Engineered interface coverage and precise cocatalyst placement in MOF-derived heterojunction photocatalysts for selective methane oxidation

通过对界面覆盖率和助催化剂的精确定位,实现MOF衍生异质结光催化剂的选择性甲烷氧化

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Abstract

While the rational fabrication of heterojunction photocatalysts with tunable interfaces and precise location control of cocatalysts holds great promise for enhanced photocatalysis, the synergistic integration of these parameters remains a substantial challenge. Herein, a series of metal-organic framework (MOF) composites with compact interfaces and customizable interface coverage are designed by epitaxial growth of ZIF-8 on the surface of MIL-125-NH(2), yielding ZIF-8 (m) /MIL-125-NH(2) (m = 21, 35, 65, representing the coverage percentage of ZIF-8 on the MIL-125-NH(2) surface). These composites are then converted into ZnO/TiO (x) heterojunctions through a two-step thermal treatment, termed ZTO-m, for photocatalytic CH(4) oxidation. The results reveal that the interface coverage in ZTO-m plays critical roles in charge separation, where ZTO-65 gives the best activity. With ZTO-65 as a basis, the cocatalysts, Au clusters and CoO (x) species, are respectively positioned onto TiO (x) and ZnO. The targeted positioning of cocatalysts not only improves charge separation but also facilitates O(2) activation. As a result, the resulting Au-Co-ZTO demonstrates excellent activity toward liquid oxygenate production, achieving 1723.5 μmol g(-1) h(-1) with a selectivity of 99%, in photocatalytic CH(4) oxidation.

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