Fire-induced radiological integrated assessment : aerosol characterization

Abstract

This report on detailed aerosol characterization of fire smoke emissions is part of the Fire-Induced Radiological Integrated Assessment (FIRIA; CERN, Switzerland). In this study, carried out at Lund University, a number of materials were combusted in a cone calorimeter at varied heat fluxes. In a few experiments, the effect of reduced O2 content of supply air was investigated (vitiated conditions). The materials included electrical components, magnets, plastic components, oil and cables and were selected due to their high probability of experiencing ionizing radiation in the research facilities at CERN. The aerosol particle yield in the combustion emissions was determined in terms of number and mass emissions. In addition, the particle physical properties in terms of size distributions, the mass - mobility relationship, and the black carbon fraction of emitted particles was determined. Finally, the particle morphology was determined with transmission electron microscopy (TEM) and elemental composition of trace elements by ICP-MS. The total range of aerosol mass yields spanned from approximately 0.005 (g/g fuel) to 0.23 (g/g fuel). Electrical components and magnets were identified as the combustibles with highest mass yields. Mass yields for cables spanned from 0.005-0.09 g/g fuel. The emissions were highly dynamic, with rapid shifts in concentrations and the particle number size distribution as measured with a fast mobility spectrometer (DMS500). The number yields ranged from approximately 0.05*10^14 to 2*10^14 emitted particles per gram of fuel and was measured within the size range 5-1000 nm. The emissions could be parameterized for future modelling applications into nucleation mode particles (with geometric mean diameter that varied between 20-50 nm) and accumulation mode particles (with geometric mean diameter 100-230 nm). The aerosol mass yields were governed primarily by the concentration and size distribution of accumulation mode particles. Mass yields were determined from 1) Impactor measurements (Dekati Gravimetric Impactor) and 2) Simultaneous measurements of the electrical mobility size distribution (DMS500) and effective density distribution (DMA-APM). The general agreement between the two techniques was good (R2=0.93). Black carbon is indicative of refractory carbonaceous particles which form in fuel rich conditions of the hot flame environment and associated with the black color of soot (smoke). Black carbon yields were for most experiments similar to the derived mass yields. TEM images showed typical refractory black carbon aggregates at high BC fractions. The primary particle size was larger than for diesel exhaust. However, at reduced heat flux and during vitiated combustion (reduced O2 concentration), black carbon yields were sometimes much lower than the derived particle mass yields. TEM analysis for a sample with low BC fraction showed only very few particles and those that were found had distinctly different properties to the high BC fraction sample. We hypothesize that particles emitted under these conditions were dominated by low volatility organic matter formed in the pyrolysis of the materials. Such components were likely co-emitted with black carbon also in conventional experiments, although in minor mass fractions. Based on previous studies it can be hypothesized that H:C ratios are low for the cases with high BC fraction

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