Characterization of dissolved organic nitrogen in wet deposition from Lake Erhai basin by using ultrahigh resolution FT-ICR mass spectrometry

Feng, Shuang; Zhang, Li; Wang, Shengrui; Nadykto, Alexey B.; Xu, Yisheng; Shi, Quan; Jiang, Bin; Qian, Wei

doi:10.1016/j.chemosphere.2016.04.039

Cited by 25 publications

(16 citation statements)

References 38 publications

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“…They can positively shift the net direct radiation forcing (DRF) (Saleh et al, 2014;Laskin et al, 2015;Kirchstetter and Thatcher, 2012). According to a simulation model, the inclusion of BrC may enhance total aerosol absorption by 7 %-19 % (Feng et al, 2013). According to previous studies, BrC in atmospheric aerosols mainly originates from emissions from biomass burning (BB) and coal combustion (CC), vehicle exhaust, and the formation of secondary organic aerosol (SOA) (Zhu et al, 2018;Laskin et al, 2015;Xie et al, 2017;Kumar et al, 2018).…”

Section: Introductionmentioning

confidence: 99%

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

et al. 2020

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Abstract. Brown carbon (BrC) plays an essential impact on radiative forcing due to its ability to absorb sunlight. In this study, the optical properties and molecular characteristics of water-soluble and methanol-soluble organic carbon (OC; MSOC) emitted from the simulated combustion of biomass and coal fuels and vehicle emissions were investigated using ultraviolet–visible (UV–vis) spectroscopy, excitation–emission matrix (EEM) spectroscopy, and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). The results showed that these smoke aerosol samples from biomass burning (BB) and coal combustion (CC) had a higher mass absorption efficiency at 365 nm (MAE365) than vehicle emission samples. A stronger MAE365 value was also found in MSOC than water-soluble organic carbon (WSOC), indicating low polar compounds would possess a higher light absorption capacity. Parallel factor (PARAFAC) analysis identified six types of fluorophores (P1–6) in WSOC including two humic-like substances (HULIS-1) (P1 and P6), three protein-like substances (PLOM) (P2, P3, and P5), and one undefined substance (P4). HULIS-1 was mainly from aging vehicle exhaust particles; P2 was only abundant in BB aerosols; P3 was ubiquitous in all tested aerosols; P4 was abundant in fossil burning aerosols; and P5 was more intense in fresh vehicle exhaust particles. The MSOC chromophores (six components; C1–6) exhibited consistent characteristics with WSOC, suggesting the method could be used to indicate the origins of chromophores. FT-ICR mass spectra showed that CHO and CHON were the most abundant components of WSOC, but S-containing compounds appeared in a higher abundance in CC aerosols and vehicle emissions than BB aerosols, while considerably fewer S-containing compounds largely with CHO and CHON were detected in MSOC. The unique formulas of different sources in the van Krevelen (VK) diagram presented different molecular distributions. To be specific, BB aerosols with largely CHO and CHON had a medium H ∕ C and low O ∕ C ratio, while CC aerosols and vehicle emissions largely with S-containing compounds had an opposite H ∕ C and O ∕ C ratio. Moreover, the light absorption capacity of WSOC and MSOC was positively associated with the unsaturation degree and molecular weight in the source aerosols. The above results are potentially applicable to further studies on the EEM-based or molecular-characteristic-based source apportionment of chromophores in atmospheric aerosols.

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Section: Introductionmentioning

confidence: 99%

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

et al. 2020

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“…These nutrients could accumulate on benthic biofilms and be used by bacterial communities [36,[54][55][56]. In Erhai watershed, streams pass through mountain areas and urbanized areas, which causes significant differences of water quality in these heterogeneity ecosystems under different degrees of human activities perturbations [23]. Under these heterogeneity stream ecosystems, physicochemical-factor provides a diverse environment for bacterial communities [52,57], and DOC, NO 3 − , SRP, and TP provide available nutrients for bacterial growth [40,58].…”

Section: Discussionmentioning

confidence: 99%

“…Erhai Lake is the second largest plateau lake and the seventh largest freshwater lake in China. This lake has valuable functions in supporting human life and regional development, including drinkable water supply, agricultural irrigation, climate regulation, tourism, and hydroelectric power generation [21][22][23]. Anthropogenic activities in the basin generate a large amount of nutrients and waste, which directly perturb biogeochemical cycles and accelerate whole-basin ecosystem deterioration [24].…”

Section: Introductionmentioning

confidence: 99%

Impact of Nutrient and Stoichiometry Gradients on Microbial Assemblages in Erhai Lake and Its Input Streams

