Amorphous core/shell Ti-doped SnO_(2) with synergistically improved N_(2) adsorption/activation and electrical conductivity for electrochemical N_(2) reduction

摘要

Electrochemical nitrogen reduction reaction(NRR)has been considered as an appealing and sustainable method to produce ammonia from N_(2) under ambient conditions,attracting increasing interest.Limited by low solubility of N_(2) in water and high stability of Ntriple bondN triple bond,developing NRR electrocatalysts with both strong N_(2) adsorption/activation and high electrical conductivity remain challenging.Here,we demonstrate an efficient strategy to develop NRR electrocatalyst with synergistically enhanced N_(2) adsorption/activation and electrical conductivity by heteroatom doping.Combining computational and experimental study,the DFT-designed Ti-doped SnO_(2) exhibits significantly enhanced NRR performance with ammonia yield rate of 13.09µg h^(-1) mg^(-1) at −0.2 V vs.RHE.Particularly,the Faradaic efficiency reaches up to 42.6%,outperforming most of Sn-based electrocatalysts.The fundamental mechanism for improving NRR performance of SnO_(2) by Ti doping is also revealed.Our work highlights a powerful strategy for developing high-activity electrocatalysts for NRR and beyond.