Oxidation products of α- and β-amyrins: potential tracers of abiotic degradation of vascular-plant organic matter in aquatic environments

2016 ◽  
Vol 13 (4) ◽  
pp. 732 ◽  
Author(s):  
M.-A. Galeron ◽  
F. Vaultier ◽  
J.-F. Rontani
Keyword(s):  
Organic Matter ◽  
Degradation Products ◽  
Vascular Plant ◽  
Oxidation Products ◽  
Aquatic Environments ◽  
Rhône River ◽  
Abiotic Degradation ◽  
Suspended Particulate ◽  
Rhone River

Environmental contextHow can we know what happens to organic matter in aquatic environments? Although several compounds exist that can be used to trace the origin and state of organic matter, not many are sufficiently stable and specific to trace degradation processes, but α- and β-amyrins can fulfil that role. Such knowledge will help us better understand and better quantify carbon fluxes in riverine and marine environments. AbstractIn order to fulfil the current need for stable and specific tracers to monitor vascular-plant organic matter degradation in aquatic environments, α-amyrin (urs-12-en-3β-ol) and β-amyrin (olean-12-en-3β-ol) were oxidised in vitro and their abiotic degradation products quantified in environmental samples from the Rhône River in France. Although they appear inert to photooxidation, they are clearly affected by autoxidation and the tracer potential of the resulting products was confirmed. Autoxidation of α- and β-amyrins produces urs or olean-12-en-3-one, 3β-hydroxy-urs or olean-12-en-11-one, urs or olean-12-en-3β,11α-diol and urs or olean-12-en-3,11-dione. 3β-Hydroxy-urs-12-en-11-one and 3β-hydroxy-olean-12-en-11-one, the main oxidation products detected, were selected as autoxidation tracers. These compounds, specific to autoxidation, were detected in dry leaves of Smilax aspera and in suspended particulate matter samples collected in the Rhône River and evidenced the importance of autoxidation in the degradation of organic matter of terrestrial origin.

scholarly journals Seasonal survey of the composition and degradation state of particulate organic matter in the Rhone River using lipid tracers

2014 ◽  
Vol 11 (10) ◽  
pp. 14197-14237 ◽  
Author(s):  
M.-A. Galeron ◽  
R. Amiraux ◽  
B. Charriere ◽  
O. Radakovitch ◽  
P. Raimbault ◽  
...  
Keyword(s):  
Organic Matter ◽  
Particulate Organic Matter ◽  
Degradation Products ◽  
Significant Proportion ◽  
Free Radical Oxidation ◽  
Bacterial Degradation ◽  
Higher Plant ◽  
Rhône River ◽  
Radical Oxidation ◽  
Rhone River

Abstract. Lipid tracers including fatty acids, hydroxyacids, n-alkanols, sterols and triterpenoids were used to determine the origin and fate of suspended particulate organic matter (POM) collected in the Rhone River (France). This seasonal survey (April 2011 to May 2013) revealed a year-round strong terrigenous contribution to the plant-derived particulate organic matter (POM), with significant algal inputs observed in March and attributed to phytoplanktonic blooms likely dominated by diatoms. Major terrigenous contributors to our samples are gymnosperms, and more precisely their roots and stems, as evidenced by the presence of high proportions of ω-hydroxydocosanoic acid (a suberin biomarker). The high amounts of coprostanol detected clearly show that the Rhone River is significantly affected by sewage waters. Specific sterol degradation products were quantified and used to assess the part of biotic and abiotic degradation of POM within the river. Plant-derived organic matter appears to be mainly affected by photo-oxidation and autoxidation (free radical oxidation), while organic matter of human origin, evidenced by the presence of coprostanol, is clearly more prone to bacterial degradation. Despite the involvement of an intense autoxidation-inducing homolytic cleavage of peroxy bonds, a significant proportion of hydroperoxides is still intact in higher plant debris. These compounds could affect the degradation of terrestrial material by inducing an intense autoxidation upon its arrival at sea.

scholarly journals Seasonal survey of the composition and degradation state of particulate organic matter in the Rhône River using lipid tracers

