The construction of CN/UiO-67 (CNU) S-scheme heterojunction composites through in situ formation of UiO-67 on carbon nitride (CN) helps to address the limitations of carbon nitride (CN) in photocatalytic NO elimination. The optimized CNU demonstrates superior photocatalytic efficiency, which is attributed to electronic channels constructed by Zr-N bonds and S-scheme electron transport mechanism, effectively promoting the efficient separation of photogenerated charge carriers with high redox potentials. Density Functional Theory (DFT) calculations reveal redistributed electronic orbitals in CNU, with progressive and continuous energy levels near the Fermi level, which bolsters electronic conduction. Comprehensive quenching experiments, Electron Paramagnetic Resonance (EPR), and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analyses highlight a synergistic interplay of electrons, holes, and superoxide radicals in CNU, inhibiting the generation of toxic nitrogen oxide intermediates and culminating in highly efficient photocatalytic NO oxidation. This study not only elucidates the mechanisms underpinning the enhanced performance of CNU heterojunctions but also offers new perspectives on the preparation and interfacial charge separation of heterojunction photocatalysts.
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http://dx.doi.org/10.1016/j.jcis.2024.02.221 | DOI Listing |
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