Theoretical Investigation of W(CO)6 and CO Selenization Process

Yıl 2022, , 283 - 291, 30.04.2022

Nadire Nayir

https://doi.org/10.16984/saufenbilder.1038357

Cited By: 2

Öz

Detailed atomic-level insight into the mechanism of W(CO)6 and CO selenization is essential for the fabrication of cheap and environmentally benign transition metal chalcogenides such as MoS2 and WSe2. Earlier discussions in literature have focused mainly on the CO methanation by sulfur and its derivatives but H2Se mediated CO methanation at the atomic level is yet to be explored. First-principles calculations and ReaxFF-based molecular dynamics simulations are conducted here to explore the relative stabilities of intermediates formed during the gas-phase interactions of W(CO)6 and H2Se, determined associated reaction energies and kinetic barriers. The methanation of CO, which is released from the organometal, by H2Se is further investigated. The results indicate that the chain reactions of W(CO)6 and H2Se lead to the formation of a thermodynamically stable end product of W(SeH)2Se2. Depending on the temperature, W(HSe)2Se2 is expected to go through a last uphill reaction by releasing H2Se into the environment and evolving into a WSe3 molecule. Additionally, the dehydrogenation of organometallic molecules is thermodynamically feasible but kinetically controlled, requiring a significant activation energy. When all CO groups are released from the W atom, the H2 release from W-compund becomes nearly barrierless. Since CO radical groups are dominant byproducts formed during the MOCVD chain reactions but in a chalcogen rich environment, this work also shed light into the CO selenization during the growth of transition metal diselenides (e.g., WSe2, MoSe2, CrSe2) and discusses the formation of potential products such as CSe2, CH4, H2Se, CO, H2O, Se2.

Anahtar Kelimeler

Density functional theory, ReaxFF molecular dynamics, W(CO)6 and H2Se interactions, CO methanation.

Destekleyen Kurum

Karamanoğlu Mehmetbey University and the National Science Foundation (NSF) through the Pennsylvania State University 2D Crystal Consortium−Materials Innovation Platform (2DCC-MIP)