2015 ◽  
Vol 12 (5) ◽  
pp. 1431-1446 ◽  
Author(s):  
M.-A. Galeron ◽  
R. Amiraux ◽  
B. Charriere ◽  
O. Radakovitch ◽  
P. Raimbault ◽  
...  
Keyword(s):  
Organic Matter ◽  
Particulate Organic Matter ◽  
Degradation Products ◽  
Significant Proportion ◽  
Free Radical Oxidation ◽  
Bacterial Degradation ◽  
Higher Plant ◽  
Rhône River ◽  
Radical Oxidation ◽  
Rhone River

Abstract. Lipid tracers including fatty acids, hydroxyacids, n-alkanols, sterols and triterpenoids were used to determine the origin and fate of suspended particulate organic matter (POM) collected in the Rhône River (France). This seasonal survey (April 2011 to May 2013) revealed a year-round strong terrestrial higher-plant contribution to the particulate organic matter (POM), with significant algal inputs observed in March and attributed to phytoplanktonic blooms likely dominated by diatoms. Major terrigenous contributors to our samples are gymnosperms, and more precisely their roots and stems, as evidenced by the presence of high proportions of ω-hydroxydocosanoic acid (a suberin biomarker). The high amounts of coprostanol detected clearly show that the Rhône River is significantly affected by sewage waters. Specific sterol degradation products were quantified and used to assess the part of biotic and abiotic degradation of POM within the river. Higher-plant-derived organic matter appears to be mainly affected by photo-oxidation and autoxidation (free radical oxidation), while organic matter of mammal or human origin, evidenced by the presence of coprostanol, is clearly more prone to bacterial degradation. Despite the involvement of an intense autoxidation-inducing homolytic cleavage of peroxy bonds, a significant proportion of hydroperoxides is still intact in higher plant debris. These compounds could affect the degradation of terrestrial material by inducing an intense autoxidation upon its arrival at sea.

scholarly journals Fluorescence and absorption properties of chromophoric dissolved organic matter (CDOM) in coastal surface waters of the northwestern Mediterranean Sea, influence of the Rhône River

2010 ◽  
Vol 7 (12) ◽  
pp. 4083-4103 ◽  
Author(s):  
J. Para ◽  
P. G. Coble ◽  
B. Charrière ◽  
M. Tedetti ◽  
C. Fontana ◽  
...  
Keyword(s):  
Organic Matter ◽  
Optical Properties ◽  
Mediterranean Sea ◽  
Surface Waters ◽  
Chromophoric Dissolved Organic Matter ◽  
River Plumes ◽  
Rhône River ◽  
Rhone River ◽  
Northwestern Mediterranean Sea ◽  
Northwestern Mediterranean

Abstract. Seawater samples were collected monthly in surface waters (2 and 5 m depths) of the Bay of Marseilles (northwestern Mediterranean Sea; 5°17'30" E, 43°14'30" N) during one year from November 2007 to December 2008 and studied for total organic carbon (TOC) as well as chromophoric dissolved organic matter (CDOM) optical properties (absorbance and fluorescence). The annual mean value of surface CDOM absorption coefficient at 350 nm [aCDOM(350)] was very low (0.10 ± 0.02 m−1) in comparison to values usually found in coastal waters, and no significant seasonal trend in aCDOM(350) could be determined. By contrast, the spectral slope of CDOM absorption (SCDOM) was significantly higher (0.023 ± 0.003 nm−1) in summer than in fall and winter periods (0.017 ± 0.002 nm−1), reflecting either CDOM photobleaching or production in surface waters during stratified sunny periods. The CDOM fluorescence, assessed through excitation emission matrices (EEMs), was dominated by protein-like component (peak T; 1.30–21.94 QSU) and marine humic-like component (peak M; 0.55–5.82 QSU), while terrestrial humic-like fluorescence (peak C; 0.34–2.99 QSU) remained very low. This reflected a dominance of relatively fresh material from biological origin within the CDOM fluorescent pool. At the end of summer, surface CDOM fluorescence was very low and strongly blue shifted, reinforcing the hypothesis of CDOM photobleaching. Our results suggested that unusual Rhône River plume eastward intrusion events might reach Marseilles Bay within 2–3 days and induce local phytoplankton blooms and subsequent fluorescent CDOM production (peaks M and T) without adding terrestrial fluorescence signatures (peaks C and A). Besides Rhône River plumes, mixing events of the entire water column injected relative aged (peaks C and M) CDOM from the bottom into the surface and thus appeared also as an important source of CDOM in surface waters of the Marseilles Bay. Therefore, the assessment of CDOM optical properties, within the hydrological context, pointed out several biotic (in situ biological production, biological production within Rhône River plumes) and abiotic (photobleaching, mixing) factors controlling CDOM transport, production and removal in this highly urbanized coastal area.

