TS-1 zeolite encapsulated Pt clusters with enhanced electronic metal-support interaction of Pt−O(H)−Ti for nearly-zero-carbon-emitting photocatalytic hydrogen production from methanol

Abstract

Photocatalytic H2 production from methanol is sustainable, yet challenges remain in avoiding carbon-containing gaseous by-products. Titanium silicalite-1 (TS-1) zeolite possesses attractive photocatalytic performance, but lack of modification strategies due to its microporous framework. Herein, we developed a pre-anchoring strategy to confine ultra-small Pt clusters inside TS-1 with ultra-low loading (0.2 mol%), in which Pt were anchored in Ti−OH nests by electronic metal-support interaction (EMSI). The optimal catalyst achieved a remarkable H2 generation rate of 63.2 mmol g–1 h–1 in CH3OH solutions, along with the production of high-value chemical HCHO as the oxidation product with 96.9% selectivity. Investigations reveal that the EMSI between Pt and Ti facilitated the selective decomposition of CH3OH to H2 and HCHO, leading to a nearly zero-carbon-emission process. Accordingly, we propose a light-driven carbon-negative "CO2→CH3OH→H2" route, coupling CO2 utilization and green H2 production with CH3OH as the intermediate, therefore offering a new perspective for "liquid sunshine".