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  • 1
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2012. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 117 (2012): D13303, doi:10.1029/2011JD017153.
    Description: Carbon isotopic signatures (δ13C, Δ14C) of aerosol particulate matter total organic carbon (TOC) and operationally defined organic carbon (OC) components were measured in samples from two background sites in the eastern U.S. TOC and water-soluble OC (WSOC) δ13C values (−27 to −24‰) indicated predominantly terrestrial C3 plant and fossil derived sources. Total solvent extracts (TSE) and their aliphatic, aromatic, and polar OC components were depleted in δ13C (−30 to −26‰) relative to TOC and WSOC. Δ14C signatures of aerosol TOC and TSE (−476 to +25‰) suggest variable fossil contributions (~5–50%) to these components. Aliphatic OC while comprising a small portion of the TOC (〈1%), was dominated by fossil-derived carbon (86 ± 3%), indicating its potential utility as a tracer for fossil aerosol OC inputs. In contrast, aromatic OC contributions (〈1.5%) contained approximately equal portions contemporary (52 ± 8%) and fossil (48 ± 8%) OC. The quantitatively significant polar OC fraction (6–25% of TOC) had fossil contributions (30 ± 12%) similar to TOC (26 ± 7%) and TSE (28 ± 9%). Thus, much of both of the fossil and contemporary OC is deduced to be oxidized, polar material. Aerosol WSOC consistently showed low fossil content (〈8%) relative to the TOC (5–50%) indicating that the majority of fossil OC in aerosol particulates is insoluble. Therefore, on the basis of solubility and polarity, aerosols are predicted to partition differently once deposited to watersheds, and these chemically distinct components are predicted to contribute in quantitatively and qualitatively different ways to watershed carbon biogeochemistry and cycling.
    Description: ASW was partially supported by a Graduate Fellowship from the Hudson River Foundation during the course of this study. Additional funding for this work came from a NOSAMS student internship award, a fellowship award from Sun Trust Bank administered through the VIMS Foundation, a student research grant from VIMS, and the following NSF awards: DEB Ecosystems grant DEB-0234533, Chemical Oceanography grant OCE-0327423, and Integrated Carbon Cycle Research Program grant EAR-0403949 to JEB; and Chemical Oceanography grant OCE-0727575 to RMD and JEB.
    Description: 2013-01-04
    Keywords: Aerosols ; Isotopes ; Organic carbon ; Particulate matter ; Radiocarbon ; Water soluble organic carbon
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 2
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2012. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 39 (2012): L18602, doi:10.1029/2012GL052974.
    Description: Marine dissolved organic carbon (DOC) is the largest reservoir of reduced carbon in seawater and persists up to 4,000–6,000 conventional radiocarbon (14C) years on average. Photochemical degradation has been suggested as a geochemical sink for these long-lived molecules, yet there have been no studies relating photochemical lability to the 14C-ages of surface DOC. We observed apparent second order (2°) kinetics with respect to DOC and a strong trend from Δ14C-enriched to depleted values during exhaustive photomineralization of surface marine DOC with high energy UV light. Geochemically, these results suggest that surface DOC is an isotopically-heterogeneous mixture of molecules for which photochemical lability and 14C ages are correlated. Photochemical mineralization may therefore be an important control on the persistence of 14C-depleted DOC in the ocean.
    Description: This study was supported under NSF grant OCE-0961980 to E. R. M. Druffel.
    Description: 2013-03-20
    Keywords: DOC ; Kinetics ; Photochemistry ; Radiocarbon
    Repository Name: Woods Hole Open Access Server
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  • 3
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2012. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 39 (2012): L19703, doi:10.1029/2012GL052883.
    Description: Carbon cycling studies focusing on transport and transformation of terrigenous carbon sources toward marine sedimentary sinks necessitate separation of particulate organic carbon (OC) derived from many different sources and integrated by river systems. Much progress has been made on isolating and characterizing young biologically-formed OC that is still chemically intact, however quantification and characterization of old, refractory rock-bound OC has remained troublesome. Quantification of both endmembers of riverine OC is important to constrain exchanges linking biologic and geologic carbon cycles and regulating atmospheric CO2 and O2. Here, we constrain petrogenic OC proportions in suspended sediment from the headwaters of the Ganges River in Nepal through direct measurement using ramped pyrolysis radiocarbon analysis. The unique results apportion the biospheric and petrogenic fractions of bulk particulate OC and characterize biospheric OC residence time. Compared to the same treatment of POC from the lower Mississippi-Atchafalaya River system, contrast in age spectra of the Ganges tributary samples illustrates the difference between small mountainous river systems and large integrative ones in terms of the global carbon cycle.
    Description: This work was partially supported by U.S. National Science Foundation (NSF) Cooperative Agreement OCE-228996 to NOSAMS and NSF grants OCE-0851015 & OCE-0928582 to VG.
    Description: 2013-04-03
    Keywords: Ganges ; Himalaya ; Mississippi ; POC ; Carbon cycle ; Radiocarbon
    Repository Name: Woods Hole Open Access Server
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