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Humic-like substances (HULIS) are macromolecular complex groups in water-soluble organic compounds (WSOC). pH is a crucial factor that influences the chemical transformations of HULIS in atmospheric particles, but this has been rarely investigated, especially under varying pH conditions. This study attempted to unveil the chemical transformation mechanisms of HULIS under a range of pH conditions using optical methods. The pH-dependent light absorption and fluorescence properties of HULIS were comprehensively analyzed; the acidity coefficient (p

Bioaccumulation of methylmercury (MeHg) in rice grains has been an emerging issue of human health, but the mechanism of bioaccumulation is still poorly understood. Mercury (Hg) isotope measurements are powerful tools for tracing the sources and biogeochemical cycles of Hg in the environment. In this study, MeHg compound-specific stable isotope analysis (CSIA) was developed in paddy soil and rice plants to trace the biogeochemical cycle of Hg in a paddy ecosystem during the whole rice-growing season. Isotopic fractionation was analyzed separately for MeHg and inorganic Hg (IHg). Results showed distinct isotopic signals between MeHg and IHg in rice plants, indicating different sources. δ202Hg values of MeHg showed no significant differences between roots, stalks, leaves, and grains at each growth stage. The similar Δ199Hg values of MeHg between rice tissues (0.14 ± 0.08‰, 2SD, n = 12), soil (0.13 ± 0.03‰, 2SD, n = 4), and irrigation water (0.17 ± 0.09‰, 2SD, n = 5) suggested that the soil-water system was the original source of MeHg in rice plants. Δ199Hg values of IHg in the paddy ecosystem indicated that water, soil, and atmosphere contributed to IHg in grains, leaves, stalks, and roots with varying degree. This study demonstrates that successful application of MeHg CSIA can improve our understanding of the sources and bioaccumulation mechanisms of MeHg and IHg in the paddy ecosystems.

This study demonstrates a new approach to examine the chemical interaction between fluorophores and acid/base functional groups in water-soluble organic compounds (WSOC) of particulate matter (PM2....

Organic soil is an important transient reservoir of mercury (Hg) in terrestrial ecosystems, but the fate of deposited Hg in organic forest soil is poorly understood. To understand the dynamic changes of deposited Hg on forest floor, the composition of stable Hg and carbon (C) isotopes in decomposing litters and organic soil layer was measured to construct the 500 year history of postdepositional Hg transformation in a subtropical evergreen broad-leaf forest in Southwest China. Using the observational data and a multiprocess isotope model, the contributions of microbial reduction, photoreduction, and dark reduction mediated by organic matter to the isotopic transition were estimated. Microbial reduction and photoreduction play a dominant role in the initial litter decomposition during first 2 years. Dark redox reactions mediated by organic matter become the predominant process in the subsequent 420 years. After that, the values of Hg mass dependent fractionation (MDF), mass independent fractionation (MIF), and Δ

Brown carbon (BrC), an aerosol carbonaceous matter component, impacts atmospheric radiation and global climate because of its absorption in the near-ultraviolet-visible region. Simultaneous air sampling was conducted in two megacities of Xi'an (northern) and Hong Kong (southern) in China in winter of 2016-2017. The aim of this study is to determine and characterize the BrC compounds in collected filter samples. Characteristic absorption peaks corresponding to aromatic C-C stretching bands, organo-nitrates, and C═O functional groups were seen in spectra of Xi'an samples, suggesting that the BrC was derived from freshly smoldering biomass and coal combustion as well as aqueous formation of anthropogenic secondary organic carbon. In Hong Kong, the light absorption of secondary BrC accounted for 76% of the total absorbances of BrC. The high abundance of strong C═O groups, biogenic volatile organic compounds (BVOCs) and atmospheric oxidants suggest secondary BrC was likely formed from photochemical oxidation of BVOCs in Hong Kong. Several representative BrC molecular markers were detected using Fourier transform ion cyclotron resonance mass spectrometry and their absorption properties were simulated by quantum chemistry. The results demonstrate that light absorption capacities of secondary anthropogenic BrC with nitro-functional groups were stronger than those of biogenic secondary BrC and anthropogenic primary BrC.

