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

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-10-02 DOI:10.1021/acs.nanolett.5c04170

Xiangwei Zhang,Qingze Chen,Haoyang Fu,Peng Liu,Jieyang Xie,Xun Geng,Zhihao Lei,Shuzhou Li,Runliang Zhu

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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-APSiO2) for toluene oxidation. The amino-functionalized silica provides coordination environments for [PtCl6]2- precursors that regulate the reduction kinetics to favor polyhedral morphology formation. The resulting Pt-APSiO2 catalyst showed exceptional performance in toluene oxidation with an extremely low T90 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 O2. This work demonstrates the feasibility of morphology-directed synthesis for tailoring active site coordination environments, advancing rational design principles for environmental catalysis.

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通过负载多面体纳米颗粒工程低协调Pt位点增强低温甲苯催化氧化。

工程低协调Pt位点代表了一种很有前途的促进催化的策略，但它们的精确控制优化挥发性有机化合物氧化的结构-活性关系仍然具有挑战性。在这里，我们通过在多孔二氧化硅载体（Pt- apsio2）上构建高度分散和定义明确的多面体Pt纳米颗粒来获得丰富的低配位Pt位点。氨基功能化二氧化硅为[PtCl6]2-前驱体提供了配位环境，调节还原动力学，有利于多面体形态的形成。所制得的Pt-APSiO2催化剂表现出优异的甲苯氧化性能，T90极低，为148℃。结构表征表明，多面体Pt纳米粒子的配位数降低了7.38，导致d波段中心向上移动至-1.88 eV。这种转变使Pt位点对甲苯和O2具有更强的吸附和活化作用。这项工作证明了形态定向合成用于裁剪活性位点协调环境的可行性，为环境催化提出了合理的设计原则。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.