Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

The gaseous or particulate forms of divalent mercury (Hg^II) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux (FLX). In the new nested-grid GEOS-Chem model, we try to modify the Hg^II gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg (GOM), particulate-bound Hg (PBM), and PM_2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature (T) and organic aerosol (OA) concentrations under different relative humidity (RH). Results showed that with increasing RH, the dominant process of Hg^II gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of Hg^II gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases (NMBs) of monthly gaseous element mercury (GEM), GOM, PBM, WFLX were reduced from −33%–29%, 95%–300%, 64%–261%, 117%–122% to −13%–0%, −20%–80%, −31%–50%, −17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.     

Peroxymonosulfate enhanced photoelectrocatalytic oxidation of organic contaminants and simultaneously cathodic recycling of silver

Degradation of organic contaminants with simultaneous recycling of Ag⁺ from silver-containing organic wastewater such as photographic effluents is desired. Although photoelectrocatalysis (PEC) technology is a good candidate for this type of wastewater, its reaction kinetics still needs to be improved. Herein, peroxymonosulfate (PMS) was employed to enhance the PEC kinetics for oxidation of phenol (PhOH) at the anode and reduction of Ag⁺ at the cathode. The degradation efficiency of phenol (PhOH, 0.1 mmol/L) was increased from 42.8% to 96.9% by adding 5 mmol/L PMS at a potential of 0.25 V. Meanwhile, the Ag (by wt%) deposited on the cathode was 28.1% (Ag₂O) in PEC process, while that of Ag (by wt%) was 69.7% (Ag⁰) by adding PMS. According to the electrochemistry analysis, PMS, as photoelectrons acceptor, enhances the separation efficiency of charges and the direct h⁺ oxidation of PhOH at the photoanode. Meantime, the increasing cathode potential avoided H₂ evolution and strongly alkaline at the surface of cathode, thus enabling the deposition of Ag⁺ in the form of metallic silver with the help of PMS. In addition, PMS combined with PEC process was effective in treating photographic effluents.     

Reducing ammonia gas from chicken manure with lime and soybean plants

This research is aimed at addressing the complaints of local people living near chicken farms who are disturbed by odors caused by livestock activities, and specifically, by the generation of ammonia gas from chicken manure. Methods that are expected to reduce the intensity of ammonia gas odors include both scattering lime on the surface of the soil and planting soybeans around the cages. The results obtained showed a reduction in the levels of ammonia gas by 57.48%–from 1.67 parts per million (ppm) near an untreated cage to 0.71 ppm near the cage that achieved the best results. The study found that spreading lime evenly over the chicken manure was the most effective method that farmers could use to reduce ammonia odors. The sample area treated by the addition of soybean plants showed a reduction in the levels of ammonia gas from 1.67 to 0.78 ppm.     

Mesoscale variability of organic matter composition in nw adriatic sediments

We investigated the spatial variability of sediment organic matter content and composition in three areas (A, B and C) of the Northwestern Adriatic Sea, subjected to a putative gradient of trophic state ( i.e. , increasing distance from the Po river outflow) in order to determine the appropriate sample size and replication. The analysis of the mesoscale variability was carried out comparing variability on the scale of meters ( i.e. among different deployments) with the variability observed on a scale of several kilometres ( i.e. among different sampling areas). Sediment samples, collected on April 1999, October 1999, April and October 2000, were analysed for chloropigment content (chlorophyll-a and phaeopygments) and protein, carbohydrate and lipid concentrations. Chloropigment, protein, carbohydrate and lipid concentrations were high, indicating that this system shares trophic conditions typical of highly productive environments. All organic matter components displayed a distribution independent from the increasing distance from the Po river outflow and a clear spatial variability, characterised by significant differences among different areas, but not among deployments. Carbohydrates were the biochemical compound displaying the highest spatial variability among the three areas. Chloropigment, protein, carbohydrate and lipid concentrations displayed also significant temporal changes. When spatial and temporal variability were compared, chlorophyll-a, phaeopigment and protein concentrations displayed a higher temporal than spatial variability. Conversely, for carbohydrates and lipids spatial and temporal variability was of the same order of magnitude. Organic matter composition displayed limited changes among areas, but a strong temporal variability. The results from the Adriatic sea suggest that analyses from sediments collected from a single deployment are sufficient for assessing organic matter concentration and composition over areas of several hundreds of square meters. However, for estimating organic matter composition over larger spatial scales ( i.e. miles) the identification of different sampling areas is needed.     

