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ReaxFF force field development and application for toluene adsorption on MnMOx (M=Cu, Fe, Ni) catalysts

In numerous studies the application of the molecular dynamics scheme based on reactive force field (ReaxFF) method has been proven effective in modeling catalytic behavior of metallic- organic compounds [1]. Recently, the method has been successfully applied for MOx (M=Cu, Fe, Mn, Ni) transition-metal oxides [2]. Yet, the problem arose during this analysis, since not all the force field parameters were available at the time. To bridge this gap, the force field for modeling mixed metal oxides had to be developed. For Mn-Fe bond, this was done within the work presented in a recent conference [3]. Here we establish the remaining two needed force field parameter sets (namely, Cu-Mn and Ni-Mn) and apply them to the problem of toluene adsorption on such catalyst mixed metal-oxide surfaces in order to verify their validity. The training set consisted of at least 10 crystal structures containing at minimum Ni-Mn-O or Cu-Mn-O atoms obtained from the Material project database [4]. The parameter training has been done using the in-home compiled version of the ReaxFF code. After training the force fields for geometry reproduction, the parameters were refined using the optimization by atom charges, comparing the ReaxFF values to those obtained for the respective structures using periodic crystal DFT codes implemented in Quantum Espresso [5] and Abinit [6]. [1] T. P. Senftle et al, npj Comput Mater, 2 15011 (2016). [2] M. Duplančić, V. Gomzi, A. Pintar, S. Kurajica, V. Tomašić, Ceramics Int. 47(3), 3108- 3121 (2021). [3] V. Gomzi, M. Duplančić, V. Tomašić Reactive force field optimization and MnFeO3 catalyst theoretical investigation, 18th Ruzicka Days, September 16–18, 2020 / Vukovar, Croatia. [4] (a) A. Jain, S.P. Ong et al, APL Materials, 1(1), 011002 (2013). (b) S. P. Ong et al, Comp. Mat. Sci., 68, 314–319 (2013). [5] (a) P. Giannozzi et. al., J.Phys.:Condens.Matter 21, 395502 (2009) (b) P Giannozzi et al, J.Phys.:Condens.Matter 29, 465901 (2017) (c) P. Giannozzi et al, J. Chem. Phys. 152, 154105 (2020). [6] X. Gonze et al, Comput. Phys. Commun. 248, 107042 (2020).

molecular dynamics, reactive force field, metal-oxide catalyst

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