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Metal-Organic Frameworks (MOFs) have shown great potential in catalysis due to their high surface area, tunable pore size, and diverse chemical functionality. In this study, we present the preparation of a novel MOF, (Cu-N-COF), consisting of atomically dispersed copper sites coordinated to nitrogen and carbon atoms in a two-dimensional imine linked framework. These highly dispersed copper sites facilitated the efficient reduction of nitrogen dioxide (NO2) to nitrogen monoxide (NO) in the presence of hydrogen (H2) at room temperature and atmospheric pressure. X-ray photoelectron spectroscopy (XPS) confirmed the successful incorporation of copper into the framework. Transmission electron microscopy (TEM) indicated that the Cu-N-COF framework was composed of interconnected two-dimensional sheets with well-defined pores, and the copper sites were homogeneously dispersed throughout the framework. Catalytic tests were performed under different reaction conditions to investigate the effect of temperature, pressure, and reaction time on the catalytic activity. Remarkably, Cu-N-COF showed high catalytic activity and selectivity toward the reduction of NO2 to NO, with a conversion rate of 100% and a selectivity of 95% under optimal conditions. The turnover frequency (TOF) of Cu-N-COF was nearly eight times higher than that of Cu dispersed on activated carbon and 2.3 times higher than that of CuO nanoparticles supported on aluminum oxide. The outstanding catalytic performance of Cu-N-COF could be attributed to the high dispersion of copper sites and the synergistic interaction between nitrogen, carbon, and copper atoms in the framework. Density functional theory (DFT) calculations suggested that the active intermediates were coordinated to the copper sites and could be easily reduced by H2 assimilated on the nitrogen atoms in the framework. In conclusion, we have successfully synthesized a novel MOF with highly dispersed copper sites for efficient reduction of NO2 to NO. This work provides a new strategy for designing highly efficient and selective catalysts based on atomically dispersed metal sites in MOFs Copper scrap analysis Scrap Copper wire recycling

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