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Predicted Electrocatalyst Properties on Metal Insulator MoTe2 for Hydrogen Evolution Reaction and Oxygen Reduction Reaction Application in Fuel Cells

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    Fuel Cells

    Predicted Electrocatalyst Properties on Metal Insulator MoTe2 for Hydrogen Evolution Reaction and Oxygen Reduction Reaction Application in Fuel Cells
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    Energy & Fuels

    Cite this: Energy Fuels 2021, 35, 9, 8275–8285
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    https://doi.org/10.1021/acs.energyfuels.1c00814
    Published April 20, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Systematic spin-polarized density functional theory (DFT) calculations were executed to study the catalytic performance of the topological insulator MoTe2 (2H, 1T, and 1T′) phase. Topological insulator materials, including robust surface states and excellent carrier mobility, are suitable for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) catalysts. Topological materials usually have a strong contribution to the density of states close to the Fermi level and high carrier mobility, which is a prerequisite for designing highly efficient catalysts. The binding energy of hydrogen (G*H) is almost zero and is a promising candidate for producing hydrogen from water. A linear scaling relationship was established depending upon the binding strengths of ORR intermediates. The limiting potential diagram could modulate the catalytic efficiency by ΔG*OH between different activity sites on MoTe2, and a volcano plot for the ORR overpotential as a function of ΔG*OH was found. According to our analysis, the best system is 1T′-MoTe2 with a γ site for the ORR and an α′ site for the HER, which are predicted to have an overpotential of 0.20 V for the HER and 0.33 V for the ORR with spin–orbit coupling calculation. HER and ORR occur along the most favorable paths on the same phase MoTe2 but at different sites, which can be considered promising candidates for both ORR and HER. Specifically, spin–orbit coupling in a metal insulator tends to interact with oxygen molecules to contribute to the ORR process, and localized electron spin coupling can guarantee the moderate binding strength of *OH intermediates. This study may provide guidance to explore new and efficient catalysts based on the theory predictions, which has been proven to be feasible for catalyst design.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.energyfuels.1c00814.

    • Gibbs free energy (ΔG) diagrams for all intermediates during the ORR process, with the RDS also highlighted with arrows: (a) 2H-MoTe2@α, (b) 2H-MoTe2@β, (c) 2H-MoTe2@γ, (d) 1T-MoTe2@α, (e) 1T-MoTe2@β, and (f) 1T-MoTe2@γ adsorption sites (Figure S1), Gibbs free energy (ΔG) diagrams for all intermediates during the ORR process, with the RDS also highlighted with arrows: (a) 1T′-MoTe2@α, (b) 1T′-MoTe2@β, (c) 1T′-MoTe2@γ, (d) 1T′-MoTe2@α′, (e) 1T′-MoTe2@β′, and (f) 1T′-MoTe2@γ′ adsorption sites (Figure S2), linear relationships of intermediate species between binding energies without SOC: (a) ΔG*OH versus ΔG*OOH and (b) ΔG*OOH versus ΔG*O and ΔG*OH versus ΔG*O (Figure S3), Gibbs free energy diagrams without SOC calculations for the ORR on metal insulator monolayer MoTe2 catalysts under an applied potential, with the reduction potential for ΔGmax and equilibrium potential (U = 1.23 V) in acidic conditions (pH 0): (a) 2H-MoTe2@α, (b) 2H-MoTe2@β, (c) 2H-MoTe2@γ, (d) 1T-MoTe2@α, (e) 1T-MoTe2@β, (f) 1T-MoTe2@γ, (g) 1T′-MoTe2@α, (h) 1T′-MoTe2@β and 1T′-MoTe2@γ, (i) 1T″-MoTe2@α′, (j) 1T″-MoTe2@β′, (k) 1T″-MoTe2@γ′, (l) 1T′-MoTe2@β′ (Figure S4), volcano plot of overpotential for the (a) ORR and (b) OER, with the binding energies obtained without SOC (Figure S5), (a) activity selectivity between HER and ORR for each active site and (b) overpotential on the different adsorption sites of HER, with all of the binding energies without SOC calculations (Figure S6), activity prediction of the thermodynamical limiting potential for oxygen reduction to H2O using ΔG*OH, without SOC calculations, which can be obtained from the negative of the change in free energy (−ΔG) for the different reaction steps at the equilibrium potential (U = 1.23) as a function of ΔG*OH, which is usually a descriptor of the catalytic efficiency for 4e– ORR (Figure S7), linear correlation of the calculated ORR overpotentials without SOC calculations and comparison of the SHE versus ΔG*OH on different adsorption sites for various MoTe2 phases (Figure S8), electronic band structure for the metal insulator MoTe2 phase of (a and b) bulk surface and O2 adsorption configuration phase, (c and d) bulk surface and O2 adsorption configuration of the 2H-MoTe2 phase with SOC hybrid PBE functional calculations, (e and f) bulk surface and O2 adsorbed configuration phase, and (g and h) bulk surface and O2 adsorption configuration of the 1T-MoTe2 phase with SOC hybrid PBE functional calculations, with the Fermi level set to zero (Figures S9 and S10), Gibbs free energies at 298.15 K corresponding to the each species along the O2 conversion into water catalyzed by the MoTe2 different phase surfaces (Table S1), binding energy values of adsorbates for both HER and ORR on each adsorption site for the three different phase MoTe2 structures without and with SOC (Table S2), limiting potentials for the ORR and HER and UL(O2)–UL(H2) for the as-selected adsorption site on different MoTe2 phases and binding energy values of adsorbates for both *H and *O2 on each adsorption site for the three different phase MoTe2 structures without and with SOC (Table S3), Gibbs free energy profile, limiting potentials, and overpotential of each elementary reaction step for the ORR with and without SOC calculation (Table S4), and calculated band gap and SOC (ΔSOC) of the valence band maximum at K points for monolayer 2H-MoTe2 and 1T-MoTe2 for between K and Γ points with PBE without and with SOC (Table S5) (PDF)

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    Energy & Fuels

    Cite this: Energy Fuels 2021, 35, 9, 8275–8285
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.energyfuels.1c00814
    Published April 20, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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