A Janus antimony sulfide catalyst for highly selective N2 electroreduction

Abstract

The antimony sulfide Sb₂S₃ is firstly explored as a Janus catalyst for highly selective nitrogen reduction reaction (NRR). The developed Sb₂S₃ nanoflowers delivered an excellent faradaic efficiency of 24.1% and a high NH₃ yield of 33.4 μg h⁻¹ mg⁻¹ at −0.3 V. Theoretical calculations revealed that the high NRR selectivity of Sb₂S₃ originated from the Janus role of active Sb centers: on one hand, Sb exhibited a strong Sb5p–N2p hybridization upon initial N₂ protonation, capable of effectively activating the NRR with a low reaction barrier. On the other hand, Sb could concurrently impede the hydrogen evolution by hindering the H⁺ adsorption.