Journal
ADVANCED ENERGY MATERIALS
Volume 13, Issue 6, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202203201
Keywords
diatomic Pt-Ce; chemical affinity; electrochemical nitrate reduction; interlayer spacing regulation; p-orbital delocalization
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This study reports a method to tailor the interlayer spacing of 2D SnS nanosheets, which enhances the chemical affinity towards NO3- and NO2- while inhibiting hydrogen generation. This promotes the rate-determining step in electrochemical nitrate reduction to ammonia and achieves excellent Faradaic efficiency and yield rate.
Electrochemical nitrate reduction to ammonia (eNO(3)RR) is a green and appealing method for ammonia synthesis, but is hindered by the multistep chemical reaction and competitive hydrogen generation. Herein, the synthesis of 2D SnS nanosheets with tailored interlayer spacing is reported, including both expansion and compression, through the active diatomic Pt-Ce pairs. Taking together the experimental results, in situ Raman spectra, and DFT calculations, it is found that the compressed interlayer spacing can tune the electron density of localized p-orbital in Sn into its delocalized states, thus enhancing the chemical affinity towards NO3- and NO2- but inhibiting hydrogen generation simultaneously. This phenomenon significantly facilitates the rate-determining step (*NO3 ->*NO2) in eNO(3)RR, and realizes an excellent Faradaic efficiency (94.12%) and yield rate (0.3056 mmol cm(-2) h(-1)) for NH3 at -0.5 V versus RHE. This work provides a powerful strategy for tailoring flexible interlayer spacing of 2D materials and opens a new avenue for constructing high-performance catalysts for ammonia synthesis.
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