Engineering Low-Coordinated Pt Sites through Supported Polyhedral Nanoparticles for Enhanced Low-Temperature Toluene Catalytic Oxidation.

Zhang, Xiangwei; Chen, Qingze; Fu, Haoyang; Liu, Peng; Xie, Jieyang; Geng, Xun; Lei, Zhihao; Li, Shuzhou et al. · Nano Lett · 2025

basic_science · Level V

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Abstract

Engineering low-coordinated Pt sites represents a promising strategy to boost catalysis, yet their precise control to optimize structure-activity relationships for volatile organic compounds oxidation remains challenging. Herein, we achieved abundant low-coordinated Pt sites by constructing highly dispersed and well-defined polyhedral Pt nanoparticles on a porous silica support (Pt-APSiO<sub>2</sub>) for toluene oxidation. The amino-functionalized silica provides coordination environments for [PtCl<sub>6</sub>]<sup>2-</sup> precursors that regulate the reduction kinetics to favor polyhedral morphology formation. The resulting Pt-APSiO<sub>2</sub> catalyst showed exceptional performance in toluene oxidation with an extremely low <i>T</i><sub>90</sub> of 148 °C. Structural characterization revealed that the polyhedral Pt nanoparticles possessed a reduced coordination number of 7.38, leading to an upward shift in the d-band center to -1.88 eV. This shifts endowed Pt sites with stronger adsorption and activation for both toluene and O<sub>2</sub>. This work demonstrates the feasibility of morphology-directed synthesis for tailoring active site coordination environments, advancing rational design principles for environmental catalysis.