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原子层状WO 岛负载的铂:用于高效低温挥发性有机化合物燃烧的铂 - 钨异质结构的电子调控

Pt on Atomic-Layered WO Islands: Electronic Tuning of Platinum-Tungsten Heterostructures for Highly Efficient Low-Temperature VOC Combustion.

作者信息

Ni Jiangwei, Huang Zhiwei, Tian Mingshuo, Chen Wen, Zhou Qiqi, Gong Juanjuan, Liao Xinlong, Chen Junhong, Gan Shuangning, Chen Jia, Wu Xiaomin, Shen Huazhen, Zhao Huawang, Jing Guohua

机构信息

Department of Environmental Science & Engineering, College of Chemical Engineering, Huaqiao University, Xiamen 361021, Fujian, China.

出版信息

Environ Sci Technol. 2024 Apr 23;58(16):7020-7031. doi: 10.1021/acs.est.4c00123. Epub 2024 Apr 12.

Abstract

Adjusting the electronic state of noble metal catalysts on a nanoscale is crucial for optimizing the performance of nanocatalysts in many important environmental catalytic reactions, particularly in volatile organic compound (VOC) combustion. This study reports a novel strategy for optimizing Pt catalysts by modifying their electronic structure to enhance the electron density of Pt. The research illustrates the optimal 0.2Pt-0.3W/FeO heterostructure with atomic-thick WO layers as a bulking block to electronically modify supported Pt nanoparticles. Methods such as electron microscopy, X-ray photoelectron spectroscopy, and in situ Fourier transform infrared spectroscopy confirm Pt's electron-enriched state resulting from electron transfer from atomic-thick WO. Testing for benzene oxidation revealed enhanced low-temperature activity with moderate tungsten incorporation. Kinetic and mechanistic analyses provide insights into how the enriched electron density benefits the activation of oxygen and the adsorption of benzene on Pt sites, thereby facilitating the oxidation reaction. This pioneering work on modifying the electronic structure of supported Pt nanocatalysts establishes an innovative catalyst design approach. The electronic structure-performance-dependent relationships presented in this study assist in the rational design of efficient VOC abatement catalysts, contributing to clean energy and environmental solutions.

摘要

在纳米尺度上调节贵金属催化剂的电子态对于优化纳米催化剂在许多重要环境催化反应中的性能至关重要,尤其是在挥发性有机化合物(VOC)燃烧中。本研究报告了一种通过修饰Pt催化剂的电子结构以提高其电子密度来优化Pt催化剂的新策略。该研究表明,以原子级厚度的WO层作为增厚块的最佳0.2Pt-0.3W/FeO异质结构可对负载的Pt纳米颗粒进行电子修饰。电子显微镜、X射线光电子能谱和原位傅里叶变换红外光谱等方法证实了由于原子级厚度的WO发生电子转移而导致Pt处于富电子状态。苯氧化测试表明,适度掺入钨可提高低温活性。动力学和机理分析揭示了富电子密度如何有利于氧的活化以及苯在Pt位点上的吸附,从而促进氧化反应。这项关于修饰负载型Pt纳米催化剂电子结构的开创性工作建立了一种创新的催化剂设计方法。本研究中提出的电子结构-性能依赖关系有助于合理设计高效的VOC减排催化剂,为清洁能源和环境解决方案做出贡献。

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