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Early particle formation and evolution in iron-doped flames

机译:Early particle formation and evolution in iron-doped flames

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摘要

? 2022In flame synthesis of nanoparticles, the temperature history experienced by the nascent particle aerosol defines the morphology, composition, and crystallinity of the resulting nanomaterial. Commonly, flame-synthesis processes are modeled with an isothermal approximation assuming that the particle temperature replicates that of the surrounding gas phase, avoiding inclusion of an additional internal coordinate in the population balance model, and thus reducing the computational cost. This simplification neglects the influence of matter- and energy-exchange as well as thermochemistry between the particle and reactive gas phase, impacting the particle temperature. In this work, we investigate the temperature history of the particles in incipient formation stages and their evolution in iron-doped flames, prototypical for many other transition-metal (oxide) synthesis systems. The temperature and relative volume-fraction distributions of early particles forming in H2/O2/Ar flames doped with iron pentacarbonyl were determined for the first time, based on spectrally and spatially resolved flame emission measurements and pyrometric analysis of the continuum emission emanating from the nascent particle aerosol. The nascent particle temperature was found to be several hundred degrees above the gas-phase temperature for all physically reasonable assumptions concerning particle composition and emission efficiency. Early particles volume fraction rises sharply shortly after the decomposition of iron pentacarbonyl and decreases steeply in the flame front, in excellent agreement with previous particle-mass spectrometry/quartz-crystal microbalance measurements. By modeling the evaporation process of isothermal iron particles, we show that vanishing of particles in the flame front cannot be explained by evaporation of particles that are in thermal equilibrium with the gas phase. A single-particle Monte-Carlo simulation based on a simple model comprising Fe-monomer condensation, concurrent with oxidation, reduction, etching, and evaporation occurring at the particle surface, captures both the flame structure with respect to early particle formation and their excess temperature compared to the gas phase.

著录项

  • 来源
    《Combustion and Flame》 |2022年第10期|1-19|共19页
  • 作者单位

    Department of Natural Sciences The Open University of Israel;

    IVG Institute for Combustion and Gas Dynamics – Fluid Dynamics University of Duisburg-Essen;

    IVG Institute for Combustion and Gas Dynamics – Fluid Dynamics University of Duisburg-EssenIVG Institute for Combustion and Gas Dynamics – Fluid Dynamics University of Duisburg-Essen||CENIDE Center for Nanointegration Duisburg?Essen University of DuisburgIVG Institute for Combustion and Gas Dynamics – Reactive Fluids University of Duisburg-EssenIVG Institute for Combustion and Gas Dynamics – Reactive Fluids University of Duisburg-Essen||CENIDE Center for Nanointegration Duisburg?Essen University of Duisburg-EssenSchool of Chemistry Sackler Faculty of Exact Sciences Tel Aviv University;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 英语
  • 中图分类
  • 关键词

    Emission; Flame structure; Iron oxide; Material synthesis; Nanoparticles; Temperature history;

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