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Abstract

Carbonaceous electrocatalysts offer advantages over metal-based counterparts, being cost-effective, sustainable, and electrochemically stable. Their high surface area increases reaction kinetics, making them valuable for environmental applications involving contaminant removal. However, their rational synthesis is challenging due to the applied high temperatures and activation steps, leading to disordered materials with limited control over doping. Here, a new synthetic pathway using carbon oxide precursors and tin chloride as a p-block metal salt melt is presented. As a result, highly porous oxygen-rich carbon sheets (with a surface area of 1600 m² g^-1) are obtained at relatively low temperatures (400 °C). Mechanistic studies reveal that Sn(II) triggers reductive deoxygenation and concomitant condensation/cross-linking, facilitated by the Sn(II) → Sn(IV) transition. Due to their significant surface area and oxygen doping, these materials demonstrate exceptional electrocatalytic activity in the nitrate-to-ammonia conversion, with an ammonia yield rate of 221 mmol g^-1 h^-1 and a Faradic efficiency of 93%. These results surpass those of other carbon-based electrocatalysts. In situ Raman studies reveal that the reaction occurs through electrochemical hydrogenation, where active hydrogen is provided by water reduction. This work contributes to the development of carbonaceous electrocatalysts with enhanced performance for sustainable environmental applications.