APLICACIÓN DEL SISTEMA TANDEM DMA-MS AL ANÁLISIS ATMOSFÉRICO
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1 APLICACIÓN DEL SISTEMA TANDEM DMA-MS AL ANÁLISIS ATMOSFÉRICO TANDEM DMA-MS SYSTEM APPLICATION TO ATMOSPHERIC ANALYSIS ARTURO ÁLVARO CARBALLIDO 1,2, DAOIZ ZAMORA PÉREZ 1, GONZALO FERNANDEZ DE LA MORA 1 1 Sociedad Europea de Análisis Diferencial de Movilidad, 2 Universidad de Valladolid arturo.alvaro@seadm.com Atmospheric aerosols 1
2 INDEX Introduction: Brief description of the application and the device The problem addressed: Existence of background contaminants at ppq Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Increase mobility resolution via polar dopants addition Mass discrimination approach Conclusions Atmospheric aerosols 2
3 Introduction: Brief description of the application and the device The application: Explosive screening on cargo through vapours and suspended particles collection Sample collection & preconcentration Sample Analysis Adsorbed sample Atmospheric aerosols 3
4 Introduction: Brief description of the application and the device The device: Preconcentrator (Adsorption/desorption), Mobility analyzer, mass spectrometer. Channel definition: Fixed volatility, size, mass and mass fragment. Sampler Adsorbent Thermal desorber LFSESI Ionization DMA Triple Quadrupole MS^2 Atmospheric aerosols 4
5 INDEX Introduction: Brief description of the application and the device The problem addressed: Existence of background contaminants at ppq Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Increase mobility resolution via polar dopants addition Mass discrimination approach Conclusions Atmospheric aerosols 5
6 Required sensitivity Available sensitivity The problem addressed: Existence of background contaminants at ppq 0.1ppq= atm 1000l 0.1ppq = molecules A moth can detect 1 pheromone molecule! Interferent substances abundance: 0.1-1ppq THE REAL PROBLEM IS TO ACHIEVE VERY HIGH RESOLUTION! Atmospheric aerosols 6
7 The problem addressed: Existence of background contaminants at ppq Abundance data of interferent substances on four explosive channels in cargo containers: Atmospheric aerosols 7
8 ppq ppq ppq The problem addressed: Existence of background contaminants at ppq Abundance data of interferent substances on three explosive channels in Spanish Airports atmosphere: 1,50 1,00 0,50 0,00 NG 0,20 0,15 0,10 0,05 0,00 TNT 0,040 0,030 0,020 0,010 0,000 RDX WHAT ARE THESE INTERFERING SIGNALS? THE REAL EXPLOSIVE? SOMETHING ELSE? Atmospheric aerosols 8
9 INDEX Introduction: Brief description of the application and the device The problem addressed: Existence of background contaminants at ppq Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Increase mobility resolution via polar dopants addition Mass discrimination approach Conclusions Atmospheric aerosols 9
10 Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Gaussian deconvolution Average contaminants reduction in atmospheric samples [average ppq] EGDN NG PETN RDX TNT Average samples without deconvolution Average samples with deconvolution Average Ratio improvement 76% 93% 83% 85% 5% Atmospheric aerosols 10
11 ppq Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Effect of deconvolution: NG in ambient air Removal of isomers Reduction of interferent signals Reduction of variability (Place, time, season & temperature effects ) 7,00 6,00 5,00 4,00 NG Atmospherical Air Boecillo (Spain) Summer 2013 Wihout Alg With Alg 3,00 IS THE REMAINING CONTAMINANT SEPARABLE FROM THE EXPLOSIVE AT HIGHER RESOLUTION? 2,00 1,00 0, # samples Atmospheric aerosols 11
12 V(N2+1% 2-propanol) Dopant addition. Efforts to separate contaminants: Increase mobility resolution via polar dopants addition Shift of mobility peak for a diversity of ions after adding 1% of 2-propanol. Various ions shift differently. (unpublished data from G. Vidal and A. Alvaro) y=x 50 C 75 C V1 (N2) Atmospheric aerosols 12
13 Intensity (counts) Efforts to separate contaminants: Increase mobility resolution via polar dopants addition Effect of polar dopants addition: RDX & TNT RDX: Addition to 2-propanol vapors shifts mobility due to ion solvation TNT: One interferent displaced. One interferent not displaced Inteferent 0% Real Explosive 0% Real explosive 0.5% Inteferent 0.5% TNT DMA voltage (V) Atmospheric aerosols 13
14 Efforts to separate contaminants: Mass discrimination approach Increase mass resolution by comparing curves of fragment ratio versus collision energy: FRi(CE) No difference found. Singularity at near zero intensity Atmospheric aerosols 14
15 Efforts to separate contaminants: Mass discrimination approach Increase mass resolution using abundance ratio (FR) of several minor fragments. Too low intensity of minor fragments to make conclusions. TNT TNT TNT TNT TNT TNT TNT ul 22,599 28, ,739 53,959 30,310 29,350 59,656 1 ul 21,250 28, ,641 50,766 26,645 29,854 55,955 1 ul 18,846 25, ,529 47,875 24,179 26,623 50,687 Exp. 529, ,269 6,230,384 1,329, , ,127 1,430,301 Exp. 1,794,964 2,433,479 20,897,713 4,519,795 2,448,399 2,505,966 4,849,996 Interf ,027 1, FR1 FR2 FR0 FR3 FR4 FR5 FR6 1 ul ul ul Exp Exp Interf DIFFERENCES ARE SEEN, BUT THERE ARE STILL INDISTINGUISHABLE SIGNALS! Atmospheric aerosols 15
16 INDEX Introduction: Brief description of the application and the device The problem addressed: Existence of background contaminants at ppq Efforts to separate contaminants: Increase mobility resolution via Gaussian deconvolution Increase mobility resolution via polar dopants addition Mass discrimination approach Conclusions Atmospheric aerosols 16
17 Conclusions The explosive trace detection application requires very sensitive equipment. Below of a few ppq for some explosives At these levels, there are atmospheric interferences in the signal that make discrimination really challenging The atmosphere contains up to 1 ppq of substances indistinguishable from actual explosives based on mobility, mass and fragment mass We have tried several estrategies to separate real explosive from atmospheric interferent Mobility deconvolution enables removal of most of these contaminants. Other strategies are usefull, but there are some resilient interfering signals that can t be separated from real explosives Everything seems to point that these most recalcitrant apparent false positives are in fact real explosive vapors produced in the atmosphere There are some mechanisms that could produce this molecules in the atmosphere at the concentrations analized, but the exact path is still being investigated Atmospheric aerosols 17
18 Thanks for your attention! Any questions? Atmospheric aerosols 18
19 APLICACIÓN DEL SISTEMA TANDEM DMA-MS AL ANÁLISIS ATMOSFÉRICO TANDEM DMA-MS SYSTEM APPLICATION TO ATMOSPHERIC ANALYSIS ARTURO ÁLVARO CARBALLIDO 1,2, DAOIZ ZAMORA PÉREZ 1, GONZALO FERNANDEZ DE LA MORA 1 1 Sociedad Europea de Análisis Diferencial de Movilidad, 2 Universidad de Valladolid arturo.alvaro@seadm.com Atmospheric aerosols 19
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