Efficient bi-functional catalysis of coupled MoSe2 nanosheet/Pt nanoparticles for methanol-assisted water splitting

doi:10.1016/S1872-2067(23)64469-9

Abstract

Abstract:

Efficient metal-support interaction induced high catalysis performance plays a significant role in energy conversion reactions. Herein, two-dimensional (2D) MoSe₂ nanosheet-coupled Pt nanoparticles as efficient bi-functional catalysts were demonstrated for hydrogen production from the methanol-assisted water-splitting reaction. The oxophilic MoSe₂ component with 2D structures optimized the adsorption of CO* and H* on Pt sites as demonstrated by spectroscopic and theoretical analysis, which resulted in enhanced catalytic ability in methanol-assisted water splitting reaction. The peak current density was 2.5 times higher than that of commercial Pt/C catalyst for methanol oxidation and a small overpotential of 32 mV was demanded to achieve a current density of 10 mA cm^-2 for hydrogen evolution reaction in the methanol-containing electrolyte. When serviced as both cathode and anode, a low cell voltage of 0.66 V was required at 10 mA cm^-2, significantly lower than that of 1.75 V required for water splitting. The high performance can be attributed to the oxophilicity of MoSe₂ and their strong metal-support interaction that promoted the charge transfer and anti-CO poisoning of Pt sites. This work would be instructive for the development of novel bi-functional catalyst platforms for methanol-assisted water splitting in hydrogen production.

Key words: Molybdenum Selenide, 2D structure, Hydrogen production, Methanol-assisted water splitting, Pt nanoparticles

Wei Qiao, Lice Yu, Jinfa Chang, Fulin Yang, Ligang Feng. Efficient bi-functional catalysis of coupled MoSe₂ nanosheet/Pt nanoparticles for methanol-assisted water splitting[J]. Chinese Journal of Catalysis, 2023, 51: 113-123.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64469-9

https://www.cjcatal.com/EN/Y2023/V51/I8/113

Figures/Tables 6

Fig. 1. SEM image of MoSe2 (a) and Pt/MoSe2 (b). TEM (c,d) and HRTEM (e) images and the corresponding SAED pattern (f), EDS spectra (g), STEM image (h) and corresponding elemental mapping images (i?k) and overlap image (l) of Pt/MoSe2 catalyst.

Fig. 2. (a) XRD patterns of Pt/MoSe2, PtMo/C and Pt/C. (b) Pt 4f XPS spectra of the Pt/MoSe2, PtMo/C and Pt/C. (c) Mo 3d spectra for Pt/MoSe2 and PtMo/C. (d) Se 3d spectrum for Pt/MoSe2.

Fig. 3. (a) CV curves of Pt/MoSe2, PtMo/C, Pt/C and MoSe2 catalysts. (b) The graphical comparison of peak current density after different scan cycles, CA curves (c), CO stripping curves (d), and the graphical comparison of mass and specific activity (e) of Pt/MoSe2, PtMo/C and Pt/C catalysts.

Fig. 4. (a) CV curves of the Pt/MoSe2 catalyst recorded at scan rates of 5 mV to 150 mV s-1. (b) The corresponding plot of different catalysts with forward peak current density as a function of the square root of the scan rate (v1/2). (c) Nyquist plots of different catalysts. (d) The in situ FTIR spectra of Pt/MoSe2.

Fig. 5. (a) LSV polarization curves of Pt/MoSe2, PtMo/C, Pt/C and MoSe2. Tafel plots (b), specific activity (c) and TOF curves (d) of Pt/MoSe2, PtMo/C, Pt/C catalysts. (e) LSV polarization curves before and after 1000 CV cycles of Pt/MoSe2 (inset: CA curve for Pt/MoSe2 in 0.5 mol L?1 H2SO4 + 1.0 mol L?1 CH3OH at an overpotential of 32 mV). (f) LSV polarization curves of the Pt/MoSe2 || Pt/MoSe2 and Pt/C || Pt/C electrodes in 0.5 mol L?1 H2SO4 with and without 1.0 mol L?1 CH3OH (inset: CA curve for Pt/MoSe2 in 0.5 mol L?1 H2SO4 + 1 mol L?1 CH3OH at a potential of 0.66 V).

Fig. 6. (a) The optimized model of Pt/MoSe2. (b) The optimized atomic geometries of the intermediates on Pt/MoSe2 surface. (c) Free energy diagram for MOR on Pt/MoSe2 (red) and Pt (grey) surface. (d) Calculated ECO* on the different sites of different Pt (111) surface of Pt/MoSe2, PtMo and Pt. (e) Electron density difference of Pt/MoSe2 (yellow: electron depletion and blue: electron accumulation). (f) Calculated ΔGH* of Pt/MoSe2, PtMo and Pt/C.

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Efficient bi-functional catalysis of coupled MoSe₂ nanosheet/Pt nanoparticles for methanol-assisted water splitting

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