Influence of anthropogenic sources on total gaseous mercury variability in grenoble suburban air (France)

doi:10.1016/S0048-9697(02)00133-X

Science of The Total Environment

Volume 297, Issues 1–3, 7 October 2002, Pages 203-213

https://doi.org/10.1016/S0048-9697(02)00133-X Get rights and content

Abstract

Total gaseous mercury (TGM) has been monitored at Champ sur Drac, a suburban site of Grenoble in southern east France. TGM measurements have been made over 4 periods of approximately 10 days throughout 1999–2000 using cold vapour atomic fluorescence absorption technique. The first monitoring campaign was initiated on November 4, 1999, followed by three other campaigns respectively on January 12, 2000, April 10, 2000 and July 17, 2000. Concurrent monitoring of O₃, NO, NO₂, SO₂ and of meteorological parameters have also been performed. The mean TGM concentration was 3.4 ng m⁻³ with maximum hourly mean concentration of 37.1 ng m⁻³. Although mean TGM concentration was not greatly different from those previously measured in the troposphere, the greater TGM variability as well as the occurrence of high TGM concentration linked to particular wind conditions suggested the strong influence of anthropogenic sources. The chlor-alkali plant located nearby, the others chemical industries using fuel combustion and the municipal waste incinerator were thought to contribute to mercury pollution events.

Introduction

Since the pollution prevention concept emerged many years ago (Pacyna, 1986), there has been a growing concern about air quality in urban areas. To improve urban air quality, environmental policy makers expressed widespread interest in controlling and regulating major gaseous pollutants such as O₃, CO, NO, NO₂, SO₂ and volatile organic compounds. However gaseous mercury supervision is only from time to time included in urban pollution monitoring whereas the knowledge of its distribution and transport pathways are of critical importance. Enlarging air pollution monitoring program to atmospheric gaseous mercury survey can only ensure this.

Gaseous elemental mercury (Hg⁰) is the dominant form (∼98% e.g. Poissant, 2000) of mercury in the atmosphere. Elemental mercury is very insoluble, unreactive (Schroeder and Munthe, 1998, Tokos et al., 1998) and thus has a residence time in the atmosphere of approximately 0.5–2 years (Lindqvist and Rodhe, 1985, Slemr et al., 1985, Munthe and McElroy, 1992). Therefore Hg⁰ is well mixed atmospherically and total gaseous mercury (TGM) concentration is in the range 1–5 ng m⁻³ in the troposphere (Lee et al., 1998, Ebinghaus and Slemr, 2000, Urba et al., 2000).

Mercury is emitted into the atmosphere from a variety of natural and anthropogenic sources. The natural sources include volcanoes, crustal degassing, forests, lakes and oceans (Lindqvist and Rodhe, 1985, Mason et al., 1994), while fossil-fuel combustions, incineration, metallurgical processes and chlor-alkali plants constitute the largest part of anthropogenic Hg emissions (Pirrone et al., 1996). In French urban areas, waste incineration is the major source of Hg (CITEPA, 2000). The other contributions are coal combustion followed by chlor-alkali plants, wood combustion and metallurgic processes. Once emitted, mercury is involved in many physical and chemical transformations (Schroeder and Munthe, 1998, Lin and Pehkonen, 1999) and can be deposited by wet and dry processes to environmental surfaces. These deposition processes are more efficient if mercury is in the +II oxidation state (Lindberg and Stratton, 1998).

Since information on background concentrations and anthropogenic sources are still lacking for many places in Europe, we present here the first automated long-term, high time resolution measurements of TGM concentration in France. To our knowledge, this report constitutes the first presentation of extended atmospheric mercury data from a site in France. We attempted to compare these data with other pollutants (O₃, NO, NO₂, SO₂) concentrations and meteorological parameters (wind speed, wind direction, atmospheric pressure, temperature, solar irradiation and precipitation intensity). An assessment of potential anthropogenic mercury sources and their influence on our measurement site are also provided.

Section snippets

Site characteristics

TGM concentrations were determined in the vicinity of Grenoble in the south east of France (Fig. 1). The measurement station is located at Champ sur Drac (45.080°N, 5.730°E, 267 m a.s.l.) which is a suburban site of Grenoble, characterized by an industrial zone in the north and particularly a chlor-alkali plant (Fig. 2) using mercury cell process. Grenoble (∼400 000 inhabitants) is ∼10 km north from the site and has one of the largest municipal waste incinerator in the area.

Sampling and analysis

TGM measurements were

Annual, seasonal and diurnal variability of TGM

A statistical summary of TGM data subdivided into their respective seasons is presented in Table 1. The mean seasonal TGM concentration varies throughout the year from 1.9 to 4.8 ng m⁻³. The mean TGM concentration (+1 S.D.) calculated over the year is 3.4±3.6 ng m⁻³ (N=3596). Maximum TGM concentration was recorded in July (45.9 ng m⁻³) with an hourly mean concentration of 37.1 ng m⁻³ for this event.

Ozone mean concentrations are ranging from ∼7 ppbv for winter data to ∼30 ppbv for summer data with

Conclusions

The high variability of TGM values is the first clear evidence of the influence of local anthropogenic sources. We estimated that the main local anthropogenic sources were the chlor-alkali plant and the waste incinerator (we speculated a total amount of ∼900 kgHg emitted per year). A similarity between SO₂ and TGM concentrations profiles was sometimes observed that may indicate common sources.

Relationship between emission sources north of the site and wind direction was clearly identified. Most

Acknowledgements

This work has been financially supported by the Centre National de la Recherche Scientifique (CNRS, France) in the frame of A.T.I. (Action Thématique Innovante 1999). We would like to thank the AS.CO.P.A.R.G. (ASsociation pour le COntrôle et la Prévention de l'Air dans la Région Grenobloise) for their technical support. We also thank Grenoble Alpes Métropole (Athanor, La Compagnie de Chauffage de Grenoble) and Atofina for their help for emission data collection.

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Influence of anthropogenic sources on total gaseous mercury variability in grenoble suburban air (France)

Abstract

Introduction

Section snippets

Site characteristics

Sampling and analysis

Annual, seasonal and diurnal variability of TGM

Conclusions

Acknowledgements

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