P-mediated Cu-N 4 sites in carbon nitride realizing CO 2 photoreduction to C 2 H 4 with selectivity modulation.

Photocatalytic CO 2 reduction to high value-added C 2 products (e.g., C 2 H 4 ) is of considerable interest but challenging. The C 2 H 4 product selectivity strongly hinges on the intermediate energy levels in the CO 2 reduction pathway. Herein, we design the Cu-N 4 sites anchored phosphorus-modulated carbon nitride (CuACs/PCN) as the photocatalyst to tailor the intermediate energy levels in the C 2 H 4 formation reaction pathway for realizing its high production with tunable selectivity. Theoretical calculations combined with experimental data demonstrate that the formation of the C-C coupling intermediates can be realized on Cu-N 4 sites and the surrounding doped P facilitate the production of C 2 H 4 . Thus, CuACs/PCN exhibits a high C 2 H 4 selectivity of 53.2% with a yielding rate of 30.51 μmol·g -1 . The findings reveal the significant role of the coordination environment and surrounding microenvironment of Cu single atoms in C 2 H 4 formation and offer an effective approach for highly selective CO 2 photoreduction to produce C 2 H 4 . This article is protected by copyright. All rights reserved.