scholarly journals Modeling biogeochemical processes in sediments from the Rhône River prodelta area (NW Mediterranean Sea)

2011 ◽  
Vol 8 (1) ◽  
pp. 549-592 ◽  
Author(s):  
L. Pastor ◽  
C. Cathalot ◽  
B. Deflandre ◽  
E. Viollier ◽  
K. Soetaert ◽  
...  
Keyword(s):  
Organic Matter ◽  
Oxygen Consumption ◽  
Continental Shelf ◽  
Carbon Mineralization ◽  
River Mouth ◽  
Total Carbon ◽  
Large Contribution ◽  
Organic Carbon Content ◽  
Rhône River ◽  
Rhone River

Abstract. In-situ oxygen microprofiles, sediment organic carbon content and pore-water concentrations of nitrate, ammonium, iron, manganese and sulfides obtained in sediments from the Rhône River prodelta and its adjacent continental shelf were used to constrain a numerical diagenetic model. Results showed that (1) organic matter from the Rhône River is composed of a fraction of fresh material associated to high first-order degradation rate constants (11–33 yr−1), (2) burial efficiency (burial/input ratio) in the Rhône prodelta (within 3 km of the river outlet) can be up to 80%, and decreases to ~20% on the adjacent continental shelf 10–15 km further offshore (3) there is a large contribution of anoxic processes to total mineralization in sediments near the river mouth, certainly due to large inputs of fresh organic material combined with high sedimentation rates, (4) diagenetic by-products originally produced during anoxic organic matter mineralization are almost entirely precipitated (>97%) and buried in the sediment, which leads to (5) a low contribution of the re-oxidation of reduced products to total oxygen consumption. Consequently, total carbon mineralization rates as based on oxygen consumption rates and using Redfield stoichiometry can be largely underestimated in such River Ocean dominated Margins (RiOMar) environments.

scholarly journals Biogeochemical characterization of the riverine particulate organic matter transferred to the NW Mediterranean Sea

2014 ◽  
Vol 11 (1) ◽  
pp. 157-172 ◽  
Author(s):  
M. Higueras ◽  
P. Kerhervé ◽  
A. Sanchez-Vidal ◽  
A. Calafat ◽  
W. Ludwig ◽  
...  
Keyword(s):  
Organic Matter ◽  
Particulate Organic Matter ◽  
High Water ◽  
Terrestrial Organic Matter ◽  
Rhône River ◽  
Δ13c And Δ15n ◽  
Coastal Rivers ◽  
Rhone River ◽  
Nw Mediterranean ◽  
Nw Mediterranean Sea

