A Single-Atomic Noble Metal Enclosed Defective MOF via Cryogenic UV Photoreduction for CO Oxidation with Ultrahigh Efficiency and Stability.

ABSTRACT

Noble metal single-atom catalysts (SACs) can provide maximized interaction with the reactants and tunable electronic structure dictated by the coordinated support, thus enabling unprecedented high activity at a reduced noble metal cost. However, the practical utilization of SACs that enabled heterogeneous catalysis has the bottlenecks in high manufacturing cost, low catalytic efficiency, and low atomic utilization of metals due to poor porosity of supporting structures, low affinity between SACs and supports, and high-temperature synthesis involved. A scalable and low-energy consumption synthesis of SACs strongly coordinated with an atomically designed 3D nanostructure is needed to realize higher catalytic efficiency and atomic utilization efficiency. Here, a facile synthesis strategy is developed by applying low-cost cerous MOF (Ce-MOF) with tailored defects across the porous and crystalline structure. SACs (Pt) synthesized by cryogenic photoreduction can be enclosed at the defects in Ce-MOF. Due to the uniform dispersion and the unique electronic hybridization with Ce-MOF, the conjugated catalyst with a low weight content of 0.12 wt % exhibited 100% conversion of CO at a low temperature of 150 °C, consuming only 10% of Pt required by state-of-the-art catalysts operating under the same conditions, standing as the most effective catalyst reported to date.