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通过 CO 活化增强原子分散 Pt/CeO 催化剂的催化氧化反应活性。

Enhanced Catalytic Oxidation Reactivity over Atomically Dispersed Pt/CeO Catalysts by CO Activation.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China.

出版信息

Environ Sci Technol. 2024 Jul 9;58(27):12201-12211. doi: 10.1021/acs.est.4c02022. Epub 2024 Jun 27.

DOI:10.1021/acs.est.4c02022
PMID:38934498
Abstract

The elevation of the low-temperature oxidation activity for Pt/CeO catalysts is challenging to meet the increasingly stringent requirements for effectively eliminating carbon monoxide (CO) from automobile exhaust. Although reducing activation is a facile strategy for boosting reactivity, past research has mainly concentrated on applying H as the reductant, ignoring the reduction capabilities of CO itself, a prevalent component of automobile exhaust. Herein, atomically dispersed Pt/CeO was fabricated and activated by CO, which could lower the 90% conversion temperature () by 256 °C and achieve a 20-fold higher CO consumption rate at 200 °C. The activated Pt/CeO catalysts showed exceptional catalytic oxidation activity and robust hydrothermal stability under the simulated working conditions for gasoline or diesel exhausts. Characterization results illustrated that the CO activation triggered the formation of a large portion of Pt terrace sites, acting as inherent active sites for CO oxidation. Besides, CO activation weakened the Pt-O-Ce bond strength to generate a surface oxygen vacancy (V). It served as the oxygen reservoir to store the dissociated oxygen and convert it into active dioxygen intermediates. Conversely, H activation failed to stimulate V, but triggered a deactivating transformation of the Pt nanocluster into inactive PtO in the presence of oxygen. The present work offers coherent insight into the upsurging effect of CO activation on Pt/CeO, aiming to set up a valuable avenue in elevating the efficiency of eliminating CO, CH, and NH from automobile exhaust.

摘要

提高低温氧化活性对于满足日益严格的汽车尾气中有效消除一氧化碳 (CO) 的要求具有挑战性。虽然降低活性是提高反应性的一种简便策略,但过去的研究主要集中在使用 H 作为还原剂,而忽略了 CO 本身作为汽车尾气中常见成分的还原能力。本文通过 CO 来制备和激活原子分散的 Pt/CeO,这可以将 90%转化率温度 () 降低 256°C,并在 200°C 下实现 20 倍更高的 CO 消耗速率。在模拟的汽油或柴油废气工作条件下,激活的 Pt/CeO 催化剂表现出优异的催化氧化活性和强的水热稳定性。表征结果表明,CO 激活引发了大量 Pt 平台位的形成,作为 CO 氧化的固有活性位。此外,CO 激活削弱了 Pt-O-Ce 键的强度,产生表面氧空位 (V)。它充当氧储库,储存解离的氧,并将其转化为活性的双氧中间物。相反,H 激活未能刺激 V 的产生,但在有氧存在的情况下,会引发 Pt 纳米团簇向非活性 PtO 的失活转变。本工作为 CO 激活对 Pt/CeO 的增强效应提供了一致的见解,旨在为提高汽车尾气中 CO、CH 和 NH 的消除效率开辟一条有价值的途径。

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