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High-Density Formation of Ir/MoO_x Interface through Hybrid Clustering for Chemoselective Nitrostyrene Hydrogenation.

ABSTRACT: To form high-density metal/oxide interfacial active sites, we developed a catalyst preparation method based on hybrid clustering. An iridium-molybdenum (Ir-Mo) hybrid clustering catalyst was prepared by using the hybrid cluster [(IrCp*)₄Mo₄O₁₆] (Cp* = η⁵-C₅Me₅) as the precursor. The Ir-Mo hybrid clustering catalyst selectively reduced the nitro group in the hydrogenation of 4-nitrostyrene, whereas the coimpregnated Ir-Mo catalyst reduced both the nitro and vinyl groups nonselectively. The hybrid clustering catalyst also exhibited high selectivity, even at a high Ir loading (5 wt %), in contrast to Ir/MoO₃, which exhibited high selectivity only at low Ir loadings (<0.3 wt %). In situ X-ray absorption spectroscopy analysis revealed that oxygen vacancies were formed at the Ir/MoO_x interface in the presence of H₂. We concluded that a high-density Ir/MoO_x interface contributes to the preferential adsorption of nitro groups on vacant sites, promoting the selective hydrogenation of nitro groups.

SUBMITTER: Hayashi S

PROVIDER: S-EPMC10557123 | biostudies-literature | 2023 Oct

REPOSITORIES: biostudies-literature

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High-Density Formation of Ir/MoOx Interface through Hybrid Clustering for Chemoselective Nitrostyrene Hydrogenation.

Hayashi Shun S Shishido Tetsuya T

ACS organic & inorganic Au 20230713 5

To form high-density metal/oxide interfacial active sites, we developed a catalyst preparation method based on hybrid clustering. An iridium-molybdenum (Ir-Mo) hybrid clustering catalyst was prepared by using the hybrid cluster [(IrCp*)4Mo4O16] (Cp* = η5-C5Me5) as the precursor. The Ir-Mo hybrid clustering catalyst selectively reduced the nitro group in the hydrogenation of 4-nitrostyrene, whereas the coimpregnated Ir-Mo catalyst ...[more]

PMID: 37810415

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Project description:Efficient and cost-effective electrocatalysts for the hydrogen oxidation/evolution reaction (HOR/HER) are essential for commercializing alkaline fuel cells and electrolyzers. The sluggish HER/HOR reaction kinetics in base is the key issue that requires resolution so that commercialization may proceed. It is also quite challenging to decrease the noble metal loading without sacrificing performance. Herein, we report improved HER/HOR activity as a result of hydrogen spillover on platinum-supported MoO3 (Pt/MoO3-CNx-400) with a Pt loading of 20%. The catalyst exhibited a decreased over-potential of 66.8 mV to reach 10 mA cm-2 current density with a Tafel slope of 41.2 mV dec-1 for the HER in base. The Pt/MoO3-CNx-400 also exhibited satisfactory HOR activity in base. The mass-specific exchange current density of Pt/MoO3-CNx-400 and commercial Pt/C are 505.7 and 245 mA mgPt-1, respectively. The experimental results suggest that the hydrogen binding energy (HBE) is the key descriptor for the HER/HOR. We also demonstrated that the enhanced HER/HOR performance was due to the hydrogen spillover from Pt to MoO3 sites that enhanced the Volmer/Heyrovsky process, which led to high HER/HOR activity and was supported by the experimental and theoretical investigations. The work function value of Pt [Φ = 5.39 eV) is less than that of β-MoO3 (011) [Φ = 7.09 eV], which revealed the charge transfer from Pt to the β-MoO3 (011) surface. This suggested the feasibility of hydrogen spillover, and was further confirmed by the relative hydrogen adsorption energy [ΔGH] at different sites. Based on these findings, we propose that the H2O or H2 dissociation takes place on Pt and interfaces to form Pt-Had or (Pt/MoO3)-Had, and some of the Had shifted to MoO3 sites through hydrogen spillover. Then, Had at the Pt and interface, and MoO3 sites reacted with H2O and HO- to form H2 or H2O molecules, thereby boosting the HER/HOR activity. This work may provide valuable information for the development of hydrogen-spillover-based electrocatalysts for use in various renewable energy devices.

Dataset Information

High-Density Formation of Ir/MoO_x Interface through Hybrid Clustering for Chemoselective Nitrostyrene Hydrogenation.

Publications

High-Density Formation of Ir/MoO<sub><i>x</i></sub> Interface through Hybrid Clustering for Chemoselective Nitrostyrene Hydrogenation.

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