Brønsted Acid‐Driven Dynamic LMCT Sites Transform Pt/Zeolite Into a Light‐Responsive Oxidation Platform

Photocatalysis provides a low‐temperature oxidation route, yet typically underperforms thermal catalysis owing to inefficient O 2 activation and limited surface‐bounded intermediates utilization. Here, a conventional Pt/zeolite catalyst is transformed into a photothermal‐photoelectronic platform by leveraging Brønsted acid‐mediated dynamic ligand‐to‐metal charge transfer (LMCT) sites. Using toluene oxidation over Pt/ZSM‐5 as a model, we show that benzyl alcohol formed under UV irradiation undergoes acid‐assisted deprotonation and coordinates with Pt, forming Pt‐O‐CH 2 ‐Ar complexes. These species enable visible‐light absorption and O 2 activation via LMCT mechanism, thereby significantly enhancing the oxidation efficiency. This UV‐enabled formation and visible‐light‐triggered LMCT excitation of surface intermediates merges photothermal effects and photoelectronic effects, achieving complete degradation of 1000 ppm toluene under light‐only conditions at 240–480 L g −1 h −1 with only 0.5 wt.% Pt. The strategy extends to other aromatic hydrocarbons through alcohol‐ or phenol‐type intermediates. This study establishes a general approach to boost light‐driven O 2 activation through dynamic intermediate coordination, opening avenues for energy‐efficient oxidation.