Impact Factor:

22.1

DOI number:

10.1016/j.apcatb.2026.127024

Journal:

Applied Catalysis B: Environment and Energy

Key Words:

Lu single atoms; electron bridge; carbon nitride; photocatalysis; CO2 conversion

Abstract:

Photocatalytic CO₂ reduction on graphitic carbon nitride (CN) is hindered by slow interlayer charge transfer. While single-atom catalysts (SACs) are often confined to in-plane sites, we propose a distinct interlayer-SAC strategy by anchoring lutetium (Lu) single atoms within CN interlayers (LuCNv0. 20). Advanced characterizations and density functional theory (DFT) confirm the formation of unique interlayer Lu-N electronic bridges, which serve as dedicated vertical charge channels. Femtosecond transient absorption (fs-TA) spectroscopy reveals a longer-lived kinetic component (τ2= 15.75 ps) that is reasonably assigned to bridge-mediated interlayer charge transport, together with suppressed recombination. The catalyst achieves a high CO production rate of 56.30 μmol g-1 h-1 with 97.80% selectivity and an apparent quantum yield (AQY) of 11.69% at 400 nm, representing a 2.36-fold gain over pristine CN and demonstrating competitive performance among representative non-precious-metal photocatalysts reported for CO2 reduction. In situ DRIFTS shows the bridges also facilitate CO2 activation via* COOH stabilization. This work introduces interlayer electronic bridges as a new design principle to engineer charge transport in layered photocatalysts. This work establishes rare-earth single-atom Lu-N6 interlayer electronic bridges in polymeric carbon nitride, linking a quantified interlayer charge-transfer acceleration with CO2 adsorption/activation control, thereby translating interlayer engineering into CO-selective photocatalysis without cocatalysts or sacrificial agents.

Co-author:

刘彬,张祎

Indexed by:

SCI

Correspondence Author:

LYH

Document Code:

125007

Document Type:

Journal Article

Volume:

352

Page Number:

125007

ISSN No.:

0926-3373

Translation or Not:

no

Date of Publication:

2026-05-26

Included Journals:

SCI