Pd Nanoparticles on Cu(111)-Supported Ultrathin Ceria Films: Sintering, Alloying, Encapsulation, and Catalytic Activity

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL
Clemens Barth*, 
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Abstract

Metal nanoparticles (NP) on metal-supported cerium oxide (ceria) ultrathin films are important model catalysts for the study of various catalytic reactions. The thermal stability of such systems is of crucial importance as the catalytic NP activity can change due to thermally induced sintering, alloying, and oxide encapsulation of the NPs. Here, it is shown that ultrahigh vacuum (UHV) annealing of PdNPs on ceria/Cu(111) leads to sintering and Pd–Cu alloying, as observed by scanning tunneling microscopy (STM), noncontact atomic force microscopy (nc-AFM), Kelvin probe force microscopy (KPFM), and low energy electron diffraction (LEED): the PdNPs originally grown at room temperature sinter up to a temperature of 673 K to form larger PdNPs. At 773 and 853 K, the NPs increase their volume due to the diffusion of Cu from the Cu(111) support onto the ceria film and into the PdNPs forming bimetallic PdCuNPs. Due to alloying, the catalytic NP activity changes, as observed by KPFM during the water-forming reaction between atomic O and H on the NPs. Especially after annealing at 853 K, the high Cu content deactivates the NPs. Apart from sintering and alloying, annealing between 500 and 700 K leads to a possible encapsulation of the PdNPs with ceria.

Abstract Image

Cu(111)支撑的超薄氧化铈薄膜上的钯纳米粒子:烧结、合金化、封装和催化活性
金属负载氧化铈(ceria)超薄膜上的金属纳米颗粒(NP)是研究各种催化反应的重要模型催化剂。这种体系的热稳定性至关重要,因为NP的催化活性会因NP的热诱导烧结、合金化和氧化物包封而改变。通过扫描隧道显微镜(STM)、非接触原子力显微镜(nc-AFM)、开尔文探针力显微镜(KPFM)和低能电子衍射(LEED)观察到,在ceria/Cu(111)上对PdNPs进行超高真空(UHV)退火导致了烧结和Pd-Cu合金化:最初在室温下生长的PdNPs烧结至673 K,形成更大的PdNPs。在773和853 K时,由于Cu从Cu(111)载体上扩散到氧化铈膜上并进入PdNPs中,形成双金属PdCuNPs, NPs的体积增加。通过KPFM观察到,由于合金化,催化NP活性发生了变化。特别是在853 K退火后,高Cu含量使NPs失活。除了烧结和合金化外,500 - 700 K之间的退火也可能导致PdNPs被铈包裹。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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