Liu

Elser

et al. 2019

Water

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Networks of lakes and streams are linked by downslope flows of material and energy within catchments. Understanding how bacterial assemblages are associated with nutrients and stoichiometric gradients in lakes and streams is essential for understanding biogeochemical cycling in freshwater ecosystems. In this study, we conducted field sampling of bacterial communities from lake water and stream biofilms in Erhai Lake watershed. We determined bacterial communities using high-throughput 16S rRNA gene sequencing and explored the relationship between bacterial composition and environmental factors using networking analysis, canonical correspondence analysis (CCA), and variation partitioning analysis (VPA). Physicochemical parameters, nutrients, and nutrient ratios gradients between the lake and the streams were strongly associated with the differences in community composition and the dominant taxa. Cyanobacteria dominated in Erhai Lake, while Proteobacteria dominated in streams. The stream bacterial network was more stable with multiple stressors, including physicochemical-factors and nutrient-factors, while the lake bacterial network was more fragile and susceptible to human activities with dominant nutrients (phosphorus). Negative correlations between bacterial communities and soluble reactive phosphorus (SRP) as well as positive correlations between bacterial communities and dissolved organic carbon (DOC) in the network indicated these factors had strong effect on bacterial succession. Erhai Lake is in a eutrophic state, and high relative abundances of Synechococcus (40.62%) and Microcystis (16.2%) were noted during the course of our study. CCA indicated that nutrients (phosphorus) were key parameters driving Cyanobacteria-dominated community structure. By classifying the environmental factors into five categories, VPA analyses identified that P-factor (total phosphorus (TP) and SRP) as well as the synergistic effect of C-factor (DOC), N-factor (NO3−), and P-factor (TP and SRP) played a central role in structuring the bacterial communities in Erhai Lake. Heterogeneous physicochemical conditions explained the variations in bacterial assemblages in streams. This study provides a picture of stream–lake linkages from the perspective of bacterial community structure as well as key factors driving bacterial assemblages within lakes and streams at the whole watershed scale. We further argue that better management of phosphorus on the watershed scale is needed for ameliorating eutrophication of Erhai Lake.

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“…The combination of Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI) and EEM is a powerful platform for characterizing BrC chromophores, and is expected to enable us to deduce the molecular compositions of these chromophores. FT-ICR MS has been successfully used to characterize organic aerosol (Jiang et al, 2016;Song et al, 2018;Mo et al, 2018), cloud water (Zhao et al, 2013), and natural organic matter (Sleighter et al, 2012;Feng et al, 2016). The ultrahigh resolution, accuracy of mass measurements, and high sensitivity make this technique suitable for studying complex mixtures at the molecular level, and for identifying the chemical compositions of the substances being studied with a high degree of confidence (Feng et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

Molecular compositions and optical properties of dissolved brown carbon in smoke particles illuminated by excitation-emission matrix spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis

Tang

et al. 2019

Preprint

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<p><strong>Abstract.</strong> We investigated the fluorescence and chemical-structural characteristics of dissolved brown carbon (BrC) in smoke particulates emitted from the combustion of biomass and fossil fuels (coal and vehicle exhaust) by excitation-emission matrix (EEM) spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). Six components were resolved by parallel factor analysis (PARAFAC) of the water-soluble and methanol-soluble organic carbon (MSOC) fractions, respectively. These fluorescent components varied among sources. Combined with FT-ICR MS ion groups, we found that the fluorescent components agreed well with the functional groups, particularly with nitrogen (N)- and sulfur (S)-containing groups. Among the six PARAFAC components (P1&#8211;6) retrieved from the water-soluble organic carbon (WSOC) fraction, except for the P3 component, the other components exhibited different values among the three types of emission sources tested. Vehicle exhaust was characterized by high P1 and P6 components, which are mainly associated with aromatic organosulfate compounds, and a high P5 component, mainly associated with sulfonates; coal combustion was characterized by a high P4 component, which is associated with nitrooxy-organosulfate (nitrooxy-OS) compounds; and biomass burning was characterized by the P2 component. Similar results were observed in the case of the MSOC fraction. This study reveals the source contribution and possible structures of previously unclear excitation-emission matrix (EEM) fluorescent components in combustion-derived aerosols. These are the first findings of this type and are potentially applicable to further studies on EEM-based source apportionment of dissolved BrC in aerosols.</p>

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Characterization of dissolved organic nitrogen in wet deposition from Lake Erhai basin by using ultrahigh resolution FT-ICR mass spectrometry

Cited by 25 publications

References 38 publications

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

Impact of Nutrient and Stoichiometry Gradients on Microbial Assemblages in Erhai Lake and Its Input Streams

Molecular compositions and optical properties of dissolved brown carbon in smoke particles illuminated by excitation-emission matrix spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis

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