Proje Numarası

The NSF cooperative agreement DMR-1539916

Teşekkür

The author also thanks Prof. Adri van Duin for the fruitful discussions

Kaynakça

• [1] A. Eftekhari, “Tungsten Dichalcogenides (WS2, WSe2, and WTe2): Materials Chemistry and Applications,” J. Mater. Chem. A, vol. 5, no. 35, pp. 18299–18325, 2017.
• [2] T.H. Choudhury, X. Zhang, Z.Y.A. Balushi, M. Chubarov, J.M. Redwing, “Epitaxial Growth of 2D Layered Transition Metal Dichalcogenides,” ArXiv190903502 Cond-Mat 2019. [3] H. Qin, Q.-X. Pei, Y. Liu, Y.-W. Zhang, “The Mechanical and Thermal Properties of MoS2–WSe2 Lateral Heterostructures,” Phys. Chem. Chem. Phys., vol. 21, no. 28, pp. 15845–15853, 2019.
• [4] W. Choi, N. Choudhary, G.H. Han, J. Park, D. Akinwande, Y.H. Lee, “Recent Development of Two-Dimensional Transition Metal Dichalcogenides and Their Applications,” Mater. Today, vol. 20, no. 3, 116–130, 2017.
• [5] D. Andrzejewski, H. Myja, M. Heuken, A. Grundmann, H. Kalisch, A. Vescan, T. Kümmell, G. Bacher, “Scalable Large-Area p–i–n Light-Emitting Diodes Based on WS2 Monolayers Grown via MOCVD,” ACS Photonics, vol. 6, no. 8, pp. 1832–1839, 2019.
• [6] X. Zhang, F. Zhang, Y. Wang, D.S. Schulman, T. Zhang, A. Bansal, N. Alem, S. Das, V.H. Crespi, M. Terrones, J.M. Redwing, “Defect-Controlled Nucleation and Orientation of WSe2 on HBN: A Route to Single-Crystal Epitaxial Monolayers,” ACS Nano, vol. 13, no. 3, pp. 3341–3352, 2019.
• [7] B.D. Keller, A. Bertuch, J. Provine, G. Sundaram, N. Ferralis, J.C. Grossman, “Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS2 Monolayers,” Chem. Mater., vol. 29, no. 5, pp. 2024–2032, 2017.
• [8] W. Hao, C. Marichy, C. Journet, “Atomic Layer Deposition of Stable 2D Materials,” 2D Mater., vol. 6, no. 1, 012001, 2018.
• [9] G.-H. Park, K. Nielsch, A. Thomas, “Atomic Layer Deposition: 2D Transition Metal Dichalcogenide Thin Films Obtained by Chemical Gas Phase Deposition Techniques (Adv. Mater. Interfaces 3/2019),” Adv. Mater. Interfaces, vol. 6, no. 3, 1970024, 2019.
• [10] X. Zhang, Z.Y. Al Balushi, F. Zhang, T.H. Choudhury, S.M. Eichfeld, N. Alem, T.N. Jackson, J.A. Robinson, J.M. Redwing, “Influence of Carbon in Metalorganic Chemical Vapor Deposition of Few-Layer WSe2 Thin Films,” J. Electron. Mater., vol. 45, no. 12, pp. 6273–6279, 2016. [11] T.H. Choudhury, H. Simchi, R. Boichot, M. Chubarov, S.E. Mohney, J.M. Redwing, “Chalcogen Precursor Effect on Cold-Wall Gas-Source Chemical Vapor Deposition Growth of WS2,” Cryst. Growth Des., vol. 18, no. 8, pp. 4357–4364, 2018.
• [12] Y. Gong, X. Zhang, J.M. Redwing, T.N. Jackson, “Thin Film Transistors Using Wafer-Scale Low-Temperature MOCVD WSe2,” J. Electron. Mater., vol. 45, no. 12, pp. 6280–6284, 2016.
• [13] L. Jiao, H.J. Liu, J.L. Chen, Y. Yi, W.G. Chen, Y. Cai, J.N. Wang, X.Q. Dai, N. Wang, W.K. Ho, M.H. Xie, “Molecular-Beam Epitaxy of Monolayer MoSe2: Growth Characteristics and Domain Boundary Formation,” New J. Phys., vol. 17, no. 5, 053023, 2015.
• [14] Y. Zhang, T.-R. Chang, B. Zhou, Y.-T. Cui, H. Yan, Z. Liu, F. Schmitt, J. Lee, R. Moore, Y. Chen, H. Lin, H.-T. Jeng, S.-K. Mo, Z. Hussain, A. Bansil, Z.-X. Shen, “Direct Observation of the Transition from Indirect to Direct Bandgap in Atomically Thin Epitaxial MoSe2,” Nat. Nanotechnol., vol. 9, no. 2, pp. 111–115, 2014.
• [15] H.J. Liu, L. Jiao, L. Xie, F. Yang, J.L. Chen, W.K. Ho, C.L. Gao, J.F. Jia, X.D. Cui, M.H. Xie, “Molecular-Beam Epitaxy of Monolayer and Bilayer WSe2: A Scanning Tunneling Microscopy/Spectroscopy Study and Deduction of Exciton Binding Energy,” 2D Mater., vol. 2, no. 3, 034004, 2015.
• [16] M. Nakano, Y. Wang, Y. Kashiwabara, H. Matsuoka, Y. Iwasa, “Layer-by-Layer Epitaxial Growth of Scalable WSe2 on Sapphire by Molecular Beam Epitaxy,” Nano Lett., vol. 17, no. 9, pp. 5595–5599, 2017.
• [17] Y. Xuan, A. Jain, S. Zafar, R. Lotfi, N. Nayir, Y. Wang, T.H. Choudhury, S. Wright, J. Feraca, L. Rosenbaum, JM Redwing, V. Crespi, A.C.T. van Duin, “Multi-Scale Modeling of Gas-Phase Reactions in Metal-Organic Chemical Vapor Deposition Growth of WSe2,” J. Cryst. Growth, vol. 527, 125247, 2019.
• [18] A.D. Bochevarov, E. Harder, T.F. Hughes, J.R. Greenwood, D.A. Braden, D.M. Philipp, D. Rinaldo, M.D. Halls, J. Zhang, R.A. Friesner, “Jaguar: A High-Performance Quantum Chemistry Software Program with Strengths in Life and Materials Sciences,” Int. J. Quantum Chem., vol. 113, no. 18, pp. 2110–2142, 2013.
• [19] Amsterdam Modeling Suite Making Computational Chemistry Work For You https://www.scm.com/ (accessed 2020 -11 -10).
• [20] K. Chenoweth, A.C.T. van Duin, W.A. Goddard, “ReaxFF Reactive Force Field for Molecular Dynamics Simulations of Hydrocarbon Oxidation,” J. Phys. Chem. A, vol. 112, no. 5, pp. 1040–1053, 2008.
• [21] K. Momma, F. Izumi, “VESTA 3 for Three-Dimensional Visualization of Crystal, Volumetric and Morphology Data,” J. Appl. Crystallogr., vol. 44, no. 6, pp. 1272–1276, 2011.
• [22] S.M. Eichfeld, L. Hossain, Y.-C. Lin, A.F. Piasecki, B. Kupp, A.G. Birdwell, R.A. Burke, N. Lu, X. Peng, J. Li, A. Azcatl, S. McDonnell, R.M. Wallace, M.J. Kim, T.S. Mayer, J.M. Redwing, J.A. Robinson, “Highly Scalable, Atomically Thin WSe2 Grown via Metal–Organic Chemical Vapor Deposition,” ACS Nano, vol. 9, no. 2, pp. 2080–2087, 2015.
• [23] K.L. Joshi, S. Raman, A.C.T. van Duin, “Connectivity-Based Parallel Replica Dynamics for Chemically Reactive Systems: From Femtoseconds to Microseconds,” J. Phys. Chem. Lett., vol. 4, no. 21, pp. 3792–3797, 2013.
• [24] K.M. Bal, E.C. Neyts, “Merging Metadynamics into Hyperdynamics: Accelerated Molecular Simulations Reaching Time Scales from Microseconds to Seconds,” J. Chem. Theory Comput., vol. 11, no. 10, pp. 4545–4554, 2015.
• [25] K.M. Bal, E.C. Neyts, “Direct Observation of Realistic-Temperature Fuel Combustion Mechanisms in Atomistic Simulations,” Chem. Sci., vol. 7, no. 8, pp. 5280–5286, 2016.