Abstract. A large amount of terrestrial organic matter is annually delivered by rivers to the continental shelf, where this material is either degraded, buried or transferred to the deep sea by hydrodynamic processes such as storms. The relative amount of terrestrial organic matter in the marine sediments is often determined by analysing the stable isotopes (δ13C and δ15N) and the C / N ratio of organic matter because the various particulate organic matter (POM) sources have distinct isotopic compositions. With the objective to refine and better interpret POM sources in the marine environment, we have characterized monthly terrestrial POM delivered by eight rivers discharging to the NW Mediterranean Sea: the Rhône, Hérault, Orb, Aude, Têt, Fluvià, Ter and Tordera rivers. These rivers were simultaneously sampled from November 2008 to December 2009 and the concentrations of total suspended matter (TSM), particulate organic carbon (POC) and nitrogen (PN), as well as their stable isotopic ratios (δ13C and δ15N) were determined. During the survey, three rainstorm events with winds coming from the E–NE and the S–SE impacted the NW Mediterranean. Depending on the direction of incoming winds, the fluvial response (amount of water discharge and TSM) was different. Rivers draining the Alps (Rhône River) and Central Massif (Hérault, Orb, and Aude rivers) were mostly impacted by rainstorms associated with winds coming from the S–SE, while rivers draining the Pyrenees (Têt, Fluvià, and Ter rivers) and the Montseny Massif (Tordera River) were impacted by rainstorms associated with winds coming from the E–NE. In addition, the spatial evolution of water discharges shows a different hydrological regime of the Rhône River, with relatively constant and high water stages and TSM concentrations when compared to coastal rivers, characterized by long periods of low water stages. TSM concentrations are positively correlated to water discharges (high water flows resuspended riverbed sediments) but show an inverse relationship with POC and PN relative contents (mostly due to dilution and by low availability of light in river waters during flood events). TSM in most of the coastal rivers have on average 2.5–3 times higher POC and PN mean contents than the Rhône River (8.5 and 1.5%, respectively, for coastal rivers compared to 3.6 and 0.5%, respectively, for the Rhône River). This discrepancy may be caused by the long drought periods in small coastal Mediterranean watersheds that enhance the eutrophication in studied coastal rivers. The δ13C ratios of organic matter also reflect this discrepancy between high and low water stages with values ranging from −33.2 to −24.5‰. The enriched 13C values (−26.3 ± 0.4‰ for the Rhône River and −26.9 ± 1.2‰ for coastal rivers), measured during high water stages, express mostly a mixture of terrestrial source (plant remains and soils) whereas depleted 13C values (∼ −30‰) associated with low water stages exhibit a source with predominant freshwater algae. The high δ15N mean values (>8‰) found in Têt, Ter and Tordera rivers may underline the importance of denitrification processes as a consequence of the eutrophication and anthropogenic impact.

PY-GC-MS analysis of organic matter in suspended material and deposits of the submarine delta of the rhone river (France)

1989 ◽  
Vol 81-82 ◽  
pp. 71-80 ◽  
Author(s):  
A. Puigbo ◽  
F. Gadel ◽  
J.M. Alcaniz ◽  
L. Comellas
Keyword(s):  
Organic Matter ◽  
Suspended Material ◽  
Rhône River ◽  
Ms Analysis ◽  
Rhone River

scholarly journals Depositional Processes of Organic Matter in the Rhône River Delta (Gulf of Lions, France) Traced by Density Fractionation Coupled with Δ14C and δ13C

Radiocarbon ◽  
2013 ◽  
Vol 55 (2) ◽  
pp. 920-931 ◽  
Author(s):  
Flora Toussaint ◽  
Nadine Tisnérat-Laborde ◽  
Cécile Cathalot ◽  
Roselyne Buscail ◽  
Philippe Kerhervé ◽  
...  
Keyword(s):  
Organic Matter ◽  
Stable Carbon Isotopes ◽  
Density Fractionation ◽  
Rhône River ◽  
Density Fraction ◽  
Density Fractions ◽  
Depositional Processes ◽  
Single Station ◽  
Rhone River ◽  
Coastal Sea

As a main source of freshwater and particles, the Rhône River plays a major role in the biogeochemical cycle of organic carbon (OC) in the Mediterranean Sea. To better understand the origin of organic matter and the processes leading to its export to the coastal sea near the Rhône River, we measured radiocarbon (Δ14C) and stable carbon isotopes (δ13C) in the sediments of the delta, after density fractionation. In April 2007, 3 sites located along an offshore transect (A, C, and E) were sampled for surface sediments, and bulk sediment was separated into 4 fractions of different densities (<1.6, 1.6–2, 2–2.5, and >2.5 g cm−3). In order to better understand the evolution of the OC along the transect, we investigated the OC sources and their evolution for each density fraction. Bulk OC shows a large increase in δ13C from −27.2′ nearshore to −24.5′ at offshore stations while Δ14C decreased from 59′ to −320′. The distribution of δ13C with density displayed a convex pattern at all stations. Except for fraction >2.5 g cm−3, δ13C increases by 2.5′ between stations A and E, indicating a loss of terrestrial signature. The distribution of Δ14C versus density had a concave pattern at all stations: at a single station, it showed a large heterogeneity with a difference of 500–600′ between the <1.6 and 2–2.5 g cm−3 fractions. A decrease in Δ14C of −400′ among the different density fractions was observed along the offshore transect. The density fraction >2.5 g cm−3 had less variability, with an average δ13C of −24.6 ± 0.4′ and Δ14C of −370 ± 115′. Several processes may explain this distribution: retention in the prodelta of large particles; mineralization of all fractions during the transport and deposition in the delta and shelf sediments; and dilution of terrestrial particles in continental shelf pool.

