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新型氧化铈-氧化铝负载高活性和高稳定性钯催化剂在一氧化碳和碳氢化合物氧化反应中的应用。

Highly Active and Stable Palladium Catalysts on Novel Ceria-Alumina Supports for Efficient Oxidation of Carbon Monoxide and Hydrocarbons.

机构信息

Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States.

College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, China.

出版信息

Environ Sci Technol. 2021 Jun 1;55(11):7624-7633. doi: 10.1021/acs.est.1c00077. Epub 2021 Apr 19.

Abstract

Precious metal catalysts with superior low-temperature activity and excellent thermal stability are highly needed in environmental catalysis field. In this work, a novel two-step incipient wetness impregnation (T-IWI) method was developed for the fabrication of a unique and highly stable CeO/AlO support (CA-T). Pd anchored on CA-T exhibited a much higher low-temperature catalytic activity and superior thermal stability in carbon monoxide (CO) and hydrocarbon (HC) oxidations, compared to Pd anchored on conventional CeO/AlO (CA), which was prepared by a one-step IWI method. After aging treatment at 800 °C, the CO oxidation rate on Pd/CA-T (1.69 mmol/(g s)) at 120 °C was 4.1 and 84.5 times of those on Pd/CA (0.41 mmol/(g s)) and Pd/AlO (0.02 mmol/(g s)), respectively. It was revealed that the CA-T support with well-controlled small CeO particles ( 12 nm) possessed abundant defects for Pd anchoring, which created rich Pd-CeO interfaces with strengthened interaction between Pd and CeO where oxygen could be efficiently activated. This resulted in the significantly improved oxidation activity and thermal stability of Pd/CA-T catalysts. The T-IWI method developed herein can be applied as a universal approach to prepare highly stable metal oxide-alumina-based supports, which have broad application in environmental catalyst design, especially for automobile exhaust aftertreatment.

摘要

在环境催化领域,非常需要具有优越低温活性和优异热稳定性的贵金属催化剂。在这项工作中,开发了一种新颖的两步初始湿浸渍(T-IWI)方法,用于制备独特且高度稳定的 CeO/AlO 载体(CA-T)。与通过一步 IWI 方法制备的传统 CeO/AlO(CA)上负载的 Pd 相比,负载在 CA-T 上的 Pd 在一氧化碳(CO)和碳氢化合物(HC)氧化中表现出更高的低温催化活性和更好的热稳定性。在 800°C 老化处理后,在 120°C 下,Pd/CA-T(1.69 mmol/(g s))的 CO 氧化速率分别是 Pd/CA(0.41 mmol/(g s))和 Pd/AlO(0.02 mmol/(g s))的 4.1 和 84.5 倍。结果表明,具有良好控制的小 CeO 颗粒( 12nm)的 CA-T 载体具有丰富的 Pd 锚定位点,形成了富含 Pd-CeO 界面的丰富结构,增强了 Pd 和 CeO 之间的相互作用,从而可以有效地激活氧。这导致 Pd/CA-T 催化剂的氧化活性和热稳定性得到显著提高。所开发的 T-IWI 方法可以作为一种通用方法来制备高度稳定的金属氧化物-氧化铝基载体,在环境催化剂设计中具有广泛的应用前景,特别是在汽车尾气后处理中。

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