Construction of single-atom copper-loaded iron-based MOF/carbon nitride nanosheet heterojunction for enhanced N₂ photofixation under visible light

Abstract

The utilization of photocatalytic nitrogen fixation, a process celebrated for its environmental friendliness and sustainability, has emerged as a promising avenue for ammonia synthesis. The rational design of photocatalysts containing single atoms and heterojunctions has been a long-standing challenge for achieving efficient nitrogen fixation. This study innovatively constructs composite catalysts integrating single-atom copper within metal–organic frameworks (Fe-MOF, NH₂-MIL-101) and carbon nitride nanosheet (CNNS). The nitrogen fixation efficiency of the Cu@MIL-CNNS heterojunction was 8 and 12 times those of the original MOF and CNNSs, respectively. Through detailed characterization, we unveil a unique charge transfer pathway facilitated by the synergy between single-atom copper and heterojunctions, highlighting the critical function of copper centers as potent active sites. Our findings underscore the transformative potential of single atomic sites in amplifying charge transfer efficiency, propelling advancements in the photocatalyst design.

Graphical abstract

Keywords

single atom copper / photocatalytic nitrogen fixation / metal–organic framework / carbon nitride nanosheet

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