Improved analysis of micro‐ and nanomole‐scale sulfur multi‐isotope compositions by gas source isotope ratio mass spectrometry

Yang, David Au; Landais, Guillaume; Assayag, N.; Wîdory, David; Cartigny, Pierre

doi:10.1002/rcm.7513

Cited by 25 publications

(29 citation statements)

References 39 publications

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“…No further corrections were carried out, other than normalization of the data to CDT. Δ 33 S and Δ 36 S IAEA-standards were within values reported elsewhere (Labidi et al, 2012;Defouilloy et al, 2016;Au Yang et al, 2016). Our analysis (n = 8) of IAEA-S1 standard yielded: δ 34 S = -0.29 ± 0.04‰, Δ 33 S = 0.080 ± 0.010‰ and Δ 36 S = -0.852 ± 0.085‰ vs CDT.…”

Section: Sulfur Multi-isotope Analysissupporting

confidence: 85%

Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2

Yang¹,

Cartigny²,

Desboeufs³

et al. 2018

Preprint

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Abstract. Sulfates present in urban aerosols collected worldwide usually exhibit significant non-zero &#916;33S signatures (from &#8722;0.6 to 0.5&#8201;&#8240;) whose origin still remains unclear. To better address this issue, we recorded the seasonal variations of the multiple sulfur isotope compositions of PM10 aerosols collected over the year 2013 at five stations within the Montreal Island (Canada), each characterized by distinct types and levels of pollution. The &#948;34S-values (n&#8201;=&#8201;155) vary from 2.0 to 11.3&#8201;&#8240; (&#177; 0.2&#8201;&#8240;, 2&#963;), the &#916;33S-values from &#8722;0.080 to 0.341&#8201;&#8240; (&#177; 0.01&#8201;&#8240;, 2&#963;) and the &#916;36S-values from &#8722;1.082 to 1.751&#8201;&#8240; (&#177; 0.2&#8201;&#8240;, 2&#963;). Our study evidences a seasonality for both the &#948;34S and &#916;33S, which can be observed either when considering all monitoring stations or, to a lesser degree, when considering them individually. Among them, the monitoring station located at the most western end of the island, upstream of local emissions, yields the lowest mean &#948;34S coupled to the highest mean &#916;33S-values. The &#916;33S-values are higher during both summer and winter, and are <&#8201;0.1&#8201;&#8240; during both spring and autumn. As these higher &#916;33S-values are measured in "upstream" aerosols, we conclude that the mechanism responsible for these highly positive S-MIF also occurs outside and not within the city, at odds with common assumptions. While the origin of such variability in the &#916;33S-values of urban aerosols (i.e. &#8722;0.6 to 0.5&#8201;&#8240;) is still subject to debate, we suggest that oxidation by Criegee radicals and/or photooxidation of atmospheric SO2 in presence of mineral dust may play a role in generating such large ranges of S-MIF.

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Section: Sulfur Multi-isotope Analysissupporting

confidence: 85%

Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2

Yang¹,

Cartigny²,

Desboeufs³

et al. 2018

Preprint

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“…Δ 36 S = -0.970 ± 0.277 ‰ vs V-CDT. All values are within the ranges of δ 34 S, Δ 33 S, Δ 36 S accepted or measured by other laboratories for these international standards (Au Yang et al, 2016;Farquhar et al, 2007b;Labidi et al, 2014;Ono et al, 2006b). Analysis of the international sulfate standard NBS-127 was also performed and gave a δ 34 S of 20.8 ± 0.4 ‰ (2σ; n=12), consistent with the 20.3 ± 0.4 ‰ value reported by the IAEA.…”

supporting

confidence: 82%

“…China and California result from stratospheric fallout of SO 2 (with ∆ 33 S potentially up to +10 ‰ higher; Ono et al (2013)), which underwent UV photolysis by short wavelength (Au Yang et al, 2016;Lin et al, 2018a;Lin et al, 2018b;Romero and Thiemens, 2003). This suggestion primarily relies on the similarities between ∆ 33 S-∆ 36 S values of sulfate aerosols and laboratory experiments of SO 2 photolysis conducted at different wavelengths…”

Section: A New Oxidation Pathway Implying Magnetic Isotope Effect 455mentioning

confidence: 99%

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative ∆33S-reservoir of sulfate aerosols?

