ZIF-induced d-band Modification in Bimetallic Nanocatalyst: Achieving >44% Efficiency in 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 Yi Pang, Chee Leng Lay, Srikanth Pedireddy, In Yee Phang, Edwin Kok Lee Yeow, Xing Yi Ling

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

Abstract

Electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance due to preferential catalyst-H formation and the consequential hydrogen evolution reaction (HER). Herein, we electronically modify PtAu electrocatalyst d-band structure 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 at ambient conditions. Our 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 electrocatalyst doubles as a hydrophobic layer to suppress HER, further improves FE by >44-fold compared to without ZIF (~1%). Experimental and in-silico studies reveal PtAu-N ZIF interaction is key to enable strong N 2 adsorption over H atom. Our electrocatalytic design is universal and can be extended across metal electrocatalysts for diverse applications in NRR and air-to-fuel conversion.
Original languageEnglish (US)
JournalAngewandte Chemie (International ed. in English)
DOIs
StatePublished - May 29 2020

Fingerprint

Dive into the research topics of 'ZIF-induced d-band Modification in Bimetallic Nanocatalyst: Achieving >44% Efficiency in Ambient Nitrogen Reduction Reaction.'. Together they form a unique fingerprint.

Cite this