4.7 Article

In situ exsolution of Co/CoOx core-shell nanoparticles on double perovskite porous nanotubular webs: A synergistically active catalyst for soot efficient oxidation

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 372, Issue -, Pages 752-764

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.04.176

Keywords

Electrospinning; Double perovskite; Porous nanotubular webs; Soot oxidation; Synergistic effects

Funding

  1. National Key Research and Development Program of China [2016YFC0204301]
  2. Natural Science Fund for Colleges and Universities in Jiangsu Province [18KJB530008]
  3. Foundation from State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University [ZK201712]
  4. Research and Innovation Training Project for Graduate in General Universities of Jiangsu Province [SJKY19_1040]

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The PrBa0.5Sr0.5Co0.2Fe1.8O5+delta double perovskite porous nanotubular webs are prepared by a simple electrospinning technique following calcination. It shows better catalytic activity compared with the bulk PrBa0.5Sr0.5Co0.2Fe1.8O5+delta prepared by citrate method, due to its larger specific surface area and higher utilization of active sites. On basis of this, introducing multiple active sites is conducive to enhancing the catalytic activity. In this work, the PrBa0.5Sr0.5Co0.2Fe1.8O5+delta double perovskite porous nanotubular webs are further reduced at 750 degrees C in a 10% H-2/N-2 gas flow, which can give rise to the in situ exsolution of Co core-shell nanoparticles and obtain double active sites. Meanwhile, series of related catalysts are also prepared for comparison, and the physicochemical properties of these catalysts are studied by a lot of characterization techniques. The catalytic performance for soot combustion is evaluated by a temperature programmed oxidation test, which can simulate the soot combustion process. Turn of frequency (TOF) and activation energy (E-a) are calculated by isothermal studies to further evaluate the activity of the as-prepared catalyst. Among all the prepared catalysts, the PrBa0.5Sr0.5Co0.2Fe1.8O5+delta porous nanotubular webs after reductive treatment at 750 degrees C in H-2 atmosphere exhibits the best catalytic activity for soot combustion, showing the lowest activation energy and the highest TOF values. Furthermore, its catalytic activity is significantly promoted compared with the bulk-type catalyst. Firstly, it may be associated with the synergistic effects of sufficient Co core-shell nanoparticles and oxygen vacancies in double perovskite functioned as active sites. Secondly, the structure of porous nanotubular webs can make full use of these active sites.

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