue 5 https://doi.org/10.1007/s11669-004-0132-7	journal	December 2004
The correlation between the electronic structure and elastic properties of nanolaminates Music, Denis; Schneider, Jochen M. JOM, Vol. 59, Issue 7 https://doi.org/10.1007/s11837-007-0091-7	journal	July 2007
Materials Design and Discovery with High-Throughput Density Functional Theory: The Open Quantum Materials Database (OQMD) Saal, James E.; Kirklin, Scott; Aykol, Muratahan JOM, Vol. 65, Issue 11 https://doi.org/10.1007/s11837-013-0755-4	journal	September 2013
The irradiation-induced crystalline-to-amorphous phase transition in α-SiC Weber, W. J.; Wang, L. M.; Yu, N. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 116, Issue 1-4 https://doi.org/10.1016/0168-583X(96)00066-3	journal	August 1996
Strong chemical interactions in disordered alloys Pasturel, A.; Colinet, C.; Hicter, P. Physica B+C, Vol. 132, Issue 2 https://doi.org/10.1016/0378-4363(85)90062-2	journal	July 1985
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
The M_N+1AX_N phases: A new class of solids: Thermodynamically stable nanolaminates Barsoum, Michel W. Progress in Solid State Chemistry, Vol. 28, Issue 1-4, p. 201-281 https://doi.org/10.1016/S0079-6786(00)00006-6	journal	January 2000
Phase stability, electronic structure and mechanical properties of ternary-layered carbide Nb4AlC3: An ab initio study Wang, Jiemin; Wang, Jingyang; Zhou, Yanchun Acta Materialia, Vol. 56, Issue 7 https://doi.org/10.1016/j.actamat.2007.12.003	journal	April 2008
Microstructural evolution during high-temperature oxidation of Ti2AlC ceramics Cui, Bai; Jayaseelan, Daniel Doni; Lee, William Edward Acta Materialia, Vol. 59, Issue 10 https://doi.org/10.1016/j.actamat.2011.03.035	journal	June 2011
The effect of chemical disorder on defect formation and migration in disordered max phases Singh, Prashant; Sauceda, Daniel; Arroyave, Raymundo Acta Materialia, Vol. 184 https://doi.org/10.1016/j.actamat.2019.11.033	journal	February 2020
Metric-driven search for structurally stable inorganic compounds Villarreal, R.; Singh, P.; Arroyave, R. Acta Materialia, Vol. 202 https://doi.org/10.1016/j.actamat.2020.10.055	journal	January 2021
Vacancy formation energies and migration barriers in multi-principal element alloys Roy, Ankit; Singh, Prashant; Balasubramanian, Ganesh Acta Materialia, Vol. 226 https://doi.org/10.1016/j.actamat.2021.117611	journal	March 2022
Anisotropic corrosion of Ti 2 AlC and Ti 3 AlC 2 in supercritical water at 500 ºC Du, Yina; Liu, Ji-Xuan; Gu, Yifeng Ceramics International, Vol. 43, Issue 9 https://doi.org/10.1016/j.ceramint.2017.02.153	journal	June 2017
Mechanical properties and oxidation behavior of Ti-doped Nb4AlC3 Gu, Jian; Pan, Limei; Yang, Jian Journal of the European Ceramic Society, Vol. 36, Issue 4 https://doi.org/10.1016/j.jeurceramsoc.2015.10.023	journal	March 2016
Bonding and oxidation protection of Ti2AlC and Cr2AlC for a Ni-based superalloy Sokol, Maxim; Yang, Jian; Keshavan, Hrishikesh Journal of the European Ceramic Society, Vol. 39, Issue 4 https://doi.org/10.1016/j.jeurceramsoc.2018.10.019	journal	April 2019
Mechanical and oxidation behavior of textured Ti2AlC and Ti3AlC2 MAX phase materials Li, Xiaoqiang; Xie, Xi; Gonzalez-Julian, Jesus Journal of the European Ceramic Society, Vol. 40, Issue 15 https://doi.org/10.1016/j.jeurceramsoc.2020.07.043	journal	December 2020
Structural changes induced by heavy ion irradiation in titanium silicon carbide Nappé, J. C.; Monnet, I.; Grosseau, Ph. Journal of Nuclear Materials, Vol. 409, Issue 1 https://doi.org/10.1016/j.jnucmat.2010.12.235	journal	February 2011
Phase stability and physical properties of (Zr1-Nb )2AlC MAX phases Hadi, M. A.; Monira, U.; Chroneos, A. Journal of Physics and Chemistry of Solids, Vol. 132 https://doi.org/10.1016/j.jpcs.2019.04.010	journal	September 2019
Insights into the physical properties of a new 211 MAX phase Nb2CuC Hadi, M. A.; Kelaidis, N.; Naqib, S. H. Journal of Physics and Chemistry of Solids, Vol. 149 https://doi.org/10.1016/j.jpcs.2020.109759	journal	February 2021
First-principles study of Hf/Nb/Zr-doped MAX phases Ti3AlC2 and Ti3SiC2 Nie, Jinlan; Liu, Sishuo; Zhan, Xiaofei Physica B: Condensed Matter, Vol. 571 https://doi.org/10.1016/j.physb.2019.06.052	journal	October 2019
