The initial stages of multicomponent particle formation during the gas phase combustion synthesis of mixed SiO2/TiO2

The ability to properly scale the synthesis of advanced materials through combustion synthesis routes is limited by our lack of knowledge regarding the initial stages of particle formation. In flame aerosol reactors, the high temperatures, fast reaction rates, and flame chemistry can all play a critical role in determining the properties of the resulting nanomaterials. In particular, multicomponent systems pose a unique challenge as most studies rely on empirical approaches toward designing advanced composite materials. The lack of predictive capabilities can be attributed to a lack of data on particle inception and growth below 2nm. Measurements for the initial stages of particle formation during the combustion synthesis of SiO2 and composite SiO2/TiO2 using an atmospheric pressure inlet time-of-flight mass spectrometer are presented. Both positively and negatively charged clusters can be measured and results show the presence of silicic acid species which grow through dehydration, hydrogen abstraction, and interactions with hydroxyl radicals. In the case of composite SiO2/TiO2 particle formation, new molecular species containing Ti atoms emerge. Tandem differential mobility analysis-mass spectrometry (DMA-MS) provided further insight into the size-resolved chemistry of particle formation to reveal that at each cluster size, further hydroxyl-driven reactions take place. From this we can conclude that previous assumptions on collisional growth from simple monomer species of SiO2 and TiO2 do not sufficiently describe the collisional growth mechanisms for particle growth below 2nm.Copyright (c) 2018 American Association for Aerosol Research