Boosted Electrocatalytic N Reduction on Fluorine-Doped SnO Mesoporous Nanosheets.

The development of highly active and durable electrocatalysts toward the N reduction reaction (NRR) holds a key to ambient electrocatalytic NH synthesis. Herein, fluorine (F)-doped SnO mesoporous nanosheets on carbon cloth (F-SnO/CC) were developed as an efficient NRR electrocatalyst. Benefiting from the combined structural advantages of mesoporous nanosheet structure and F-doping, the F-SnO/CC exhibited high NRR activity with an NH yield of 19.3 μg h mg and a Faradaic efficiency of 8.6% at -0.45 V (vs RHE) in 0.1 M NaSO, 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 SnO 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.