Ab initio modeling of the formation and migration of monovacancies in Ti2AlC Liao, Ting; Wang, Jingyang; Zhou, Yanchun Scripta Materialia, Vol. 59, Issue 8 https://doi.org/10.1016/j.scriptamat.2008.06.044	journal	October 2008
TEM study of the early stages of Ti2AlC oxidation at 900°C Cui, Bai; Jayaseelan, Daniel Doni; Lee, William Edward Scripta Materialia, Vol. 67, Issue 10 https://doi.org/10.1016/j.scriptamat.2012.07.045	journal	November 2012
Surface energy of M2AC(0001) determined by density functional theory (M=Ti,V,Cr; A=Al,Ga,Ge) Music, D.; Sun, Z.; Ahuja, R. Surface Science, Vol. 601, Issue 4 https://doi.org/10.1016/j.susc.2006.11.025	journal	February 2007
The M_n+1AX_n phases: Materials science and thin-film processing Eklund, Per; Beckers, Manfred; Jansson, Ulf Thin Solid Films, Vol. 518, Issue 8, p. 1851-1878 https://doi.org/10.1016/j.tsf.2009.07.184	journal	February 2010
A GPU-Accelerated Parameter Interpolation Thermodynamic Integration Free Energy Method Giese, Timothy J.; York, Darrin M. Journal of Chemical Theory and Computation, Vol. 14, Issue 3 https://doi.org/10.1021/acs.jctc.7b01175	journal	January 2018
Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations Dronskowski, Richard; Bloechl, Peter E. The Journal of Physical Chemistry, Vol. 97, Issue 33 https://doi.org/10.1021/j100135a014	journal	August 1993
Refractories: Controlled microstructure composites for extreme environments Lee, W. E.; Zhang, S.; Karakus, M. Journal of Materials Science, Vol. 39, Issue 22 https://doi.org/10.1023/B:JMSC.0000045599.84988.9e	journal	November 2004
Coherent displacement of atoms during ion irradiation Nordlund, K.; Keinonen, J.; Ghaly, M. Nature, Vol. 398, Issue 6722 https://doi.org/10.1038/17983	journal	March 1999
Ionization-induced annealing of pre-existing defects in silicon carbide Zhang, Yanwen; Sachan, Ritesh; Pakarinen, Olli H. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9049	journal	August 2015
Influence of chemical disorder on energy dissipation and defect evolution in concentrated solid solution alloys Zhang, Yanwen; Stocks, G. Malcolm; Jin, Ke Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9736	journal	October 2015
Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry Bartel, Christopher J.; Millican, Samantha L.; Deml, Ann M. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06682-4	journal	October 2018
High-throughput reaction engineering to assess the oxidation stability of MAX phases Sauceda, D.; Singh, P.; Falkowski, A. R. npj Computational Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41524-020-00464-7	journal	January 2021
Effects of Al substitution by Si in Ti3AlC2 nanolaminate Hadi, M. A.; Roknuzzaman, Md; Nasir, M. T. Scientific Reports, Vol. 11, Issue 1 https://doi.org/10.1038/s41598-021-81346-w	journal	February 2021
TiO2 nanocluster modified-rutile TiO2 photocatalyst: a first principles investigation Iwaszuk, Anna; Mulheran, P. A.; Nolan, Michael Journal of Materials Chemistry A, Vol. 1, Issue 7 https://doi.org/10.1039/c2ta01582j	journal	January 2013
Prediction study of structural and elastic properties under the pressure effect of M2GaC (M=Ti,V,Nb,Ta) Bouhemadou, A.; Khenata, R. Journal of Applied Physics, Vol. 102, Issue 4 https://doi.org/10.1063/1.2773634	journal	August 2007
Ohmic contact properties of magnetron sputtered Ti3SiC2 on n- and p-type 4H-silicon carbide Buchholt, K.; Ghandi, R.; Domeij, M. Applied Physics Letters, Vol. 98, Issue 4 https://doi.org/10.1063/1.3549198	journal	January 2011
Ab-initio aprroach to the electronic, structural, elastic, and finite-temperature thermodynamic properties of Ti ₂ AX (A = Al or Ga and X = C or N) Duong, Thien; Gibbons, Sean; Kinra, Rajeev Journal of Applied Physics, Vol. 110, Issue 9 https://doi.org/10.1063/1.3652768	journal	November 2011
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
A Critical Review of the Oxidation of Ti ₂ AlC, Ti ₃ AlC ₂ and Cr ₂ AlC in Air Tallman, Darin J.; Anasori, Babak; Barsoum, Michel W. Materials Research Letters, Vol. 1, Issue 3 https://doi.org/10.1080/21663831.2013.806364	journal	September 2013
