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Single Atomic Noble Metal Enclosed Defective MOF via Cryogenic UV-photo-reduction for CO Oxidation with ultra-high Efficiency and Stability.

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 reduced noble metal cost. However, the practical utilization of SACs enabled heterogeneous catalysis has the bottlenecks in high manufacturing cost and 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. Scalable and low-energy-consumption synthesis of SACs strongly coordinated with atomically designed 3D nanostructure are 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 photo-reduction 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 low weight content of 0.12 w.t% exhibited 100% conversion of CO at low temperature of 150 °C, consuming only 10% of Pt that required by state-of-the-art catalysts operated under same condition, standing as the most effective catalyst reported to date. In addition, this catalyst is active even under low temperature 40 °C and could withstand temperature as high as 300 °C for a long time with 100% conversion efficiency. This work reveals that the porous and crystalline nature of MOF provides strong interaction and fast reaction kinetics for the gaseous reactants and product. The strong coordination of noble metal to the cerium oxide units in Ce-MOF not only promotes stability but also controls activity of the isolated catalyst, thus ensuring excellent atomic utilization of expensive precious metals.