One‐step supramolecular pre‐organizational synthesis of copper‐doped porous carbon nitride for high photocatalytic nitrogen fixation

Abstract

AbstractSolar‐driven reduction of nitrogen to ammonia is a promising green approach and is considered as a sustainable alternative to the Haber–Bosch process. Carbon nitride (g‐C3N4) is an ideal non‐metallic semiconductor photocatalyst for photocatalytic N2 reduction reaction (p‐NRR). In this work, we designed a simple supramolecular self‐assembly method to prepare copper‐doped porous graphitic nitride (Cu@pg‐C3N4) photocatalysts. The synergistic semiconductor and metal interactions enabled the obtained Cu@pg‐C3N4 to achieve larger specific surface area, more efficient photogenerated carrier separation, and stronger photoreduction ability. The specific surface area of Cu@pg‐C3N4 increased from 5.69 to 75.76 μmol/L, exposing more active sites compared to bulk g‐C3N4. The NH4+ production rate of the obtained Cu@pg‐C3N4 was 150.47 μmol/L, which is 20 times higher than that of the bulk carbon nitride, exhibiting excellent N2 photofixation ability. These findings highlight the significant progress that can be achieved by metal supramolecular network modification strategies in harnessing the potential of carbon nitride for photocatalytic reduction applications.