ZIF‐Induced d‐Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction
Howard Yi Fan Sim, Jaslyn Ru Ting Chen, Charlynn Sher Lin Koh, Hiang Kwee Lee, Xuemei Han, Gia Chuong Phan‐Quang, Jing Pang, Chee Leng Lay, Srikanth Pedireddy, In Yee Phang, Edwin K. L. Yeow, Xing Yi Ling
Abstract
Abstract 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 μg 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.