scholarly journals Origin of remineralized organic matter in sediments from the Rhone River prodelta (NW Mediterranean) traced by Δ 14 C and δ 13 C signatures of pore water DIC

2018 ◽  
Vol 163 ◽  
pp. 112-122 ◽  
Author(s):  
Lara Pozzato ◽  
Jens Rassmann ◽  
Bruno Lansard ◽  
Jean-Pascal Dumoulin ◽  
Peter van Breugel ◽  
...  
Keyword(s):  
Organic Matter ◽  
Pore Water ◽  
Rhône River ◽  
Rhone River ◽  
Nw Mediterranean

scholarly journals Distribution and lability of land-derived organic matter in the surface sediments of the Rhône prodelta and the adjacent shelf (Mediterranean sea, France): a multi proxy study

2011 ◽  
Vol 8 (2) ◽  
pp. 3353-3402 ◽  
Author(s):  
S. Bourgeois ◽  
A. M. Pruski ◽  
M.-Y. Sun ◽  
R. Buscail ◽  
F. Lantoine ◽  
...  
Keyword(s):  
Amino Acids ◽  
Fatty Acids ◽  
Organic Matter ◽  
Organic Carbon ◽  
Chlorophyll A ◽  
Surface Sediments ◽  
Shelf Area ◽  
Degradation Index ◽  
Rhône River ◽  
Rhone River

Abstract. The Gulf of Lions is a river-dominated ocean margin (RiOMar) that receives high loads of nutrients, sediments and particulate matter from the Rhône river. Most of the particulate materials from the Rhône settle rapidly on the seafloor, this raises the question of the fate of these large quantities of organic carbon delivered to the benthic boundary layer. Surface sediments (0–0.5 cm) were collected in the Rhône prodelta and its adjacent shelf during a period of low river discharge (April 2007, 16 stations). The sources, distribution and lability of sedimentary organic matter was examined using bulk (organic carbon, total nitrogen, grain size) and molecular-level (pigments, amino acids, fatty acids, δ13C of individual fatty acids) analyses. Our results confirmed previous observations of a southwestward Rhodanian imprint in the nearshore sediments. Fatty acid biomarkers and compound-specific δ13C signatures of most fatty acids clearly indicate that the Rhône inputs consist in a mixture of organic matter (OM) from different sources with a strong contribution from terrestrial plants, and a smaller input from freshwater microalgae, mostly diatoms. The influence of the Rhône River was prominent within the first ten kilometers, but may still be observed in the outer shelf (~21 km) as indicated by the occurrence of long chain fatty acids derived from vascular plants and their δ13C signatures. In the proximal prodelta, bacteria-specific fatty acids were abundant (1.65 mg g−1OC at the mouth site) and were relatively depleted in δ13C confirming that bacteria preferentially utilize terrestrial OM in this area. In the shelf area, the inputs of marine OM and its preferential utilization by the bacteria was confirmed, but the coupling between the pelagic and the benthic compartments appeared limited at this period of the year. Overall, degradation indexes based on amino acids (Dauwe's degradation index) and pigments (ratio of intact chlorophyll-a to the sum of chlorophyll-a + phaeopigment-a), as well as isotopic enrichment of source-specific fatty acids reveal an offshore gradient of OM decay reflecting the rapid deposition of the terrestrial material in the prodelta, the low mixing with OM deriving from marine sources and the efficient degradation of the OM once deposited. Terrestrial OM is usually considered as being refractory due to the presence of structural polymers and its advanced stage of degradation. However, the OM delivered by the Rhône is relatively labile as shown by the intermediary value of Dauwe's degradation index (DI = +0.1), the high proportion of bio-available nitrogen and the occurrence of polyunsaturated fatty acids. Deltaic sediments off the Rhône river should thus be of sufficiently high nutritional quality to sustain dense macrofaunal communities.

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