Single-Walled Cluster Nanotubes for Single-Atom Catalysts with Precise Structures

Abstract

Spatially confining isolated atomic sites in low-dimensional nanostructures is a promising strategy for preparing high-performance single-atom catalysts (SACs). Herein, fascinating polyoxometalate cluster-based single-walled nanotubes (POM-SWNTs) with atomically precise structures, uniform diameter, and single-cluster wall thickness are constructed by lacunary POM clusters (PW₁₁ and P₂W₁₇ clusters). Isolated metal centers are accurately incorporated into the PW₁₁-SWNTs and P₂W₁₇-SWNTs supports. The structures of the resulting MPW₁₁-SWNTs and MP₂W₁₇-SWNTs are well established (M = Cu, Pt). Molecular dynamics simulations demonstrate the stability of POM-SWNTs. Furthermore, the turnover frequency of PtP₂W₁₇-SWNTs is 20 times higher than that of PtP₂W₁₇ cluster units and 140 times higher than that of Pt nanoparticles in the alcoholysis of dimethylphenylsilane. Theoretical studies indicate that incorporating a Pt atom into the P₂W₁₇ support induces straightforward electron transfer between them, combining the nanoconfined environment to enhance the catalytic activity of PtP₂W₁₇-SWNTs. This work shows the feasibility of using subnanometric POM clusters to assemble single-walled cluster nanotubes, highlighting their potential to prepare superior SACs with precise structures.