Time-resolved size and element analysis of gas-borne nanoparticles
Physical and chemical characterization of gas-borne particles in the nanometer to sub-micrometer size range is important in many applications, such as nanoparticle related health studies, the monitoring of powder or dust distribution processes, assessing the release of engineered nanoparticles (ENP) from ENP reinforced materials due to abrasion or combustion, or exposure studies related to ENP containing spray products. Such investigations are also highly valuable in the development of technical processes, e.g. to determine distinct size fractions containing specific elements or isotopes in terms of dealing with nuclear waste, or to evaluate particulate matter in process gases and emissions from thermal waste treatment, gas turbines, or other combustion engines. Such particle speciation includes knowledge about particle size distribution and chemical composition, and if possible obtained with a high time resolution. However, most of the available techniques are offline methods and/or not able to provide such physical and chemical information simultaneously. The Scanning Mobility Particle Sizer (SMPS) is a well-established and widely used equipment for determining size distribution and number concentration of such particles, within scan durations of a few minutes. Inductively Coupled Plasma Mass Spectrometry (ICPMS) is a highly sensitive multi-element technique, which allows determining the elemental composition of normally liquid samples, with excellent detection limits and a wide dynamic concentration range. In this work, SMPS and ICPMS are coupled to one hyphenated system. A Rotating Disk Diluter (RDD) allows directing a well-defined flow of a diluted aerosol into subsequent measuring equipment, which besides is mainly argon based, due to the dilution effect. Therefore an RDD is implemented as sample introduction interface, and the SMPS flow concept is re-designed to fulfil the requirements of both different analytical methods. This coupling strategy allows achieving simultaneous information on particle size and elemental composition, with SMPS-typical time resolutions of a few minutes, and offers high flexibility in terms of dealing with different aerosols, loaded with particles in the nanometer to sub-micrometer size range. Proper SMPS operation under argon atmosphere instead of air is validated. The developed setup is tested with a model aerosol containing air-borne silver nanoparticles. The capabilities are then demonstrated on uniformly composited metal aerosols, as well as an aerosol mixture containing smaller gold and larger silver nanoparticles. Sensitivity and limit of detection, related to particle number and mass concentration, are determined for several elements and particle diameters. After the successful characterization, the instrumentation is applied in two research applications. The first is a study on aerosol particles, released by commercial consumer spray products. In the second application, particulate metal emissions from the thermal treatment of differently impregnated wood samples are investigated, with the focus on alkali metals.
Programme doctoral Sciences et Génie des matériaux
Faculté de l'environnement naturel, architectural et construit
Institut d'ingénierie de l'environnement
Jury: Prof. Anna Fontcuberta i Morral (présidente) ; Prof. Christian Ludwig (directeur de thèse) ; Prof. Satoshi Takahama, Dr Markus Kasper, Prof. Dainius Martuzevicius (rapporteurs)
Public defense: 2016-4-11
Record created on 2016-04-06, modified on 2016-08-09