Performance of Metal-Catalyzed Hydrodebromination of Dibromomethane Analyzed by Descriptors Derived from Statistical Learning

Performance of Metal-Catalyzed Hydrodebromination of Dibromomethane Analyzed by Descriptors Derived from Statistical Learning

The catalyzed semihydrogenation of dibromomethane (CH2Br2) to methyl bromide (CH3Br) is a key step in the bromine-mediated upgradation of methane. This study presents a cutting-edge strategy combining density functional theory (DFT), catalytic tests complemented with the extensive characterization o...

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Hauptverfasser: Saadun, A. J, Pablo-García, S, Paunović, V, Li, Q, Sabadell-Rendón, A, Kleemann, K, Krumeich, F, López, N, Pérez-Ramírez, J
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creator Saadun, A. J
Pablo-García, S
Paunović, V
Li, Q
Sabadell-Rendón, A
Kleemann, K
Krumeich, F
López, N
Pérez-Ramírez, J
description The catalyzed semihydrogenation of dibromomethane (CH2Br2) to methyl bromide (CH3Br) is a key step in the bromine-mediated upgradation of methane. This study presents a cutting-edge strategy combining density functional theory (DFT), catalytic tests complemented with the extensive characterization of a wide range of metal catalysts (Fe, Co, Ni, Cu, Ru, Rh, Ag, Ir, and Pt), and statistical tools for a computer-assisted investigation of this reaction. The steady-state catalytic tests identified four classes of materials comprising (i) poorly active (
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J ; Pablo-García, S ; Paunović, V ; Li, Q ; Sabadell-Rendón, A ; Kleemann, K ; Krumeich, F ; López, N ; Pérez-Ramírez, J</creator><creatorcontrib>Saadun, A. J ; Pablo-García, S ; Paunović, V ; Li, Q ; Sabadell-Rendón, A ; Kleemann, K ; Krumeich, F ; López, N ; Pérez-Ramírez, J</creatorcontrib><description>The catalyzed semihydrogenation of dibromomethane (CH2Br2) to methyl bromide (CH3Br) is a key step in the bromine-mediated upgradation of methane. This study presents a cutting-edge strategy combining density functional theory (DFT), catalytic tests complemented with the extensive characterization of a wide range of metal catalysts (Fe, Co, Ni, Cu, Ru, Rh, Ag, Ir, and Pt), and statistical tools for a computer-assisted investigation of this reaction. The steady-state catalytic tests identified four classes of materials comprising (i) poorly active (&lt;8%) Fe/SiO2, Co/SiO2, Cu/SiO2, and Ag/SiO2; (ii) Rh/SiO2 and Ni/SiO2, which exhibit intermediate CH3Br selectivity (&lt;60%); (iii) Ir/SiO2 and Pt/SiO2, which display great propensity to CH4 (&gt;50%); and (iv) Ru/SiO2, which exhibits the highest selectivity to CH3Br (up to 96%). In-depth characterization of representative catalysts in fresh and used forms was done by X-ray diffraction, inductively coupled plasma optical emission spectroscopy, N2 sorption, temperature-programmed reduction, Raman spectroscopy, electron microscopy, and X-ray photoelectron spectroscopy. The dimensionality reduction performed on the 272 DFT intermediate adsorption energies using principal component analysis identified two descriptors that, when employed together with the experimental data in a random forest regressor, enabled the understanding of activity and selectivity trends by connecting them to the energy intervals of the descriptors. In addition, a representative analytic model was found using the Bayesian inference. 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The steady-state catalytic tests identified four classes of materials comprising (i) poorly active (&lt;8%) Fe/SiO2, Co/SiO2, Cu/SiO2, and Ag/SiO2; (ii) Rh/SiO2 and Ni/SiO2, which exhibit intermediate CH3Br selectivity (&lt;60%); (iii) Ir/SiO2 and Pt/SiO2, which display great propensity to CH4 (&gt;50%); and (iv) Ru/SiO2, which exhibits the highest selectivity to CH3Br (up to 96%). In-depth characterization of representative catalysts in fresh and used forms was done by X-ray diffraction, inductively coupled plasma optical emission spectroscopy, N2 sorption, temperature-programmed reduction, Raman spectroscopy, electron microscopy, and X-ray photoelectron spectroscopy. The dimensionality reduction performed on the 272 DFT intermediate adsorption energies using principal component analysis identified two descriptors that, when employed together with the experimental data in a random forest regressor, enabled the understanding of activity and selectivity trends by connecting them to the energy intervals of the descriptors. In addition, a representative analytic model was found using the Bayesian inference. 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The steady-state catalytic tests identified four classes of materials comprising (i) poorly active (&lt;8%) Fe/SiO2, Co/SiO2, Cu/SiO2, and Ag/SiO2; (ii) Rh/SiO2 and Ni/SiO2, which exhibit intermediate CH3Br selectivity (&lt;60%); (iii) Ir/SiO2 and Pt/SiO2, which display great propensity to CH4 (&gt;50%); and (iv) Ru/SiO2, which exhibits the highest selectivity to CH3Br (up to 96%). In-depth characterization of representative catalysts in fresh and used forms was done by X-ray diffraction, inductively coupled plasma optical emission spectroscopy, N2 sorption, temperature-programmed reduction, Raman spectroscopy, electron microscopy, and X-ray photoelectron spectroscopy. 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title Performance of Metal-Catalyzed Hydrodebromination of Dibromomethane Analyzed by Descriptors Derived from Statistical Learning
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