Tailoring Unsymmetrical‐Coordinated Atomic Site in Oxide‐Supported Pt Catalysts for Enhanced Surface Activity and Stability

The catalytic properties of supported metal heterostructures critically depend on the design of metal sites. Although it is well‐known that the supports can influence the catalytic activities of metals, precisely regulating the metal–support interactions to achieve highly active and durable catalysts still remain challenging. Here, the authors develop a support effect in the oxide‐supported metal monomers (involving Pt, Cu, and Ni) catalysts by means of engineering nitrogen‐assisted nanopocket sites. It is found that the nitrogen‐permeating process can induce the reconstitution of vacancy interface, resulting in an unsymmetrical atomic arrangement around the vacancy center. The resultant vacancy framework is more beneficial to stabilize Pt monomers and prevent diffusion, which can be further verified by the density functional theory calculations. The final Pt–N/SnO2 catalysts exhibit superior activity and stability for HCHO response (26.5 to 15 ppm). This higher activity allows the reaction to proceed at a lower operating temperature (100 °C). Incorporated with wireless intelligent‐sensing system, the Pt–N/SnO2 catalysts can further achieve continuous monitoring of HCHO levels and cloud‐based terminal data storage. A nitrogen‐assisted Sn vacancy (N‐VSn) model is developed as an unsymmetrical‐arranged nanopocket to stabilize metal monomers (involving Pt, Cu, and Ni). The final Pt–N/SnO2 catalysts exhibit improved HCHO gas sensing activities (26.5 to 15 ppm) at a lower operating temperature (100 °C) and further achieve wireless monitoring of HCHO.