Jakober Chris A, Robert Michael A, Riddle Sarah G, Destaillats Hugo, Charles M Judith, Green Peter G, Kleeman Michael J
Department of Environmental Toxicology, University of California, Davis, One Shields Avenue, Davis, California 95616, USA.
Environ Sci Technol. 2008 Jul 1;42(13):4697-703. doi: 10.1021/es7029174.
Carbonyls from gasoline-powered light-duty vehicles (LDVs) and heavy-duty diesel-powered vehicles (HDDVs) operated on chassis dynamometers were measured by use of an annular denuder-quartz filter-polyurethane foam sampler with O-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine derivatization and chromatography-mass spectrometry analyses. Two internal standards were utilized based on carbonyl recovery: 4-fluorobenzaldehyde for < C8 carbonyls and 6-fluoro-4-chromanone for > or = C8 compounds. Gas- and particle-phase emissions for 39 aliphatic and 20 aromatic carbonyls ranged from 0.1 to 2000 microg/L of fuel for LDVs and from 1.8 to 27 000 microg/L of fuel for HDDVs. Gas-phase species accounted for 81-95% of the total carbonyls from LDVs and 86-88% from HDDVs. Particulate carbonyls emitted from a HDDV under realistic driving conditions were similar to concentrations measured in a diesel particulate matter (PM) standard reference material. Carbonyls accounted for 19% of particulate organic carbon (POC) emissions from low-emission LDVs and 37% of POC emissions from three-way catalyst-equipped LDVs. This identifies carbonyls as one of the largest classes of compounds in LDV PM emissions. The carbonyl fraction of HDDV POC was lower, 3.3-3.9% depending upon operational conditions. Partitioning analysis indicates the carbonyls had not achieved equilibrium between the gas and particle phases under the dilution factors of 126-584 used in the present study.
使用带有O-(2,3,4,5,6-五氟苄基)羟胺衍生化及色谱-质谱分析的环形 denuder-石英滤膜-聚氨酯泡沫采样器，对在底盘测功机上运行的汽油动力轻型车辆(LDV)和重型柴油动力车辆(HDDV)中的羰基化合物进行了测量。基于羰基回收率使用了两种内标：对于碳数小于8的羰基化合物使用4-氟苯甲醛，对于碳数大于或等于8的化合物使用6-氟-4-色满酮。39种脂肪族羰基化合物和20种芳香族羰基化合物的气相和颗粒相排放，对于轻型车辆而言为0.1至2000μg/L燃料，对于重型柴油车辆而言为1.8至27000μg/L燃料。气相物种占轻型车辆羰基化合物总量的81-95%，占重型柴油车辆羰基化合物总量的86-88%。在实际驾驶条件下重型柴油车辆排放的颗粒羰基化合物与柴油颗粒物(PM)标准参考物质中测得的浓度相似。羰基化合物占低排放轻型车辆颗粒有机碳(POC)排放的19%，占配备三元催化剂轻型车辆POC排放的37%。这表明羰基化合物是轻型车辆PM排放中最大的化合物类别之一。重型柴油车辆POC的羰基部分较低，根据运行条件为3.3-3.9%。分配分析表明，在本研究使用的126-584稀释因子下，羰基化合物在气相和颗粒相之间未达到平衡。
