Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 39, Pages 16997-17003Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202006071
Keywords
d-band modification; electrochemical nitrogen reduction reaction; interfacial cavities; metal-organic frameworks; solid@MOF nanoparticles
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Funding
- Ministry of Education, Singapore, under Tier 1 grant [RG11/18]
- Max Planck Institute-Nanyang Technological University Joint Lab
- Nanyang Technological University, Singapore
- CN Yang scholarship
- Singapore Ministry of Education
- Ministry of Education, Singapore, under Tier 2 grant [MOE2016-T21-043]
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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.
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