Genot¹,

Yang²,

Martin³

et al. 2019

Preprint

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Abstract. To better understand the formation and the oxidation pathways leading to gypsum-forming &#8220;black crusts&#8221; and investigate their bearing on the whole atmospheric SO2 cycle, we measured the oxygen (&#948;17O, &#948;18O and &#8710;17O) and sulfur (&#948;33S, &#948;34S, &#948;36S, &#8710;33S and &#8710;36S) isotopic compositions of black crust sulfates sampled on carbonate building stones along a NW-SE cross-section in the Parisian basin. The &#948;18O and &#948;34S, ranging between 7.5 and 16.7&#8201;&#177;&#8201;0.5&#8201;&#8240; (n&#8201;=&#8201;27, 2&#963;) and between &#8722;2.6 and 13.9&#8201;&#177;&#8201;0.2&#8201;&#8240; respectively, show anthropogenic SO2 as the main sulfur source (from 2 to 81&#8201;%, in average ~30&#8201;%) with host-rock sulfates making the complement. This is supported by &#8710;17O-values (up to 2.6&#8201;&#8240;, in average ~0.86&#8201;&#8240;), requiring >&#8201;60&#8201;% of atmospheric sulfates in black crusts. Both negative &#8710;33S-&#8710;36S-values between &#8722;0.34 and 0.00&#8201;&#177;&#8201;0.01&#8201;&#8240; and between &#8722;0.7 and &#8722;0.2&#8201;&#177;&#8201;0.2&#8201;&#8240; respectively were measured in black crusts sulfates, that is typical of a magnetic isotope effect that would occur during the SO2 oxidation on the building stone, leading to 33S-depletion in black crust sulfates and subsequent 33S-enrichment in residual SO2. Given that sulfate aerosols have mostly &#8710;33S&#8201;>&#8201;0&#8201;&#8240; and no processes can yet explain this enrichment, resulting in a non-consistent S-budget, black crust sulfates could well represent the complementary negative &#8710;33S-reservoir of the sulfate aerosols solving the atmospheric SO2 budget.

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“…Analysis of the IAEA-S3 (n = 8) gave the following: δ 34 S = −32.44 ± 0.30 ‰, 33 S = 0.069±0.023 ‰, and 36 S = −0.970±0.277 ‰ vs. V-CDT. All values are within the ranges of δ 34 S, 33 S, and 36 S accepted or measured by other laboratories for these international standards (Au Yang et al, 2016;Farquhar et al, 2007b;Labidi et al, 2014;Ono et al, 2006b;Geng et al, 2019).…”

Section: Samplessupporting

confidence: 58%

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33S reservoir of sulfate aerosols?

et al. 2020

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Abstract. To better understand the formation and the oxidation pathways leading to gypsum-forming “black crusts” and investigate their bearing on the whole atmospheric SO2 cycle, we measured the oxygen (δ17O, δ18O, and Δ17O) and sulfur (δ33S, δ34S, δ36S, Δ33S, and Δ36S) isotopic compositions of black crust sulfates sampled on carbonate building stones along a NW–SE cross section in the Parisian basin. The δ18O and δ34S 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 SO2 as the main sulfur source (from ∼2 % to 81 %, average ∼30 %) with host-rock sulfates making the complement. This is supported by Δ17O values (up to 2.6 ‰, on average ∼0.86 ‰), requiring > 60 % of atmospheric sulfates in black crusts. Negative Δ33S and Δ36S 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 SO2 oxidation on the building stone, leading to 33S depletion in black crust sulfates and subsequent 33S enrichment in residual SO2. Except for a few samples, sulfate aerosols mostly have Δ33S 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 Δ33S reservoir of the sulfate aerosols, thus solving the atmospheric SO2 budget.

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Improved analysis of micro‐ and nanomole‐scale sulfur multi‐isotope compositions by gas source isotope ratio mass spectrometry

Cited by 25 publications

References 39 publications

Seasonality in the Δ<sup>33</sup>S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO<sub>2</sub>

Seasonality in the Δ<sup>33</sup>S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO<sub>2</sub>

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative ∆<sup>33</sup>S-reservoir of sulfate aerosols?

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ<sup>33</sup>S reservoir of sulfate aerosols?

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Improved analysis of micro‐ and nanomole‐scale sulfur multi‐isotope compositions by gas source isotope ratio mass spectrometry

Cited by 25 publications

References 39 publications

Seasonality in the Δ&lt;sup&gt;33&lt;/sup&gt;S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO&lt;sub&gt;2&lt;/sub&gt;

Seasonality in the Δ&lt;sup&gt;33&lt;/sup&gt;S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO&lt;sub&gt;2&lt;/sub&gt;

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative ∆&lt;sup&gt;33&lt;/sup&gt;S-reservoir of sulfate aerosols?

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ&lt;sup&gt;33&lt;/sup&gt;S reservoir of sulfate aerosols?

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Seasonality in the Δ<sup>33</sup>S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO<sub>2</sub>

Seasonality in the Δ<sup>33</sup>S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO<sub>2</sub>

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative ∆<sup>33</sup>S-reservoir of sulfate aerosols?

Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ<sup>33</sup>S reservoir of sulfate aerosols?