Temporal and spatial variations of three dimethylated sulfur compounds in the Changjiang Estuary and its adjacent area during summer and winter

2017 ◽  
Vol 14 (3) ◽  
pp. 160 ◽  
Author(s):  
Nan Gao ◽  
Gui-Peng Yang ◽  
Hong-Hai Zhang ◽  
Long Liu

Environmental contextDimethylsulfide is a biogeochemically important sulfur gas emitted from the oceans that can lead to aerosol formation, thereby affecting earth albedo and climate. Studies on the biogeochemistry of dimethylsulfide and its precursors and oxidation products in coastal waters can link the atmospheric chemistry of dimethylsulfide with the bioavailable organic sulfur pool in the oceans. The ensuing information is essential for understanding the biogeochemical dynamics of sulfur and its global cycles. AbstractThe spatiotemporal distribution patterns of dimethylsulfide (DMS), dimethylsulfoniopropionate (DMSP), dimethylsulfoxide (DMSO) and chlorophyll a (Chl-a), as well as the oceanographic parameters influencing the concentrations of DMS, DMSP and DMSO, were measured in the Changjiang Estuary and its adjacent area during two cruises from 21 February to 10 March 2014 and from 10 to 22 July 2014. The concentrations of DMS and DMSP showed significant seasonal variation, i.e. higher values in summer than in winter. This result corresponded well with the seasonal change in Chl-a in the study area. The distribution of dissolved DMSO (DMSOd) decreased significantly with distance from shore, suggesting a primary source of terrestrial and riverine inputs. The seasonal variations of both DMSOd and particulate DMSO (DMSOp) were weaker than other sulfur compounds. Significant relationships were observed between DMS, particulate DMSP (DMSPp), DMSOp and Chl-a, suggesting that phytoplankton biomass plays an important role in controlling the distributions of DMS, DMSP and DMSO in the study area. The positive relationship between DMSPp and DMSOp suggested similar sources and cellular functions in algae, whereas the oxidation of DMS to DMSOd appeared to be a predominant source of DMSOd in winter in the area adjacent to the river mouth. The average sea-to-air fluxes of DMS in the Changjiang Estuary and its adjacent area were 0.37 and 1.70 µmol m–2 day–1 in winter and summer respectively; these values are much lower than those in other continental shelf seas.

2009 ◽  
Vol 9 (3) ◽  
pp. 13629-13653 ◽  
Author(s):  
T. Karl ◽  
A. Guenther ◽  
A. Turnipseed ◽  
P. Artaxo ◽  
S. Martin

Abstract. Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian aerosol characterization experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. A recently suggested novel pathway for isoprene peroxy radicals could explain the observed discrepancy and reconcile the rapid formation of these VOCs. Furthermore, if generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in substantial underestimates of modelled OH reactivity that could explain a major fraction of the missing OH sink over forests which has previously been attributed to a missing source of primary biogenic VOCs.


2019 ◽  
Vol 7 (9) ◽  
pp. 320 ◽  
Author(s):  
Chen ◽  
Liu ◽  
Xu ◽  
Wang

Particulate organic carbon (POC) plays an important role in the global carbon cycle. The POC in the Changjiang Estuary and adjacent coastal region of the East China Sea (ECS) is dominated by riverine input and marine production and is significantly influenced by the three gorges project (TGP). A coupled physical–biogeochemical model was used to evaluate TGP’s impact on POC. The results demonstrate that TGP regulates the area influenced by diluted water and POC through direct river and sediment discharge and affects the ecosystem. From the early to later TGP construction periods, the surface region with high-POC concentration (>40 μmol L−1) decreases by 20.5% in area and 11.5% in concentration. Meanwhile, POC in the whole water column decreases from 19.5 to 17.8 μmol L−1. By contrast, the concentrations of chlorophyll-a (Chl-a) and related nutrients increase. A three end-member mixing model based on quasi-conservative temperature and salinity is used to quantify relative contributions of different water sources to POC in our research area. We also estimate the biological POC production by the difference between the physical-biogeochemical model predicted POC and three end-member model mixing POC. The result demonstrate that under the regulation of TGP in the later period, the decrease of sediment load increases water transparency, which favors photosynthesis and oceanic biological produced POC. In addition, over 70% of the areas have C/Chl-a > 200 and high C/N ratios, which are circumstantial evidences that organic detritus and terrestrial input sources still dominate in the Changjiang Estuary and adjacent coastal ECS but are influenced by TGP’s regulation.


