Scalable Synthesis of Flexible Single-Atom Monolithic Catalysts for High-Efficiency, Durable CO Oxidation at Low Temperature.

Abstract

The creation of single-atom catalysts in a large-size, high-yield, and stable form represents an important direction for high-efficiency industrial catalysis in the future. Herein, we report a strategy to synthesize flexible single-atom monolithic catalysts (SAMCs) based on the hierarchical 3D assembly of single-atom-loaded oxide ceramic nanofibers. The nanofibers, which can be produced in a continuous and scalable manner, serve as an ideal support for single atoms spontaneously and almost completely exposed at the surface through the Kirkendall effect-enabled in situ ion migration during the spinning process, resulting in both high yield and large loading quantity. Moreover, the hierarchical 3D assembly of these nanofibers into a porous, flexible structure endows the SAMCs with the advantages of sufficient infiltration and oscillation tolerance when faced with high-throughput gaseous media, leading to both high catalytic efficiency and excellent durability. As a proof-of-concept demonstration, a Pt SAMC is synthesized, which exhibits 100% CO oxidation at low temperature (∼170 °C), excellent invariance toward high-frequency (10 Hz) oscillation, and high structural stability from 25 to 300 °C. This work is beneficial for the large-scale production of SAMCs in broad industrial applications.