Post 17th-century changes of European PAH emission recorded in high-altitude Alpin snow and ice

Jacopo Gabrieli; Paul Travis Vallelonga; Giulio Cozzi; Paolo Gabrielli; Andrea Gambaro; Michael Sigl; Margit Schwikowski; Fabio Decet; Heinz Gaggeler; Claude Boutron; Paolo Cescon

doi:10.1021/es903365s

Post 17th-century changes of European PAH emission recorded in high-altitude Alpin snow and ice

Jacopo Gabrieli, Paul Travis Vallelonga, Giulio Cozzi, Paolo Gabrielli, Andrea Gambaro, Michael Sigl, Margit Schwikowski, Fabio Decet, Heinz Gaggeler, Claude Boutron, Paolo Cescon

52 Citations (Scopus)

Abstract

The occurrence of organic pollutants in European Alpine snow/ice has been reconstructed over the past three centuries using a new online extraction method for polycyclic aromatic hydrocarbons (PAH) followed by liquid chromatographic determination. The meltwater flow from a continuous ice core melting system was split into two aliquots, with one aliquot directed to an inductively coupled plasma quadrupole mass spectrometer for continuous trace elements determinations and the second introduced into a solid phase C18 (SPE) cartridge for semicontinuous PAH extraction. The depth resolution for PAH extractions ranged from 40 to 70 cm, and corresponds to 0.7-5 years per sample. The concentrations of 11 PAH were determined in dated snow/ice samples to reconstruct the atmospheric concentration of these compounds in Europe for the last 300 years. The PAH pattern is dominated by phenanthrene (Phe), fluoranthene (Fla), and pyrene (Pyr), which represent 60-80% of the total PAH mass. Before 1875 the sum of PAH concentration (∑PAH) was very low with total mean concentrations less than 2 ng/kg and 0.08 ng/kg for the heavier compounds (∑PAH*, more than four aromatic rings). During the first phase of the industrial revolution (1770-1830) the PAH deposition showed a weak increase which became much greater from the start of the second phase of the industrial revolution at the end of 19th Century. In the 1920s, economic recession in Europe decreased PAH emissions until the 1930s when they increased again and reached a maximum concentration of 32 ng/kg from 1945 to 1955. From 1955 to 1975 the PAH concentrations decreased significantly, reflecting improvements in emission controls especially from major point sources, while from 1975 to 2003 they rose to levels equivalent to those in 1910. The Fla/(Fla+Pyr) ratio is often used for source assignment and here indicates an increase in the relative contribution of gasoline and diesel combustion with respect to coal and wood burning from 1860 to the 1980s. This trend was reversed during the last two decades.

Original language	English
Journal	Environmental Science and Technology
Volume	44
Issue number	9
Pages (from-to)	3260-3266
Number of pages	6
ISSN	1086-931X
DOIs	https://doi.org/10.1021/es903365s
Publication status	Published - 1 May 2010

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10.1021/es903365s

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@article{e0ac7010db5311df825b000ea68e967b,

title = "Post 17th-century changes of European PAH emission recorded in high-altitude Alpin snow and ice",

abstract = "The occurrence of organic pollutants in European Alpine snow/ice has been reconstructed over the past three centuries using a new online extraction method for polycyclic aromatic hydrocarbons (PAH) followed by liquid chromatographic determination. The meltwater flow from a continuous ice core melting system was split into two aliquots, with one aliquot directed to an inductively coupled plasma quadrupole mass spectrometer for continuous trace elements determinations and the second introduced into a solid phase C18 (SPE) cartridge for semicontinuous PAH extraction. The depth resolution for PAH extractions ranged from 40 to 70 cm, and corresponds to 0.7-5 years per sample. The concentrations of 11 PAH were determined in dated snow/ice samples to reconstruct the atmospheric concentration of these compounds in Europe for the last 300 years. The PAH pattern is dominated by phenanthrene (Phe), fluoranthene (Fla), and pyrene (Pyr), which represent 60-80% of the total PAH mass. Before 1875 the sum of PAH concentration (∑PAH) was very low with total mean concentrations less than 2 ng/kg and 0.08 ng/kg for the heavier compounds (∑PAH*, more than four aromatic rings). During the first phase of the industrial revolution (1770-1830) the PAH deposition showed a weak increase which became much greater from the start of the second phase of the industrial revolution at the end of 19th Century. In the 1920s, economic recession in Europe decreased PAH emissions until the 1930s when they increased again and reached a maximum concentration of 32 ng/kg from 1945 to 1955. From 1955 to 1975 the PAH concentrations decreased significantly, reflecting improvements in emission controls especially from major point sources, while from 1975 to 2003 they rose to levels equivalent to those in 1910. The Fla/(Fla+Pyr) ratio is often used for source assignment and here indicates an increase in the relative contribution of gasoline and diesel combustion with respect to coal and wood burning from 1860 to the 1980s. This trend was reversed during the last two decades.",

author = "Jacopo Gabrieli and Vallelonga, {Paul Travis} and Giulio Cozzi and Paolo Gabrielli and Andrea Gambaro and Michael Sigl and Margit Schwikowski and Fabio Decet and Heinz Gaggeler and Claude Boutron and Paolo Cescon",

year = "2010",

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doi = "10.1021/es903365s",

language = "English",

volume = "44",

pages = "3260--3266",

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TY - JOUR

T1 - Post 17th-century changes of European PAH emission recorded in high-altitude Alpin snow and ice

