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通过氢气处理促进Pt/CeO催化剂用于低温CO氧化

Promotion of Pt/CeO catalyst by hydrogen treatment for low-temperature CO oxidation.

作者信息

Jan Asif, Shin Jisu, Ahn Junsung, Yang Sungeun, Yoon Kyung Joong, Son Ji-Won, Kim Hyoungchul, Lee Jong-Ho, Ji Ho-Il

机构信息

Center for Energy Materials Research, Korea Institute of Science and Technology (KIST) Seoul 02792 Republic of Korea

Nanomaterials Science and Engineering, Korea University of Science and Technology (UST) KIST Campus Seoul 02792 Republic of Korea.

出版信息

RSC Adv. 2019 Aug 28;9(46):27002-27012. doi: 10.1039/c9ra05965b. eCollection 2019 Aug 23.

Abstract

Low temperature CO oxidation reaction is known to be facilitated over platinum supported on a reducible cerium oxide. Pt species act as binding sites for reactant CO molecules, and oxygen vacancies on surface of cerium oxide atomically activate the reactant O molecules. However, the impacts of size of Pt species and concentration of oxygen vacancy at the surface of cerium oxide on the CO oxidation reaction have not been clearly distinguished, thereby various diverse approaches have been suggested to date. Here using the co-precipitation method we have prepared pure ceria support and infiltrated it with Pt solution to obtain 0.5 atomic% Pt supported on cerium oxide catalyst, and then systematically varied the size of Pt from single atom to ∼1.7 nm sized nanoparticles and oxygen vacancy concentration at surface of cerium oxide by controlling the heat-treatment conditions, which are temperature and oxygen partial pressure. It is found that Pt nanoparticles in range of 1-1.7 nm achieve 100% of CO oxidation reaction at ∼100 °C lower temperature compared to Pt single atom owing to the facile adsorption of CO but weaker binding strength between Pt and CO molecules, and the oxygen vacancy in the vicinity of Pt accelerates CO oxidation below 150 °C. Based on this understanding, we show that a simple hydrogen reduction at 550 °C for the single atom Pt supported on CeO catalyst induces the formation of highly dispersed Pt nanoparticles with size of 1.7 ± 0.2 nm and the higher concentration of surface oxygen vacancies simultaneously, enabling 100% conversion from CO to CO at 200 °C as well as 16% conversion even at 150 °C owing to the synergistic effects of Pt nanoparticles and oxygen vacancies.

摘要

低温CO氧化反应已知在负载于可还原氧化铈上的铂上更容易发生。铂物种作为反应物CO分子的结合位点,氧化铈表面的氧空位以原子方式活化反应物O分子。然而,铂物种的尺寸和氧化铈表面氧空位浓度对CO氧化反应的影响尚未得到明确区分,因此迄今为止已提出了各种不同的方法。在这里,我们使用共沉淀法制备了纯氧化铈载体,并用铂溶液对其进行浸渍,以获得负载在氧化铈催化剂上的0.5原子%的铂,然后通过控制热处理条件(温度和氧分压),系统地改变铂的尺寸,从单原子到约1.7 nm大小的纳米颗粒,以及氧化铈表面的氧空位浓度。结果发现,与铂单原子相比,1-1.7 nm范围内的铂纳米颗粒由于CO的吸附容易但铂与CO分子之间的结合强度较弱,在约低100°C的温度下实现了100%的CO氧化反应,并且铂附近的氧空位在150°C以下加速了CO氧化。基于这一认识,我们表明,对负载在CeO催化剂上的单原子铂在550°C进行简单的氢还原,会同时诱导形成尺寸为1.7±0.2 nm的高度分散的铂纳米颗粒和更高浓度的表面氧空位,由于铂纳米颗粒和氧空位的协同作用,在200°C时能够实现CO到CO₂的100%转化,甚至在150°C时也能实现16%的转化。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d9e/9070415/49e9560f25a6/c9ra05965b-f1.jpg

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