Accelerated N-2 reduction kinetics in hybrid interfaces of NbTiO4 and nitrogen-doped carbon nanorod via synergistic electronic coupling effect
Chun, Hoje 1Han, Byungchan 1Shanmugam, Sangaraju 2Yesudoss, David Kumar2
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作者信息
1. Yonsei Univ
2. Daegu Gyeongbuk Inst Sci & Technol DGIST
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Abstract
Electrochemical ammonia synthesis through the atmospheric nitrogen reduction reaction (NRR) is a promising method for sustainable fertilizer and carbon-free hydrogen energy carriers. The inevitable selectivity gap against hydrogen evolution reaction and inert nitrogen (N-2) hinders the device-level usage of nitrogen cathodes. In this work, we report engineered electrocatalyst/support interface of NbTiO4 nanoparticles supported on nitrogen doped carbon nanorods (NbTiO4@NCNR) to catalyze NRR. Insisted by the pitfalls to rationally design N-2 reduction catalysts, the strong catalyst-support interaction strategy is adapted to tune the selectivity towards NRR. Electrochemical tests reveal that NbTiO4@NCNR hybrid accelerates a 10-fold increase in N-2 selectivity compared to pure metal oxide. Using first-principles calculations, we identify the underlying mechanism of enhanced performance: bridging bonds in the interface as electron transport channels to promote the N-2 reduction kinetics. Essentially, this study provides an insight into how to overcome the immense kinetic barrier of NRR using smartly engineered interfaces of hybrid materials.
NSTL
Elsevier