2009 ◽  
Vol 9 (20) ◽  
pp. 7753-7767 ◽  
Author(s):  
T. Karl ◽  
A. Guenther ◽  
A. Turnipseed ◽  
G. Tyndall ◽  
P. Artaxo ◽  
...  

Abstract. Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian Aerosol Characterization Experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. Recently reported fast secondary production could explain 50% of the observed discrepancy with the remaining part possibly produced via a novel primary production channel, which has been proposed theoretically. The observations of OVOCs are also used to test a recently proposed HOx recycling mechanism via degradation of isoprene peroxy radicals. If generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in uncertainties of modelled OH reactivity, potentially explaining a fraction of the missing OH sink over forests which has previously been largely attributed to a missing source of primary biogenic VOCs.


2005 ◽  
Vol 5 (10) ◽  
pp. 2761-2770 ◽  
Author(s):  
I. Kourtchev ◽  
T. Ruuskanen ◽  
W. Maenhaut ◽  
M. Kulmala ◽  
M. Claeys

Abstract. Oxidation products of isoprene including 2-methyltetrols (2-methylthreitol and 2-methylerythritol), 2-methylglyceric acid and triol derivatives of isoprene (2-methyl-1,3,4-trihydroxy-1-butene (cis and trans) and 3-methyl-2,3,4-trihydroxy-1-butene) have been detected in boreal forest PM1 aerosols collected at Hyytiälä, southern Finland, during a 2004 summer period, at significant atmospheric concentrations (in total 51 ng m−3 in summer versus 0.46 ng m−3 in fall). On the basis of these results, it can be concluded that photo-oxidation of isoprene is an important atmospheric chemistry process that contributes to secondary organic aerosol formation during summer in this conifer forest ecosystem. In addition to isoprene oxidation products, malic acid, which can be regarded as an intermediate in the oxidation of unsaturated fatty acids, was also detected at high concentrations during the summer period (46 ng m−3 in summer versus 5.2 ng m−3 in fall), while levoglucosan, originating from biomass burning, became relatively more important during the fall period (29 ng m−3 in fall versus 10 ng m−3 in summer). Pinic acid, a major photo-oxidation product of α-pinene in laboratory experiments, could only be detected at trace levels in the summer samples, suggesting that further oxidation of pinic acid occurs and/or that different oxidation pathways are followed. We hypothesize that photo-oxidation of isoprene may participate in the early stages of new particle formation, a phenomenon which has been well documented in the boreal forest environment.


2008 ◽  
Vol 8 (4) ◽  
pp. 13619-13632
Author(s):  
S. N. Matsunaga ◽  
A. B. Guenther ◽  
M. J. Potosnak ◽  
E. C. Apel

Abstract. Biogenic volatile organic compounds (BVOC) produced by plants are known to have an important role in atmospheric chemistry. However, our knowledge of the range of BVOCs produced by different plant processes is still expanding, and there remain poorly understood categories of BVOCs. In this study, emissions of a novel class of BVOC emissions were investigated in a desert region. Our study considered 8 species of common desert plants: blackbrush (Coleogyne ramosissima), desert willow (Chilopsis linearis), mesquite (Prosopis glandulosa), mondel pine (Pinus eldarica), pinyon pine (Pinus monophylla), cottonwood (Populus deltoides), saguaro cactus (Carnegiea gigantea) and yucca (Yucca baccata). The measurements focused on BVOCs with relatively high molecular weight (>C15) and/or an oxygenated functional group. Significantly high emission rates of two salicylic esters were found for blackbrush, desert willow and mesquite with emission rates of 1.4, 2.1 and 0.46 μgC dwg−1 h−1, respectively. The salicylic esters were identified as 2-ethylhexenyl salicylate (2-EHS) and 3,3,5-trimethylcyclohexenyl salicylate (homosalate) and are known as effective ultraviolet (UV) absorbers. We propose that the plants derive a protective benefit against UV radiation from the salicylic esters and that the emission process is driven by the physical evaporation of the salicylic esters due to the high ambient temperatures. In addition, the salicylic esters are predicted to be an effective precursor of secondary organic aerosol (SOA) because of their low vapor pressure due to a high number of carbon atoms (15 or 16) and the presence of three oxygen atoms. We estimated the contribution of the sunscreen esters themselves and their oxidation products on the SOA formation for the Las Vegas region using a BVOC emission model. The contribution was estimated to reach 90% of the biogenic SOA in the landscapes dominated by desert willow and mesquite and 25% in Las Vegas area.


