%0 Journal Article
%T Outstanding CO2 Photoreduction in Single-Atom Thulium Modified Carbon Nitride.
%A Ding C
%A Yang L
%A Lu X
%A Chi H
%A Yang Y
%A Yuan J
%A Wang X
%A Wu X
%A Zhang Y
%A Zhou Y
%A Zou Z
%J Adv Sci (Weinh)
%V 0
%N 0
%D 2024 Aug 9
%M 39120492
%F 17.521
%R 10.1002/advs.202406329
%X CO2 reduction photocatalysts are favorable for obtaining renewable energy. Enriched active sites and effective photogenerated-carriers separation are keys for improving CO2 photo-reduction. A thulium (Tm) single atom tailoring strategy introducing carbon vacancies in porous tubular graphitic carbon nitride (g-C3N4) surpassing the ever-reported g-C3N4 based photocatalysts, with 199.47 µmol g-1 h-1 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 CO2 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 CO2 photo-reduction. This work not only provides guidelines for CO2 photo-reduction catalysts design but also offers mechanistic insights into single-atom based photocatalysts for solar fuel production.