Spatial Dependence of Reduced Sulfur in Everglades Dissolved Organic Matter Controlled by Sulfate Enrichment

Poulin, Brett A.; Ryan, Joseph N.; Nagy, Kathryn L.; Stubbins, Aron; Dittmar, Thorsten; Orem, William; Krabbenhoft, David P.; Aiken, George R.

doi:10.1021/acs.est.6b04142

Spatial Dependence of Reduced Sulfur in Everglades Dissolved Organic Matter Controlled by Sulfate Enrichment

Journal Article · Wed Mar 01 00:00:00 EST 2017 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b04142· OSTI ID:1351336

^[1]; Ryan, Joseph N. ^[2]; Nagy, Kathryn L. ^[3]; Stubbins, Aron ^[4]; Dittmar, Thorsten ^[5]; Orem, William ^[6]; Krabbenhoft, David P. ^[7]; Aiken, George R. ^[8]

U.S. Geological Survey, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States)
Univ. of Illinois, Chicago, IL (United States)
Univ. of Georgia, Savannah, GA (United States)
Univ. of Oldenburg (Germany)
U.S. Geological Survey, Reston, VA (United States)
U.S. Geological Survey, Middleton, WI (United States)
U.S. Geological Survey, Boulder, CO (United States)

Sulfate inputs to the Florida Everglades stimulate sulfidic conditions in freshwater wetland sediments that affect ecological and biogeochemical processes. An unexplored implication of sulfate enrichment is alteration of the content and speciation of sulfur in dissolved organic matter (DOM), which influences the reactivity of DOM with trace metals. Here, we describe the vertical and lateral spatial dependence of sulfur chemistry in the hydrophobic organic acid fraction of DOM from unimpacted and sulfate-impacted Everglades wetlands using X-ray absorption spectroscopy and ultrahigh-resolution mass spectrometry. Spatial variation in DOM sulfur content and speciation reflects the degree of sulfate enrichment and resulting sulfide concentrations in sediment pore waters. Sulfur is incorporated into DOM predominantly as highly reduced species in sulfidic pore waters. Sulfur-enriched DOM in sediment pore waters exchanges with overlying surface waters and the sulfur likely undergoes oxidative transformations in the water column. Across all wetland sites and depths, the total sulfur content of DOM correlated with the relative abundance of highly reduced sulfur functionality. Here, the results identify sulfate input as a primary determinant on DOM sulfur chemistry to be considered in the context of wetland restoration and sulfur and trace metal cycling.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1351336

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 7 Vol. 51; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Spatial Dependence of Reduced Sulfur in Everglades Dissolved Organic Matter Controlled by Sulfate Enrichment

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