Revealing the Deposition Mechanism of the Powder Aerosol Deposition Method Using Ceramic Oxide Core-Shell Particles.

The powder aerosol deposition (PAD) method is a process to manufacture ceramic films completely at room temperature. Since the first reports by Akedo in the late 1990s, much research has been conducted to reveal the exact mechanism of the deposition process. However, it is still not fully understood. This work tackles this challenge using core-shell particles. Two coated oxides, Al2 O3 core with a SiO2 shell and LiNi0.6 Mn0.2 Co0.2 O2 core with a LiNbO3 shell, are investigated. Initially, the element ratios Al:Si and Ni:Nb of the powder are determined by energy-dispersive X-ray spectroscopy (EDX). In a second step, the change in the element ratios of Al:Si and Ni:Nb after deposition is investigated. The element ratios from powder to film strongly shift toward the shell elements, indicating that the particles fracture and only the outer parts of the particles are deposited. In the last step, this work investigates cross-sections of the deposited films with scanning transmission electron microscopy (STEM combined with EDX and an energy-selective back-scattered electron (EsB) detector to unveil the element distribution within the film itself. Therefore, the following overall picture emerges: particles impact on the substrate or on previously deposited particle, fracture, and only a small part of the impacting particles that originate from the outer part of the impacting particle gets deposited.

Functionality based detection of airborne engineered nanoparticles in quasi real time: a new type of detector and a new metric.

A new type of detector which we call the Catalytic Activity Aerosol Monitor (CAAM) was investigated towards its capability to detect traces of commonly used industrial catalysts in ambient air in quasi real time. Its metric is defined as the catalytic activity concentration (CAC) expressed per volume of sampled workplace air. We thus propose a new metric which expresses the presence of nanoparticles in terms of their functionality - in this case a functionality of potential relevance for damaging effects - rather than their number, surface, or mass concentration in workplace air. The CAAM samples a few micrograms of known or anticipated airborne catalyst material onto a filter first and then initiates a chemical reaction which is specific to that catalyst. The concentration of specific gases is recorded using an IR sensor, thereby giving the desired catalytic activity. Due to a miniaturization effort, the laboratory prototype is compact and portable. Sensitivity and linearity of the CAAM response were investigated with catalytically active palladium and nickel nano-aerosols of known mass concentration and precisely adjustable primary particle size in the range of 3-30 nm. With the miniature IR sensor, the smallest detectable particle mass was found to be in the range of a few micrograms, giving estimated sampling times on the order of minutes for workplace aerosol concentrations typically reported in the literature. Tests were also performed in the presence of inert background aerosols of SiO2, TiO2, and Al2O3. It was found that the active material is detectable via its catalytic activity even when the particles are attached to a non-active background aerosol.

An aerosol-process for the synthesis of nanostructured molybdenum oxide catalysts by integrated chemical vapour synthesis/chemical vapour deposition at atmospheric pressure.

We report the synthesis of composite nanoparticles by an integrated CVS/CVD process at atmospheric pressure. Iron oxide and silica support particles were generated by chemical vapour synthesis (CVS), using Fe(CO)5 and Si(OC2H5)4 and were directly coated in the aerosol state with molybdenum oxide by chemical vapour deposition of Mo(CO)6. Depending on the CVS temperature hematite (600 degrees C) or maghemite (1500 degrees C) iron oxide phases were determined by XRD and FTIR. Core-shell structures with a coating thickness in the lower nm range were obtained for CVD temperatures below 150 degrees C. Complete encapsulation of the core particles and uniform elemental distribution is shown by TEM and EELS measurements. Higher CVD temperatures lead to unwanted homogenous decomposition of the molybdenum precursor. Additional aerosol temperature treatment was used to reach further oxidation and the formation of a mixed oxide shell, indicated by FTIR measurements. The results show the potential of the process for the synthesis of structured core-shell nanoparticles.

Experimental Investigation of Aerosol and CO2 Dispersion for Evaluation of COVID-19 Infection Risk in a Concert Hall.

The dispersion of small aerosols in a concert hall is experimentally studied for estimating the risk of infection with SARS-CoV-2 during a concert. A mannequin was modified to emit an air stream containing aerosols and CO2. The aerosols have a size distribution with a peak diameter (δ) close to 0.3 µm and a horizontal initial particle velocity (vp,x) of 2.4 m/s. The CO2-concentration (c) emitted simultaneously is 7500 ppm. It is investigated, if the spatial dissipation of aerosols and CO2 can be correlated. This would allow the use of technically easier CO2 measurements to monitor compliance with aerosol concentration limits. Both aerosol and CO2 concentrations are mapped by different sensors placed around the mannequin. As a result, no significant enrichment of aerosols and CO2 was obtained outside a radius of 1.5 m when the fresh air ventilation in the concert hall has a steady vertical flow with a velocity of vg,z=0.05 m/s and the installed ventilation system was operating at an air change rate per hour (ACH) of 3, corresponding to an air exchange rate of 51,000 m3/h. A Pearson correlation coefficient of 0.77 was obtained for CO2 and aerosol concentrations measured simultaneously at different positions within the concert hall.

Viral aerosol transmission of SARS-CoV-2 from simulated human emission in a concert hall.

The dispersion of aerosols was studied experimentally in several concert halls to evaluate their airborne route and thus the risk of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) spreading. For this, a dummy was used that emits simulated human breath containing aerosols (mean diameter of 0.3 µm) and CO2, with a horizontal exhalation velocity of v = 2.4 m/s, measured 10 cm in front of the mouth. Aerosol and CO2 concentration profiles were mapped using sensors placed around the dummy. No substantial enrichment of aerosols and CO2 was found at adjacent seats, provided that (1) there were floor displacement outlets under each seat enabling a minimum local fresh air vertical flow of vv = 0.05 m/s, (2) the air exchange rate (ACH) was more than 3, and (3) the dummy wore a surgical face mask. Knowledge of dispersion of viral droplets by airborne routes in real environments will help in risk assessment when re-opening concert halls and theatres after a pandemic lockdown.

Film Growth Rates and Activation Energies for Core-Shell Nanoparticles Derived from a CVD Based Aerosol Process.

Silica core-shell nanoparticles of about 60-120 nm with a closed outer layer of bismuth or molybdenum oxide of 1-10 nm were synthesized by an integrated chemical vapor synthesis/chemical vapor deposition process at atmospheric pressure. Film growth rates and activation energies were derived from transmission electron microscopy (TEM) images for a deposition process based on molybdenum hexacarbonyl and triphenyl bismuth as respective coating precursors. Respective activation energies of 123 ± 10 and 155 ± 10 kJ/mol are in good agreement with the literature and support a deposition mechanism based on surface-induced removal of the precursor ligands. Clean substrate surfaces are thus prerequisite for conformal coatings. Integrated aerosol processes are solvent-free and intrinsically clean. In contrast, commercial silica substrate particles were found to suffer from organic residues which hinder shell formation, and require an additional calcination step to clean the surface prior to coating. Dual layer core-shell structures with molybdenum oxide on bismuth oxide were synthesized with two coating reactors in series and showed similar film growth rates.