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ZIF‐Induced d‐Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction
Author(s) -
Sim Howard Yi Fan,
Chen Jaslyn Ru Ting,
Koh Charlynn Sher Lin,
Lee Hiang Kwee,
Han Xuemei,
PhanQuang Gia Chuong,
Pang Jing Yi,
Lay Chee Leng,
Pedireddy Srikanth,
Phang In Yee,
Yeow Edwin Kok Lee,
Ling Xing Yi
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202006071
Subject(s) - electrocatalyst , catalysis , faraday efficiency , bimetallic strip , chemistry , electrochemistry , adsorption , inorganic chemistry , ammonia production , reversible hydrogen electrode , nitrogen , redox , chemical engineering , electrode , organic chemistry , working electrode , engineering
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.