Journal
ANALYTICAL CHEMISTRY
Volume 84, Issue 9, Pages 4161-4166Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ac3004456
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Funding
- EPSRC [EP/E027571/1]
- Innovative Research Call in Explosives and Weapons Detection
- CONTEST strategy
- Leopold Franzens Universitat
- Innsbruck
- FWF
- FFG
- Wien
- European Commission, Brussels
- JIP-FP [A-0378-RT GC]
- Marie Curie Industry-Academia Partnership and Pathways [218065]
- Engineering and Physical Sciences Research Council [EP/E027571/1] Funding Source: researchfish
- EPSRC [EP/E027571/1] Funding Source: UKRI
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Fears of terrorist attacks have led to the development of various technologies for the real-time detection of explosives, but all suffer from potential ambiguities in the assignment of threat agents. Using proton transfer reaction mass spectrometry (PTR-MS), an unusual bias dependence in the detection sensitivity of 2,4,6 trinitrotoluene (TNT) on the reduced electric field (E/N) has been observed. For protonated TNT, rather than decreasing signal intensity with increasing E/N, which is the more usual sensitivity pattern observed in PTR-MS studies, an anomalous behavior is first observed, whereby the signal intensity initially rises with increasing E/N. We relate this to unexpected ion-molecule chemistry based upon comparisons of measurements taken with related nitroaromatic compounds (1,3,5 trinitrobenzene, 1,3 dinitrobenzene, and 2,4 dinitrotoluene) and electronic structure calculations. This dependence provides an easily measurable signature that can be used to provide a rapid highly selective analytical procedure to minimize false positives for the detection of TNT. This has major implications for Homeland Security and, in addition, has the potential of making instrumentation cost-effective for use in security areas. This study shows that an understanding of fundamental ion-molecule chemistry occurring in low-pressure drift tubes is needed to exploit selectivity and sensitivity for analytical purposes.
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