Development of a multi-collector inductively coupled plasma massspectrometry method for measurement of stable sulphur isotope ratios in aerosol sulphate

Sammanfattning: Sulphur stable isotope ratios are useful tracers in geological and environmental studies. They can for example be used to trace the origin of atmospheric sulphate aerosols, because anthropogenic sulphate and natural sulphate have distinguishable δ34S-values (δ34S value of approximately +0 to +8 ‰ for anthropogenic and approximately +12 to +19 ‰ for natural). This is useful for climate modelling research, due to the net cooling effect of aerosol sulphate. In the present study a Nu Plasma II (Nu Instruments) multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) method for measuring stable sulphur isotope ratios in low sulphur content samples, such as sulphate aerosols, was developed. The method was then applied to a sulphate aerosol sample collected in the Maldives.Most of the measurements were performed at high resolution, due to the interferences on 33S. Heated spray chamber coupled to a desolvating membrane, Aridus II (Cetac), increased the sensitivity and reduced interferences notably compared to wet plasma mode. Aridus II gave more stable measurements than DSN-100 (Nu Instruments). Determinations of δ34S for IAEA S1, S3, and S4 were accurate and the determined δ34S-value of the CIT #39 seawater standard (21.05 ± 0.36 ‰, 2SD, n=42) was comparable with published data. In general, Si internal standardization correction increased precision ~2.5 times compared to non-corrected values. The δ34S-value for the sulphate aerosol sample was determined to 3.82 ±0.41 ‰ (2SD, n=40). Repeatability of ~62 nmol introduced sulphur (2 μg/mL) was generally 0.15 ‰ (2SD, n=5) for the SW and 0.19 ‰ (2SD, n=5) for the sulphate aerosol sample. Comparable results for the SW (20.61±0.09 ‰, 2SD, n=4) and sulphate aersosol sample (3.77 ± 0.08 ‰, 2SD, n=8) were obtained with the method applied to Neptune Plus (Thermo Fischer Scientific) MC-ICP-MS in a different laboratory. The determined aerosol sulphate δ34S-value indicated that the sampled sulphate aerosol originated from anthropogenic sources.