1. Creation of molecular-level surface active centers on polymeric carbon nitride for boosting selectively photocatalytic CO2 reduction to CO.
- Author
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Sun, Dawei, Han, Jinlong, Xiao, Mengya, Cao, Tieping, Li, Yuejun, and Dong, Hongjun
- Abstract
[Display omitted] • Molecular-level surface active centers are created on PCN. • Au-bpy/PCN composite can effectively impel spatial charge separation. • The photocatalytic CO 2 reduction performance is improved dramatically. • Au-bpy/PCN composite has about 100% selectivity for CO 2 reduction to CO. The directional design of constructing surface active centers has been a challenging issue in the development of efficient photocatalysts. In the contribution, the molecular-level surface active centers are created on polymeric carbon nitride (PCN) through π-π interaction with organic conjugated small molecule complex Au-bpy. In the prepared Au-bpy/PCN composite, Au-bpy is decorated on the surface of PCN in the molecular state and molecularly aggregated nanocrystal. Strikingly, the investigations of the optical properties and charge transport behaviors indicate that the modification of Au-bpy effectively extends the light response range, narrows the band gap and improves the separation efficiency of photogenerated carriers. At the same time, the structural evolution of Au-bpy/PCN composite reveals that the Au-bpy in the molecular state can be served as the surface active centers, and Au-bpy nanocrystal is reduced to Au nanoparticles that can induce local surface plasmonic resonance effect, thus significantly boosting the photocatalytic activity with about 100 % selectivity for CO 2 reduction to CO. As a consequence, the average CO evolution rate increases from 39.7 μmol g-1h−1 over primitive PCN up to 113.2 μmol g-1h−1 over the optimal Au-bpy/PCN-3 in the photocatalytic CO 2 reduction reaction. This work opens a new avenue for the design of surface active sites on the photocatalysts on the molecular scale. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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