CO reduction photocatalysts are favorable for obtaining renewable energy. Enriched active sites and effective photogenerated-carriers separation are keys for improving CO photo-reduction. A thulium (Tm) single atom tailoring strategy introducing carbon vacancies in porous tubular graphitic carbon nitride (g-CN) surpassing the ever-reported g-CN based photocatalysts, with 199.47 µmol g h CO yield, 96.8% CO selectivity, 0.84% apparent quantum efficiency and excellent photocatalytic stability, is implemented in this work. Results revealed that in-plane Tm sites and interlayer-bridged Tm-N charge transfer channels significantly enhanced the aggregation/transfer of photogenerated electrons thus promoting CO adsorption/activation and contributing to *COOH intermediates formation. Meanwhile, Tm atoms and carbon vacancies both benefit for rich active sites and enhanced photogenerated-charge separation, thus optimizing reaction pathway and leading to excellent CO photo-reduction. This work not only provides guidelines for CO photo-reduction catalysts design but also offers mechanistic insights into single-atom based photocatalysts for solar fuel production.
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| http://dx.doi.org/10.1002/advs.202406329 | DOI Listing |
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