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Optimizing Electrocatalytic Nitrogen Reduction via Interfacial Electric Field Modulation: Elevating d‐Band Center in WS2‐WO3 for Enhanced Intermediate Adsorption

Von Wiley-VCH zur Verfügung gestellt

Electrocatalytic nitrogen reduction reaction (ENRR) has emerged as a promising approach to synthesizing green ammonia under ambient conditions. Tungsten (W) has been found to be one of the most effective ENRR catalyst, with the protonation of intermediates as the rate-determining step (RDS). Enhancing the adsorption of intermediates is crucial to increase the protonation of intermediates and thus improve the catalyst's overall performance. Herein, we aimed to construct a strong interfacial electric field in WS2-WO3 to elevate the d-band center of W, thereby strengthening the adsorption of intermediates. Experimental results demonstrated that this approach led to a significantly improved ENRR performance. Specifically, WS2-WO3 exhibited a high NH3 yield of 62.38 μg h-1mgcat-1 and a promoted faraday efficiency (FE) of 24.24 %. Furthermore, in-situ characterizations and theoretical calculations showed that the strong interfacial electric field in WS2-WO3 upshifted the d-band center of W towards the Fermi level, leading to enhanced adsorption of -NH2 and -NH intermediates on the catalyst's surface. This, resulted in a significantly promoted reaction rate of the RDS. Overall, our study offers new insights into the relationship between interfacial electric field and d-band center and provides a promising strategy to enhance the intermediates adsorption during the ENRR process.

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