AU - Gabrieli, Jacopo

AU - Vallelonga, Paul Travis

AU - Cozzi, Giulio

AU - Gabrielli, Paolo

AU - Gambaro, Andrea

AU - Sigl, Michael

AU - Schwikowski, Margit

AU - Decet, Fabio

AU - Gaggeler, Heinz

AU - Boutron, Claude

AU - Cescon, Paolo

PY - 2010/5/1

Y1 - 2010/5/1

N2 - The occurrence of organic pollutants in European Alpine snow/ice has been reconstructed over the past three centuries using a new online extraction method for polycyclic aromatic hydrocarbons (PAH) followed by liquid chromatographic determination. The meltwater flow from a continuous ice core melting system was split into two aliquots, with one aliquot directed to an inductively coupled plasma quadrupole mass spectrometer for continuous trace elements determinations and the second introduced into a solid phase C18 (SPE) cartridge for semicontinuous PAH extraction. The depth resolution for PAH extractions ranged from 40 to 70 cm, and corresponds to 0.7-5 years per sample. The concentrations of 11 PAH were determined in dated snow/ice samples to reconstruct the atmospheric concentration of these compounds in Europe for the last 300 years. The PAH pattern is dominated by phenanthrene (Phe), fluoranthene (Fla), and pyrene (Pyr), which represent 60-80% of the total PAH mass. Before 1875 the sum of PAH concentration (∑PAH) was very low with total mean concentrations less than 2 ng/kg and 0.08 ng/kg for the heavier compounds (∑PAH*, more than four aromatic rings). During the first phase of the industrial revolution (1770-1830) the PAH deposition showed a weak increase which became much greater from the start of the second phase of the industrial revolution at the end of 19th Century. In the 1920s, economic recession in Europe decreased PAH emissions until the 1930s when they increased again and reached a maximum concentration of 32 ng/kg from 1945 to 1955. From 1955 to 1975 the PAH concentrations decreased significantly, reflecting improvements in emission controls especially from major point sources, while from 1975 to 2003 they rose to levels equivalent to those in 1910. The Fla/(Fla+Pyr) ratio is often used for source assignment and here indicates an increase in the relative contribution of gasoline and diesel combustion with respect to coal and wood burning from 1860 to the 1980s. This trend was reversed during the last two decades.

AB - The occurrence of organic pollutants in European Alpine snow/ice has been reconstructed over the past three centuries using a new online extraction method for polycyclic aromatic hydrocarbons (PAH) followed by liquid chromatographic determination. The meltwater flow from a continuous ice core melting system was split into two aliquots, with one aliquot directed to an inductively coupled plasma quadrupole mass spectrometer for continuous trace elements determinations and the second introduced into a solid phase C18 (SPE) cartridge for semicontinuous PAH extraction. The depth resolution for PAH extractions ranged from 40 to 70 cm, and corresponds to 0.7-5 years per sample. The concentrations of 11 PAH were determined in dated snow/ice samples to reconstruct the atmospheric concentration of these compounds in Europe for the last 300 years. The PAH pattern is dominated by phenanthrene (Phe), fluoranthene (Fla), and pyrene (Pyr), which represent 60-80% of the total PAH mass. Before 1875 the sum of PAH concentration (∑PAH) was very low with total mean concentrations less than 2 ng/kg and 0.08 ng/kg for the heavier compounds (∑PAH*, more than four aromatic rings). During the first phase of the industrial revolution (1770-1830) the PAH deposition showed a weak increase which became much greater from the start of the second phase of the industrial revolution at the end of 19th Century. In the 1920s, economic recession in Europe decreased PAH emissions until the 1930s when they increased again and reached a maximum concentration of 32 ng/kg from 1945 to 1955. From 1955 to 1975 the PAH concentrations decreased significantly, reflecting improvements in emission controls especially from major point sources, while from 1975 to 2003 they rose to levels equivalent to those in 1910. The Fla/(Fla+Pyr) ratio is often used for source assignment and here indicates an increase in the relative contribution of gasoline and diesel combustion with respect to coal and wood burning from 1860 to the 1980s. This trend was reversed during the last two decades.

U2 - 10.1021/es903365s

DO - 10.1021/es903365s

M3 - Journal article

C2 - 20392089

SN - 1086-931X

VL - 44

SP - 3260

EP - 3266

JO - Environmental Science & Technology. News & Research Notes

JF - Environmental Science & Technology. News & Research Notes

IS - 9

ER -

Post 17th-century changes of European PAH emission recorded in high-altitude Alpin snow and ice

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