Regulating Ru<sub><i>x</i></sub>Mo<sub><i>y</i></sub> Nanoalloys Anchored on Porous Nitrogen-Doped Carbon\nvia Domain-Confined Etching Strategy for Neutral Efficient Ammonia\nElectrosynthesis

Neutral\nelectrochemical nitrate (NO<sub>3</sub><sup>–</sup>) reduction\nto ammonia involves sluggish and complex kinetics, so\ndeveloping efficient electrocatalysts at low potential remains challenging.\nHere, we report a domain-confined etching strategy to construct Ru<sub><i>x</i></sub>Mo<sub><i>y</i></sub> nanoalloys\non porous nitrogen-doped carbon by optimizing the Ru-to-Mo ratio,\nachieving efficient neutral NH<sub>3</sub> electrosynthesis. Combining <i>in situ</i> spectroscopy and theoretical simulations demonstrated\na rational synergic effect between Ru and Mo in nanoalloys that reinforces\n*H adsorption and lowers the energy barrier of NO<sub>3</sub><sup>–</sup> hydrodeoxygenation for NH<sub>3</sub> production.\nThe resultant Ru<sub>5</sub>Mo<sub>5</sub>-NC surpasses 92.8% for\nNH<sub>3</sub> selectivity at the potential range from −0.25\nto −0.45 V vs RHE under neutral electrolyte, particularly achieving\na high NH<sub>3</sub> selectivity of 98.3% and a corresponding yield\nrate of 1.3 mg h<sup>–1</sup> mg<sub>cat</sub><sup>–1</sup> at −0.4 V vs RHE. This work provides a synergic strategy\nthat sheds light on a new avenue for developing efficient multicomponent\nheterogeneous catalysts.

Publication Details

Journal
Figshare
Published
2024-09-12
DOI
https://doi.org/10.1021/acs.nanolett.4c03319.s001
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
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Regulating RuxMoy Nanoalloys Anchored on Porous Nitrogen-Doped Carbon\nvia Domain-Confined Etching Strategy for Neutral Efficient Ammonia\nElectrosynthesis

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Ammonia Synthesis and Nitrogen Reduction
article

Regulating RuxMoy Nanoalloys Anchored on Porous Nitrogen-Doped Carbon\nvia Domain-Confined Etching Strategy for Neutral Efficient Ammonia\nElectrosynthesis

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Abstract

Neutral\nelectrochemical nitrate (NO<sub>3</sub><sup>–</sup>) reduction\nto ammonia involves sluggish and complex kinetics, so\ndeveloping efficient electrocatalysts at low potential remains challenging.\nHere, we report a domain-confined etching strategy to construct Ru<sub><i>x</i></sub>Mo<sub><i>y</i></sub> nanoalloys\non porous nitrogen-doped carbon by optimizing the Ru-to-Mo ratio,\nachieving efficient neutral NH<sub>3</sub> electrosynthesis. Combining <i>in situ</i> spectroscopy and theoretical simulations demonstrated\na rational synergic effect between Ru and Mo in nanoalloys that reinforces\n*H adsorption and lowers the energy barrier of NO<sub>3</sub><sup>–</sup> hydrodeoxygenation for NH<sub>3</sub> production.\nThe resultant Ru<sub>5</sub>Mo<sub>5</sub>-NC surpasses 92.8% for\nNH<sub>3</sub> selectivity at the potential range from −0.25\nto −0.45 V vs RHE under neutral electrolyte, particularly achieving\na high NH<sub>3</sub> selectivity of 98.3% and a corresponding yield\nrate of 1.3 mg h<sup>–1</sup> mg<sub>cat</sub><sup>–1</sup> at −0.4 V vs RHE. This work provides a synergic strategy\nthat sheds light on a new avenue for developing efficient multicomponent\nheterogeneous catalysts.

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Ammonia Synthesis and Nitrogen Reduction
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