The application of soft photoionization mass spectrometry methods (PIMS) for cigarette mainstream smoke analysis is demonstrated. Resonance-enhanced multiphoton ionization (REMPI) at 260 nm and vacuum ultraviolet light single-photon ionization (SPI) at 118 nm were used in combination with time-of-flight mass spectrometry (TOFMS). An optimized smoking machine with reduced memory effects of smoke components was constructed, which in combination with the REMPI/SPI-TOFMS instrument allows PIMS smoke analysis with a time resolution of up to 10 Hz. The complementary character of both PIMS methods is demonstrated. SPI allows the detection of various aliphatic and aromatic compounds in smoke up to approximately 120 m/z while REMPI is well suited for aromatic compounds. The capability of the instrument coupled to the novel sampling system for puff-by-puff resolved measurements is demonstrated. The feasibility of using the experimental system for intrapuff smoke measurements is also shown. Two main patterns of puff-by-puff behaviors are observed for different smoke constituents. The first group exhibits a constant increase in smoke constituent yield from the first to the last puff. The second group shows a high yield of the constituent in the first puff, with lower and constant or slowly increasing yields in the following puffs. A third group cannot be clearly classified and is a combination of both observed profiles.
Soft single photon ionization (SPI)-time-of-flight mass spectrometry (TOFMS) is well suited for fast and comprehensive analysis of complex organic gas mixtures, which has been demonstrated in various applications. This work describes a calibration scheme for SPI, which enables quantification of a large number of compounds by only calibrating one compound of choice, in this case benzene. Photoionization cross sections of 22 substances were determined and related to the yield of benzene. These substances included six alkanes (pentane, hexane, heptane, octane, nonane, decane), three alkenes (propene, butane, pentene), two alkynes (propyne, butyne), two dienes (butadiene, isoprene), five monoaromatic species (benzene, toluene, xylene, styrene, monochlorobenzene) and NO. The cross sections of organic compounds differ by about one order of magnitude but the photoionization properties of compounds belonging to one compound class are rather similar. Therefore, the scheme can also be used for an approximate quantification of compound classes. This is demonstrated by a fast characterization and pattern recognition of two gasoline samples with different origins (Germany and South Africa) and a diesel sample (Germany). The on-line capability of the technique and the scheme is demonstrated by quantitatively monitoring and comparing the cold engine start of four vehicles: a gasoline passenger car, a diesel van, a motorbike and a two-stroke scooter.
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