A butterfly-like lead-doped titanium-oxide compound with high performance in photocatalytic cycloaddition of CO2 to epoxide

Abstract

The cycloaddition reaction of CO₂ to epoxides is quite promising for CO₂ capture and storage as well as the production of value-added fine chemicals. Herein, a novel atomically precise lead-doped titanium-oxide cluster with the formula Ti₁₀Pb₂O₁₆(phen)₄(Ac)₁₂(DMF)₂ (denoted as Ti₁₀Pb₂; phen = 1,10-phenanthroline; Ac = acetate; DMF = dimethylformamide) was synthesized through a facile solvothermal process, and is a molecular photocatalyst with surface-anchored main-group metal active sites. Its structure was characterized by single-crystal X-ray diffraction and other complementary techniques. Ti₁₀Pb₂ showed high photo-response and charge-separation efficiency under simulated sunlight irradiation. Ti₁₀Pb₂ was successfully used in the cycloaddition reaction of CO₂ with epoxides under solvent-free conditions. While its catalytic activity due to the Lewis acidity was moderate, simulated solar light irradiation further enhanced the reaction rate, demonstrating the synergistic effect of photocatalysis and Lewis-acid thermocatalysis.