ZIF-Induced d-Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 Efficiency in the Ambient Nitrogen Reduction Reaction

摘要

The electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance owing to preferential catalyst-H formation and the consequential hydrogen evolution reaction (HER). Now, the Pt/Au electrocatalyst d-band structure is electronically modified using zeolitic imidazole framework (ZIF) to achieve a Faradaic efficiency (FE) of >44 with high ammonia yield rate of >161 mu g mg(cat)(-1) h(-1)under ambient conditions. The strategy lowers electrocatalyst d-band position to weaken H adsorption and concurrently creates electron-deficient sites to kinetically drive NRR by promoting catalyst-N(2)interaction. The ZIF coating on the electrocatalyst doubles as a hydrophobic layer to suppress HER, further improving FE by >44-fold compared to without ZIF (ca. 1 ). The Pt/Au-N(ZIF)interaction is key to enable strong N(2)adsorption over H atom.