Lead (Pb) emissions into the atmosphere from anthropogenic sources have attracted considerable attention due to lead’s high toxicity and associated human health and environmental impacts. Pb emissi...

Coal combustion has represented a very important atmospheric mercury (Hg) source in the past 5 decades, especially in eastern Asia. Compared with coal-fired power plants (CFPPs) and industrial boil...

Isotopic composition of atmospheric particulate bound mercury (PBM) was obtained at four remote sites in different geographical regions of China for three to 12 month periods. Mean (±1σ) Δ199HgPBM was the highest at the site in southwestern China (0.66 ± 0.32‰), followed by the site in northeastern China (0.36 ± 0.34‰), the site in the marine boundary layer of East China Sea (0.35 ± 0.33‰), and was the lowest at the site in northwestern China (0.27 ± 0.22‰). Δ199HgPBM was relatively higher in cold than warm season at the sites in northwestern and southwestern China, whereas the opposite was found at the site in northeastern China. We propose that the seasonal variations of Δ199HgPBM were influenced by the exposure of air masses to regional (e.g., anthropogenic and dust related) and long-range (e.g., anthropogenic and oceanic) sources in the preceding several days, with the former characterized by lower Δ199HgPBM and the latter characterized by more positive Δ199HgPBM due to sufficient atmospheric transformations. Modeling results from Potential Source Contribution Function suggested that domestic anthropogenic emission was the major contributor to PBM pollution at the sites in northeastern and eastern China, whereas long-range transboundary transport of PBM from South Asia played a more important role at the sites in southwestern and northwestern China.

This study produced gridded deposition estimates of polycyclic aromatic compounds (PACs), including 17 polycyclic aromatic hydrocarbons (PAHs), 21 alkylated PAHs (alk-PAHs), and 5 dibenzothiophenes (DBTs), over the oil sands region of Alberta, Canada and surrounding communities. Gridded annual total deposition of PACs in 2011 ranged from 55 to 175 000 μg m

To assess the relative contributions of traffic emission and other potential sources to high levels of atmospheric ammonia (NH3) in urban areas in the wintertime, atmospheric NH3 and related pollutants were measured at an urban site, ∼300 m from a major traffic road, in northern China in November and December 2015. Hourly average NH3 varied from 0.3 to 10.8 ppb with an average of 2.4 ppb during the campaign. Contrary to the common perspective in literature, traffic emission was demonstrated to be a negligible contributor to atmospheric NH3. Atmospheric NH3 correlated well with ambient water vapor during many time periods lasting from tens of hours to several days, implying NH3 released from water evaporation is an important source. Emissions from local green space inside the urban areas were identified to significantly contribute to the observed atmospheric NH3 during ∼60% of the sampling times. Evaporation of predeposited NHx through wet precipitation combined with emissions from local green space likely...

Gaseous oxidized mercury (GOM) measurement uncertainties undoubtedly impact the understanding of mercury biogeochemical cycling; however, there is a lack of consensus on the uncertainty magnitude. The numerical method presented in this study provides an alternative means of estimating the uncertainties of previous GOM measurements. Weekly GOM in ambient air was predicted from measured weekly mercury wet deposition using a scavenging ratio approach, and compared against field measurements of 2-4 hly GOM to estimate the measurement biases of the Tekran speciation instruments at 13 Atmospheric Mercury Network (AMNet) sites. Multiyear average GOM measurements were estimated to be biased low by more than a factor of 2 at six sites, between a factor of 1.5 and 1.8 at six other sites, and below a factor of 1.3 at one site. The differences between predicted and observed were significantly larger during summer than other seasons potentially because of higher ozone concentrations that may interfere with GOM sampling. The analysis data collected over six years at multiple sites suggests a systematic bias in GOM measurements, supporting the need for further investigation of measurement technologies and identifying the chemical composition of GOM.