Boosted Electrocatalytic N₂ Reduction on Fluorine-Doped SnO₂ Mesoporous Nanosheets

Abstract

The development of highly active and durable electrocatalysts toward the N₂ reduction reaction (NRR) holds a key to ambient electrocatalytic NH₃ synthesis. Herein, fluorine (F)-doped SnO₂ mesoporous nanosheets on carbon cloth (F-SnO₂/CC) were developed as an efficient NRR electrocatalyst. Benefiting from the combined structural advantages of mesoporous nanosheet structure and F-doping, the F-SnO₂/CC exhibited high NRR activity with an NH₃ yield of 19.3 μg h^-1 mg^-1 and a Faradaic efficiency of 8.6% at -0.45 V (vs RHE) in 0.1 M Na₂SO₄, comparable or even superior to those of most reported NRR electrocatalysts. Density functional theory calculations revealed that the F-doping could readily tailor the electronic structure of SnO₂ to render it with improved conductivity and increased positive charge on active Sn sites, leading to the lowered reaction energy barriers and boosted NRR activity.