Does aluminum play well with others? Intrinsic Al-A alloying behavior in 211/312 MAX phases Arróyave, R.; Talapatra, A.; Duong, T. Materials Research Letters, Vol. 5, Issue 3 https://doi.org/10.1080/21663831.2016.1241319	journal	October 2016
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Theory of bonding of transition metals to nontransition metals Gelatt, C. D.; Williams, A. R.; Moruzzi, V. L. Physical Review B, Vol. 27, Issue 4 https://doi.org/10.1103/PhysRevB.27.2005	journal	February 1983
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Electronic structures of and composition gaps among the ternary carbides Ti 2 M C Hug, G. Physical Review B, Vol. 74, Issue 18 https://doi.org/10.1103/PhysRevB.74.184113	journal	November 2006
Electronic structure and optical conductivities of 20 MAX-phase compounds Mo, Yuxiang; Rulis, Paul; Ching, W. Y. Physical Review B, Vol. 86, Issue 16 https://doi.org/10.1103/PhysRevB.86.165122	journal	October 2012
Accurate determination of band gaps within density functional formalism Singh, Prashant; Harbola, Manoj K.; Sanyal, Biplab Physical Review B, Vol. 87, Issue 23 https://doi.org/10.1103/PhysRevB.87.235110	journal	June 2013
Better band gaps with asymptotically corrected local exchange potentials Singh, Prashant; Harbola, Manoj K.; Hemanadhan, M. Physical Review B, Vol. 93, Issue 8 https://doi.org/10.1103/PhysRevB.93.085204	journal	February 2016
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Ta-Nb-Mo-W refractory high-entropy alloys: Anomalous ordering behavior and its intriguing electronic origin Singh, Prashant; Smirnov, A. V.; Johnson, Duane D. Physical Review Materials, Vol. 2, Issue 5 https://doi.org/10.1103/PhysRevMaterials.2.055004	journal	May 2018
SISSO: A compressed-sensing method for identifying the best low-dimensional descriptor in an immensity of offered candidates Ouyang, Runhai; Curtarolo, Stefano; Ahmetcik, Emre Physical Review Materials, Vol. 2, Issue 8 https://doi.org/10.1103/PhysRevMaterials.2.083802	journal	August 2018
Thermodynamic Assessment of the Gallium-Oxygen System Zinkevich, Matvei; Aldinger, Fritz Journal of the American Ceramic Society, Vol. 87, Issue 4 https://doi.org/10.1111/j.1551-2916.2004.00683.x	journal	April 2004
Preparation of Tl2Ba2Ca1 − y CeyCu2O8 − x/2Fx Ce-and F-substituted superconductors Akimov, A. I.; Tkachenko, T. M.; Lebedev, S. A. Inorganic Materials, Vol. 42, Issue 3 https://doi.org/10.1134/S0020168506030204	journal	March 2006
Elastic and Mechanical Properties of the MAX Phases Barsoum, Michel W.; Radovic, Miladin Annual Review of Materials Research, Vol. 41, Issue 1 https://doi.org/10.1146/annurev-matsci-062910-100448	journal	August 2011
Recent Progress in Theoretical Prediction, Preparation, and Characterization of Layered Ternary Transition-Metal Carbides Wang, Jingyang; Zhou, Yanchun Annual Review of Materials Research, Vol. 39, Issue 1 https://doi.org/10.1146/annurev-matsci-082908-145340	journal	August 2009
Long Time Oxidation Study of Ti[sub 3]SiC[sub 2], Ti[sub 3]SiC[sub 2]/SiC, and Ti[sub 3]SiC[sub 2]/TiC Composites in Air Barsoum, M. W.; Ho-Duc, L. H.; Radovic, M. Journal of The Electrochemical Society, Vol. 150, Issue 4 https://doi.org/10.1149/1.1556035	journal	January 2003
Long-Term Oxidation of Ti ₂ AlC in Air and Water Vapor at 1000–1300°C Temperature Range Basu, S.; Obando, N.; Gowdy, A. Journal of The Electrochemical Society, Vol. 159, Issue 2 https://doi.org/10.1149/2.052202jes	journal	January 2011
Solids and Surfaces: A Chemist's View of Bonding in Extended Structures Hoffman, Roald https://doi.org/10.21236/ADA196638	report	July 1988
Does aluminum play well with others? Intrinsic Al-A alloying behavior in 211/312 MAX phases Arróyave, R.; Talapatra, A.; Duong, T. Taylor & Francis https://doi.org/10.6084/m9.figshare.4004724.v1	dataset	January 2016

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A theoretical investigation of the effect of Ga alloying on thermodynamic stability, electronic-structure, and oxidation resistance of Ti2AlC MAX phase

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A theoretical investigation of the effect of Ga alloying on thermodynamic stability, electronic-structure, and oxidation resistance of Ti₂AlC MAX phase