2010 ◽  
Vol 7 (3) ◽  
pp. 3125-3151 ◽  
Author(s):  
G.-L. Zhang ◽  
J. Zhang ◽  
S.-M. Liu ◽  
J.-L. Ren ◽  
Y.-C. Zhao

Abstract. Dissolved nitrous oxide (N2O) was measured in the waters of the Changjiang (Yangtze River) Estuary and its adjacent marine area during five surveys covering the period of 2002–2006. Dissolved N2O concentrations ranged from 6.04 to 21.3 nM, and indicate seasonal variations with high values occurring in summer and spring. Dissolved riverine N2O was observed monthly at station Xuliujing of the Changjiang, and ranged from 12.4 to 33.3 nM with an average of 20.8±7.8 nM. The average annual input of N2O from the Changjiang to the estuary and its adjacent area was estimated to be 15.8×106 mol/yr. N2O emission rates from the sediments of the Changjiang Estuary in spring ranged from −1.88 to 2.02 μmol m−2 d−1, which suggest that sediment can act as either a source or a sink of N2O in the Changjiang Estuary. The annual sea to air N2O fluxes from the Changjiang Estuary were estimated to be 6.8±3.7, 13.3±7.2 and 14.9±8.3 μmol m−2 d−1 using LM86, W92 and RC01 relationships, respectively. The annual sea to air N2O fluxes from the adjacent marine area were estimated to be 8.5±7.8, 15.3±13.5 and 17.4&plusmn15.7 μmol m−2 d−1 using LM86, W92 and RC01 relationship, respectively. Hence the Changjiang Estuary and its adjacent marine area is a net source of atmospheric N2O.


2005 ◽  
Vol 5 (3) ◽  
pp. 2947-2971 ◽  
Author(s):  
I. Kourtchev ◽  
T. Ruuskanen ◽  
W. Maenhaut ◽  
M. Kulmala ◽  
M. Claeys

Abstract. Oxidation products of isoprene including 2-methyltetrols (2-methylthreitol and 2-methylerythritol), 2-methylglyceric acid and triol derivatives of isoprene (2-methyl-1,3,4-trihydroxy-1-butene (cis and trans) and 3-methyl-2,3,4-trihydroxy-1-butene) have been detected in boreal forest PM1 aerosols collected at Hyytiälä, southern Finland, during a 2004 summer period, at significant atmospheric concentrations (in total 51 ng m-3 in summer versus 0.46 ng m-3 in fall). On the basis of these results, it can be concluded that photo-oxidation of isoprene is an important atmospheric chemistry process that contributes to secondary organic aerosol formation during summer in this conifer forest ecosystem. In addition to isoprene oxidation products, malic acid, which can be regarded as an end-oxidation product of unsaturated fatty acids, was also detected at high concentrations during the summer period (46 ng m-3 in summer versus 5.2 ng m-3 in fall), while levoglucosan, originating from biomass burning, became relatively more important during the fall period (29 ng m-3 in fall versus 10 ng m-3 in summer). Pinic acid, a major photo-oxidation product of α-pinene in laboratory experiments, could only be detected at trace levels in the summer PM1 aerosol samples from Hyytiälä, suggesting that further oxidation of pinic acid occurs and/or that different oxidation pathways are followed. We hypothesize that photo-oxidation of isoprene may participate in the early stages of new particle formation, a phenomenon which has been well documented in the boreal forest environment.


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