ZIF-Induced d-Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction.
Howard Yi Fan SimJaslyn Ru Ting ChenCharlynn Sher Lin KohHiang Kwee LeeXuemei HanGia Chuong Phan-QuangJing Yi PangChee Leng LaySrikanth PedireddyIn Yee PhangEdwin Kok Lee YeowXing Yi LingPublished in: Angewandte Chemie (International ed. in English) (2020)
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 mgcat -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-N2 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-NZIF interaction is key to enable strong N2 adsorption over H atom.
Keyphrases
- metal organic framework
- electron transfer
- aqueous solution
- ionic liquid
- room temperature
- reduced graphene oxide
- air pollution
- visible light
- particulate matter
- gold nanoparticles
- sensitive detection
- highly efficient
- oxidative stress
- high glucose
- diabetic rats
- anaerobic digestion
- endothelial cells
- mass spectrometry
- protein kinase
- electron microscopy
- liquid chromatography