Flame emission spectroscopy of single droplet micro explosions†

IF 8 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Jan Derk Groeneveld, Suman Pokhrel and Lutz Mädler
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Abstract

Nanoparticles exhibit superior physical and chemical properties, making them highly desirable for various applications. Flame spray pyrolysis (FSP) is a versatile technique for synthesizing size and composition-controlled metal oxide/sulfide nanoparticles through a gas-phase reaction. To understand the fundamental mechanisms governing nanoparticle formation in FSP, simplified single-droplet experiments have proven to unravel the physicochemical mechanisms of liquid metal precursor combustions. This work introduces a novel method using flame emission spectroscopy and high-speed imaging to analyze combustion species and metal release during metalorganic single droplet combustions, with the example of the 2-ethylhexanoci acid (EHA)–tetrahydrothiophene (THT)–mesitylcopper (MiCu) precursor system. The method enables the tracing of precursor components released from droplet into the flame by spatial and temporal resolved emission tracking from combustion species (OH*, CH*, C2*, CS*, CS2*) and atomic spectral lines (Cu I). The tracking of metal emission enables the direct observation of the particle formation route, offering novel insights into the metalorganic precursor combustions. The findings of this work show a direct correlation between micro-explosions and nanoparticle formation through the gas-to-particle route. The release of copper emissions is observed with the micro-explosion event, marking the micro-explosions as the critical mechanism for the metal release and subsequent nanoparticle formation during the combustion process. The results indicate a metalorganic viscous shell formation (THT + MiCu) leading to the micro explosion. The EHA/THT ratio significantly affects the combustion behavior. Lower ratios lead to a gradual copper release before the micro explosion; higher ratios shorten the copper release and delay the micro explosion – the highest ratio results in two distinct burning stages.

Abstract Image

单液滴微爆炸的火焰发射光谱分析
纳米粒子具有优异的物理和化学特性,因此在各种应用中都非常受欢迎。火焰喷射热解(FSP)是一种通过气相反应合成尺寸和成分可控的金属氧化物/硫化物纳米粒子的多功能技术。为了解 FSP 中纳米粒子形成的基本机制,简化的单液滴实验已被证明可以揭示液态金属前驱体燃烧的物理化学机制。本研究以 2-乙基己酸(EHA)-四氢噻吩(THT)-中性铜(MiCu)前驱体体系为例,介绍了一种利用火焰发射光谱和高速成像分析金属有机单液滴燃烧过程中燃烧物种类和金属释放的新方法。该方法可通过对燃烧物(OH*、CH*、C2*、CS*、CS2*)和原子光谱线(Cu I)的时空分辨发射追踪,追踪从液滴释放到火焰中的前体成分。通过对金属发射的跟踪,可以直接观察颗粒的形成过程,从而对金属有机前体燃烧有新的认识。这项工作的研究结果表明,微爆炸和纳米粒子的形成通过气体到粒子的途径直接相关。在微爆炸事件中观察到铜的释放,这表明微爆炸是燃烧过程中金属释放和随后纳米粒子形成的关键机制。结果表明,金属有机粘壳的形成(THT+MiCu)导致了微爆。EHA/THT 比率对燃烧行为有很大影响。较低的比率会导致铜在微爆炸前逐渐释放;较高的比率会缩短铜的释放时间并延迟微爆炸--最高比率会导致两个不同的燃烧阶段。
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来源期刊
Nanoscale Horizons
Nanoscale Horizons Materials Science-General Materials Science
CiteScore
16.30
自引率
1.00%
发文量
141
期刊介绍: Nanoscale Horizons stands out as a premier journal for publishing exceptionally high-quality and innovative nanoscience and nanotechnology. The emphasis lies on original research that introduces a new concept or a novel perspective (a conceptual advance), prioritizing this over reporting technological improvements. Nevertheless, outstanding articles showcasing truly groundbreaking developments, including record-breaking performance, may also find a place in the journal. Published work must be of substantial general interest to our broad and diverse readership across the nanoscience and nanotechnology community.
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