Interfacial Engineering of Mo<sub>x</sub>S<sub>y</sub> via Boron-Doping for Electrochemical N<sub>2</sub>-to-NH<sub>3</sub> Conversion.
basic_science · Level V
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- Record sourced from PubMed, PMID 39494957.
- Also identified by DOI 10.1002/adma.202405578.
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Abstract
The electrocatalytic synthesis of ammonia (NH<sub>3</sub>) through the nitrogen reduction reaction (NRR) under ambient temperature and pressure is emerging as an alternative approach to the conventional Haber-Bosch process. However, it remains a significant challenge due to poor kinetics, low nitrogen (N<sub>2</sub>) solubility in aqueous electrolytes, and the competing hydrogen evolution reaction (HER), which can significantly impact NH<sub>3</sub> production rates and Faradaic efficiency (FE). Herein, a rationally designed boron-doped molybdenum sulfide (B-Mo-Mo<sub>x</sub>S<sub>y</sub>) electrocatalyst is reported that effectively enhances N<sub>2</sub> reduction to NH<sub>3</sub> with an onset potential of -0.15 V versus RHE, achieving a FE of 78% and an NH<sub>3</sub> yield of 5.83 µg h⁻¹ cm⁻<sup>2</sup> in a 0.05 m H<sub>2</sub>SO<sub>4</sub>(aq). Theoretical studies suggest that the effectiveness of NRR originates from electron density redistribution due to boron (B) doping, which provides an ideal pathway for nitrogenous species to bind with electron-deficient B sites. This work demonstrates a significant exploration, showing that Mo-based electrocatalysts are capable of facilitating artificial N<sub>2</sub> fixation.