Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - High-resolution sulphur isotope analysis of speleothem carbonate by secondary ionisation mass spectrometry
AU - Wynn, Peter M.
AU - Fairchild, Ian J.
AU - Frisia, Silvia
AU - Spoetl, Christoph
AU - Baker, Andy
AU - Borsato, Andrea
AU - EIMF
PY - 2010/3/30
Y1 - 2010/3/30
N2 - Sulphur emitted into the atmosphere from industrial activity is regarded as a key mechanism in forcing recent climate and has impacts upon the environment and human health at both local and regional scales. Trace amounts of sulphate present within speleothem carbonate can be used to provide an emissions inventory for regional sulphur loading to the atmosphere where sulphur isotopes can be extracted and used as a tool for provenance. However, speleothem sulphur concentrations are low and manual techniques for sulphur isotope analysis allow only low sampling resolution. SIMS (Secondary Ionisation Mass Spectrometry) is used here to develop records of sulphur isotopic change in speleothems from the Italian and Austrian Alps, where annual laminae are less than 100 mu m thick. Analysis at annual resolution over the past 100 years demonstrates an excursion in sulphur isotopic composition from values close to the carbonate bedrock end-member composition in the pre-industrial era, to values isotopically depleted in (34) S. This trend is mirrored by increasing concentrations of sulphate and is suggested to reflect the increase in SO2 emissions with industrial activity. Subsequent decline in speleothem sulphate concentrations in one of the stalagmites reflects the recent European decline in industrial atmospheric SO2 content and is matched by a rebound in sulphur isotopic composition to values more enriched in 345 Superimposed on this general secular trend are smaller (annual) variations in concentration reflecting cave environmental conditions. High magnitude events of short duration, potentially reflect volcanic inputs of SO2 or the incorporation of dust particulates into the speleothem carbonate. This is the first micro-analysis of carbonate-associated sulphate (CAS) sulphur isotopes by SIMS. SIMS analysis of delta S-34-SO4 in speleothem carbonate reveals a high resolution archive depicting a regional sulphur emissions inventory for SO2 loading to the atmosphere. (C) 2010 Elsevier B.V. All rights reserved.
AB - Sulphur emitted into the atmosphere from industrial activity is regarded as a key mechanism in forcing recent climate and has impacts upon the environment and human health at both local and regional scales. Trace amounts of sulphate present within speleothem carbonate can be used to provide an emissions inventory for regional sulphur loading to the atmosphere where sulphur isotopes can be extracted and used as a tool for provenance. However, speleothem sulphur concentrations are low and manual techniques for sulphur isotope analysis allow only low sampling resolution. SIMS (Secondary Ionisation Mass Spectrometry) is used here to develop records of sulphur isotopic change in speleothems from the Italian and Austrian Alps, where annual laminae are less than 100 mu m thick. Analysis at annual resolution over the past 100 years demonstrates an excursion in sulphur isotopic composition from values close to the carbonate bedrock end-member composition in the pre-industrial era, to values isotopically depleted in (34) S. This trend is mirrored by increasing concentrations of sulphate and is suggested to reflect the increase in SO2 emissions with industrial activity. Subsequent decline in speleothem sulphate concentrations in one of the stalagmites reflects the recent European decline in industrial atmospheric SO2 content and is matched by a rebound in sulphur isotopic composition to values more enriched in 345 Superimposed on this general secular trend are smaller (annual) variations in concentration reflecting cave environmental conditions. High magnitude events of short duration, potentially reflect volcanic inputs of SO2 or the incorporation of dust particulates into the speleothem carbonate. This is the first micro-analysis of carbonate-associated sulphate (CAS) sulphur isotopes by SIMS. SIMS analysis of delta S-34-SO4 in speleothem carbonate reveals a high resolution archive depicting a regional sulphur emissions inventory for SO2 loading to the atmosphere. (C) 2010 Elsevier B.V. All rights reserved.
KW - Sulphur isotopes
KW - Secondary Ionisation Mass Spectrometry
KW - Speleothem
KW - X-RAY
KW - ATMOSPHERIC SULFATE
KW - STALAGMITES
KW - CLIMATE
KW - DEPOSITION
KW - ARCHIVES
KW - SIGNALS
KW - EUROPE
KW - GROWTH
KW - OCEAN
UR - http://www.scopus.com/inward/record.url?scp=77549083964&partnerID=8YFLogxK
U2 - 10.1016/j.chemgeo.2010.01.001
DO - 10.1016/j.chemgeo.2010.01.001
M3 - Journal article
VL - 271
SP - 101
EP - 107
JO - Chemical Geology
JF - Chemical Geology
SN - 0009-2541
IS - 3-4
ER -