Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33 S reservoir of sulfate aerosols?
Isabelle Genot
(1, 2)
,
David Au Yang
(1, 3, 4)
,
Erwan Martin
(2)
,
Pierre Cartigny
(1)
,
Erwann Legendre
(2, 5)
,
Marc de Rafélis
(6)
David Au Yang
- Fonction : Auteur
- PersonId : 1209623
- IdHAL : davidauyang
- ORCID : 0000-0002-0822-3618
Erwan Martin
- Fonction : Auteur
- PersonId : 13853
- IdHAL : erwan-martin
- ORCID : 0000-0002-6414-5263
- IdRef : 112147798
Pierre Cartigny
- Fonction : Auteur
- PersonId : 837967
- ORCID : 0000-0002-4730-7419
Résumé
To better understand the formation and the oxidation pathways leading to gypsum-forming "black crusts" and investigate their bearing on the whole atmospheric SO 2 cycle , we measured the oxygen (δ 17 O, δ 18 O, and 17 O) and sulfur (δ 33 S, δ 34 S, δ 36 S, 33 S, and 36 S) isotopic compositions of black crust sulfates sampled on carbonate building stones along a NW-SE cross section in the Parisian basin. The δ 18 O and δ 34 S values, ranging between 7.5 ‰ and 16.7±0.5 ‰ (n = 27, 2σ) and between −2.66 ‰ and 13.99± 0.20 ‰, respectively, show anthropogenic SO 2 as the main sulfur source (from ∼ 2 % to 81 %, average ∼ 30 %) with host-rock sulfates making the complement. This is supported by 17 O values (up to 2.6 ‰, on average ∼ 0.86 ‰), requiring > 60 % of atmospheric sulfates in black crusts. Negative 33 S and 36 S values between −0.34 ‰ and 0.00 ± 0.01 ‰ and between −0.76 ‰ and −0.22 ± 0.20 ‰, respectively, were measured in black crust sulfates, which is typical of a magnetic isotope effect that would occur during the SO 2 oxidation on the building stone, leading to 33 S depletion in black crust sulfates and subsequent 33 S enrichment in residual SO 2. Except for a few samples, sulfate aerosols mostly have 33 S values > 0 ‰, and no processes can yet explain this enrichment, resulting in an inconsistent S budget: black crust sulfates could well represent the complementary negative 33 S reservoir of the sulfate aerosols, thus solving the atmospheric SO 2 budget.
Domaines
Océan, AtmosphèreFormat du dépôt | Fichier |
---|---|
Type de dépôt | Article dans une revue |
Résumé |
en
To better understand the formation and the oxidation pathways leading to gypsum-forming "black crusts" and investigate their bearing on the whole atmospheric SO 2 cycle , we measured the oxygen (δ 17 O, δ 18 O, and 17 O) and sulfur (δ 33 S, δ 34 S, δ 36 S, 33 S, and 36 S) isotopic compositions of black crust sulfates sampled on carbonate building stones along a NW-SE cross section in the Parisian basin. The δ 18 O and δ 34 S values, ranging between 7.5 ‰ and 16.7±0.5 ‰ (n = 27, 2σ) and between −2.66 ‰ and 13.99± 0.20 ‰, respectively, show anthropogenic SO 2 as the main sulfur source (from ∼ 2 % to 81 %, average ∼ 30 %) with host-rock sulfates making the complement. This is supported by 17 O values (up to 2.6 ‰, on average ∼ 0.86 ‰), requiring > 60 % of atmospheric sulfates in black crusts. Negative 33 S and 36 S values between −0.34 ‰ and 0.00 ± 0.01 ‰ and between −0.76 ‰ and −0.22 ± 0.20 ‰, respectively, were measured in black crust sulfates, which is typical of a magnetic isotope effect that would occur during the SO 2 oxidation on the building stone, leading to 33 S depletion in black crust sulfates and subsequent 33 S enrichment in residual SO 2. Except for a few samples, sulfate aerosols mostly have 33 S values > 0 ‰, and no processes can yet explain this enrichment, resulting in an inconsistent S budget: black crust sulfates could well represent the complementary negative 33 S reservoir of the sulfate aerosols, thus solving the atmospheric SO 2 budget.
|
Titre |
en
Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ<sup>33</sup> S reservoir of sulfate aerosols?
|
Auteur(s) |
Isabelle Genot
1, 2
, David Au Yang
1, 3, 4
, Erwan Martin
2
, Pierre Cartigny
1
, Erwann Legendre
2, 5
, Marc de Rafélis
6
1
IPGP (UMR_7154) -
Institut de Physique du Globe de Paris
( 1005035 )
- 1 rue Jussieu, 75238 Paris cedex 05 et Bât. Lamarck A case postale 7011, 75205 Paris CEDEX 13
- France
2
iSTeP -
Institut des Sciences de la Terre de Paris
( 541927 )
- 4, place Jussieu BP CC129 75252 PARIS CEDEX 05
- France
3
GEOTOP -
Centre de recherche sur la dynamique du système Terre
( 320713 )
- Université du Québec à Montréal 201, Président-Kennedy Ave. 7th floor, room PK-7150 Montréal QC H2X 3Y7 Canada
- Canada
4
EPS -
Department of Earth and Planetary Sciences [Montréal]
( 86187 )
- 3450 University St., Montreal, Canada H3A 2A7
- Canada
5
STRATO - LATMOS
( 541922 )
- France
6
GET -
Géosciences Environnement Toulouse
( 151875 )
- Observatoire Midi-Pyrénées 14 Avenue Edouard Belin 31400 Toulouse
- France
|
Volume |
20
|
Vulgarisation |
Non
|
Nom de la revue |
|
Comité de lecture |
Oui
|
Langue du document |
Anglais
|
Page/Identifiant |
4255 - 4273
|
Numéro |
7
|
Date de publication |
2020
|
Audience |
Internationale
|
Licence |
Paternité
|
Domaine(s) |
|
Projet(s) ANR |
|
Financement |
|
DOI | 10.5194/acp-20-4255-2020 |
Origine :
Publication financée par une institution
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