Effect of Pt precursor on structure and performance of Pt/CeO<sub>2</sub> catalysts

Kang XI; Yong WANG; Jing XIE; Ning WANG; Ying ZHOU; Qiulian ZHU; Hanfeng LU

doi:10.11949/0438-1157.20190468

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Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts

Catalysis, kinetics and reactors | 更新时间：2020-06-24

- Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts
- CIESC Journal Vol. 70, Issue 11, Pages: 4278-4288(2019)
- 作者机构：
  
  浙江工业大学化学工程学院，浙江杭州 310014
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20190468
  CLC： TQ 133.3;TQ 138.2⁺6
- Received：06 May 2019，
  
  Revised：2019-06-15，
  
  Published：05 November 2019
- 稿件说明：
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席康, 王勇, 谢晶, 王宁, 周瑛, 朱秋莲, 卢晗锋. 不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响[J]. 化工学报, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468.

XI Kang, WANG Yong, XIE Jing, WANG Ning, ZHOU Ying, ZHU Qiulian, LU Hanfeng. Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts[J]. CIESC Journal, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468.
席康, 王勇, 谢晶, 王宁, 周瑛, 朱秋莲, 卢晗锋. 不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响[J]. 化工学报, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468. DOI：

XI Kang, WANG Yong, XIE Jing, WANG Ning, ZHOU Ying, ZHU Qiulian, LU Hanfeng. Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts[J]. CIESC Journal, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468. DOI：

摘要

Pt与载体间的相互作用会影响到本征Pt纳米粒子的催化活性，不同Pt前体制备Pt/CeO

催化剂会使其表现出完全不同的催化性能。分别采用金属胶体粒子原位沉积法、浸渍法以及浸渍还原的方式制备了Pt/CeO

催化剂，通过X 射线衍射、程序升温还原、X射线光电子能谱以及高分辨透射电镜对催化剂进行表征，在CO氧化以及甲苯燃烧反应中评价催化剂活性。结果表明，胶体粒子原位沉积法制备Pt/CeO

催化剂，能够将优先合成好的Pt纳米粒子直接以金属态Pt

的形式负载到载体表面，且保证其高度均匀分散，丰富的表面Pt

很好地充当了CO、甲苯反应时的活化位点，催化剂表现出优异的性能；浸渍还原法中，Pt纳米粒子之间会发生团聚现象，同时部分Pt又以Pt

的形式与CeO

之间形成了Pt-O-Ce相互作用，载体表面暴露Pt

含量的下降是催化剂表现出较弱活性的主要原因；浸渍法中，以Pt离子对Pt进行负载，Pt完全以Pt

的形式参与到Pt-O-Ce键成键中，表面Pt

缺失，催化剂表现出明显的失活现象。Pt/CeO

催化剂中，起主要活性作用的是金属态Pt

，胶体粒子原位沉积法能够实现Pt

的直接负载，对于提高Pt基催化剂中Pt的利用率，降低Pt资源消耗都具有重要意义。

Abstract

The interaction between Pt and the carrier affects the catalytic activity of the intrinsic Pt nanoparticles. Herein

Pt/CeO

catalyst was successfully prepared

via

a facile Pt colloidal particle deposition method

and its physicochemical properties and catalytic performance in CO oxidation and toluene combustion were investigated. XRD

TEM

XPS and H

-TPR were used to identify the states of Pt particles on the support surface

as well as their effect on the performance of the catalysts. Formation of metallic Pt

which provided the active sites for CO oxidation and toluene combustion is one of the factors controlling catalyst activity. Pt/CeO

catalyst prepared by colloidal particle deposition was found to be more advantageous than conventional impregnation and impregnation-reduction in producing very finely dispersed metallic Pt

that did not noticeably agglomerate even after thermal treatment at 400℃ for longer duration. The CO oxidation and toluene combustion activity additionally demonstrate that the sample shows a remarkably better performance as compared to its impregnated counterparts. By contrast

all of Pt atoms were anchored with the surface oxygen of CeO

by forming Pt-O-Ce bond during the oxidative treatment in impregnation method

resulting in the absence of metallic Pt

. This change is evidence of the appearance of Pt

species

which is supported by the H

-TPR and XPS data

and could be the main reason behind the deactivation of the Pt/CeO

catalyst. Compared with impregnation method

the dispersion of metallic Pt

rised while less Pt-O-Ce bonds existed on the support surface

and a higher Pt

/Pt

ratio could be maintained even under the high thermal treatment in impregnation reduction method. The catalytic activity test of CO oxidation and toluene combustion show that the sample exhibits the better catalytic performance due to the increase of surface metallic Pt

but it is unavoidable for the sample to show a decline in catalytic activity compared with its colloidal particle depositional counterpart. Hence

it is concluded that the state and the dispersion of Pt nanoparticles on the support surface depended on the prepared method

and they are the decisive factors to promote the catalytic activity of Pt/CeO

upon the oxidative treatment

especially the abundant surface metallic Pt

. Based on characterization results

the colloidal particle deposition method is proposed to realize the direct load of metallic Pt

and gives the homogeneous dispersion of Pt nanoparticles

possessing a superiority in improving the catalytic performance.

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Keywords

references

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⁰

Effect of Pt precursor on structure and performance of Pt/CeO2 catalysts

DOI：10.11949/0438-1157.20190468

摘要

Abstract

关键词

Keywords

references

Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts