Boosted nitrate electroreduction to ammonia on Fe-doped SnS₂ nanosheet arrays rich in S-vacancies

The electrochemical nitrate reduction reaction (NO₃RR) not only holds great potential for the removal of NO₃^- contaminants from the environment, but also potentially provides a renewable-energy-driven NH₃ synthesis method to replace the Haber-Bosch process. Herein, we report that Fe-doped SnS₂ nanosheets enriched with S-vacancies can be used as an efficient NO₃RR catalyst, showing a high NH₃ yield of 7.2 mg h^-1 cm^-2 (at -0.8 V) and a faradaic efficiency of 85.6% (at -0.7 V). Density functional theory (DFT) calculations revealed that S-vacancies on Fe-SnS₂ serve as the main active sites for the NO₃RR and the Fe-doping can further regulate the electronic structure of S-vacancies to optimize the binding energies of NO₃RR intermediates, resulting in reduced energy barriers and enhanced NO₃RR activity.