Photothermally induced defect engineering: boosting photothermal synergistic selective catalytic oxidation of benzyl alcohol over <i>in situ</i> oxygen vacancy-modulated ultrathin ZnTi-LDH nanosheet

The coordination and activation of C-O bonds into high-value-added CO bond products are significant and sustainable processes. Nevertheless, most researchers have focused on converting C-O bonds either through green photocatalysis or industrial thermocatalysis independently. The coordination and activation of C-O bonds <i>via</i> defect engineering, particularly stimulated by the emerging photothermal synergy effect, remain less explored. Herein, we investigate the photothermal effect-induced construction of oxygen vacancies (OVs) with varying concentrations on ultrathin ZnTi-LDH nanosheets (denoted as <i>ZT</i>-25, <i>ZT</i>-50, and <i>ZT</i>-70; <i>T</i> = 25, 50, and 70 °C, respectively) for the selective oxidation of benzyl alcohol under visible light irradiation. Extensive experimental characterization and theoretical calculations jointly indicate that ultrathin ZnTi-LDH nanosheets can produce more coordinatively unsaturated OVs with the increase in reaction temperatures. These OV active sites can achieve the coordination and activation of benzyl alcohol effortlessly. The <i>ZT</i>-70 sample shows a 57.78% conversion efficiency for the photothermal oxidation of benzyl alcohol, higher than that achieved by <i>ZT</i>-25 (44.40%). The elevated performance is attributed to the abundant OV active sites and optimal transfer of photothermally induced charges. This work presents a green strategy to achieve the activation of C-O bonds for benzyl alcohol oxidation <i>via</i> defect engineering induced by the photothermal synergy effect.