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Engineering the Electronic Microenvironment with Bromine Functionalization for High‐Selectivity Photocatalytic CO2 Reduction

The research presents a surface bromine modification for the covalent organic framework TzPm‑COF, creating TzPm‑COF‑2Br with a tuned donor‑acceptor architecture. This brominated COF delivers a CO evolution rate of 155 µmol g⁻¹ h⁻¹ and 99.4 % selectivity under visible light, a 2.7‑fold increase over the unmodified material. Kelvin probe force microscopy and density functional theory reveal that bromine atoms enhance charge separation and direct electron flow toward CO₂ adsorption sites. The findings outline a rational design route for next‑generation CO₂‑reduction photocatalysts.