Effect of sulfur and composted manure on SO4-S,P and micronutrient availability in a calcareous saline–sodic soil

A factorial design with different levels of elemental S and cow manure was used to investigate the effects of S and manure on SO₄-S, P and micronutrient availability in a calcareous saline–sodic soil. The results revealed that the recovery of SO₄-S increased significantly (p≤0.05) in all treatments as elemental S increased, particularly when in combination with manure. The interactional effects of S° and manure application rates resulted in a decrease in soil pH of 0.1 to 0.9 units and increases in soil EC from 0.1 to 2.6 dS m^?1 as result of an increase in the number of oxidisers and the oxidation rate of elemental S. Application of S° in combination with manure led to an increase in soil-available-P (0.6–40 mg kg^?1), DTPA-Zn (0.2–3.9 mg kg^?1) and DTPA-Fe (0.1–5.6 mg kg^?1).     

Comparing measured and modelled forest carbon stocks in high-boreal forests of harvest and natural-disturbance origin in Labrador, Canada

Understanding the effects of disturbance regimes on carbon (C) stocks and stock changes is a prerequisite to estimating forest C stocks and fluxes. Live-tree, dead-tree, woody debris (WD), stump, buried wood, organic layer, and mineral soil C stock data were collected from high-boreal black spruce (Picea mariana (Mill.) B.S.P.) stands of harvest and fire origin and compared to values predicted by the Carbon Budget Model of the Canadian Forest Sector (CBM-CFS3); the core model of Canada's National Forest Carbon Monitoring, Accounting and Reporting System. Data comparing the effect of natural and anthropogenic disturbance history on forest C stocks are limited, but needed to evaluate models such as the CBM-CFS3. Results showed that adjustments to the CBM-CFS3 volume-to-biomass conversion and partitioning parameters were required for the non-merchantable and branch C pools to accurately capture live-tree C stocks in the studied black spruce ecosystems. Accuracy of the CBM-CFS3 modelled estimates of dead organic matter and soil C pools was improved relative to regional default parameters by increased snag fall and >10 cm WD base decay rates. The model evaluation process also highlighted the importance of developing a bryophyte module to account for bryophyte C dynamics and the physical burial of woody debris by bryophytes. Modelled mineral soil C estimates were improved by applying a preliminary belowground slow C pool base decay rate optimized for the soil type of the studied sites, Humo-Ferric Podzols.     

“生物有效性测量”与“全沉积物毒性识别评估(TIE)”联用有效识别出沉积物中主要致毒污染物

沉积物中污染物种类繁多,准确判断其中产生生物毒性的主要来源是个难点,本文作者先采用TIE法初步判断出主要致毒污染物为有机物和重金属(毒性描述阶段(相I)),传统的毒性单位分析结果显示Cr、Cu、Ni、Pb和Zn主要致毒重金属,而为氯氰菊酯、氯氟氰菊酯、溴氰菊酯和氟虫腈为主要致毒有机物中(毒性鉴定阶段(相II))。采用4步分级提取法和Tenax提取法分析了重金属和有机物的生物有效性。生物有效性毒性单位分析更加准确地锁定了毒性主要贡献重金属为Zn、Ni和Pb,毒性主要贡献有机物为氯氰菊酯、氯氟氰菊酯和氟虫腈。沉积物的稀释降低了重金属的毒性并使其毒性贡献鉴定变得复杂,生物有效性测量可以有效地提高TIE结果的准确性。
精选自Xiaoyi Yi, Huizhen Li, Ping Ma and Jing You. Identifying the causes of sediment-associated toxicity in urban waterways in South China: Incorporating bioavailabillity-based measurements into whole-sediment toxicity identification evaluation. Environmental Toxicology and Chemistry: Volume 34, Issue 8, pages 1744–1750, August 2015. DOI: 10.1002/etc.2970
详情请见http://onlinelibrary.wiley.com/doi/10.1002/etc.2970/full     

基于QSAR模型的蒙特卡洛方法分析有机化学物质对大型蚤(Daphnia magna)的毒性

本文建立一系列758种有机化合物对大型蚤(Daphnia magna)毒性的定量结构-活性关系(QSARs)。用简化的分子线性输入系统(SMILES)代表分子结构。用CORAL(关联和逻辑)软件作为工具来开发QSAR模型。这些模型使用蒙特卡罗方法建立,依据的原理是QSAR是一个“随机事件”,假设检验一组随机数据分布在可见的训练集和不可见的验证集。检验了三组分布于可见的训练、校准、测试集中的数据以及不可见的验证集。最佳模型的预测潜能,也就是其不可见的验证集的统计特征如下:n = 87,r² = 0.8377,RMSE = 0.564。建议和讨论了所构建模型的机械解释和适用领域。
精选自Alla P. Toropova, Andrey A. Toropov, Aleksandar M. Veselinovi?, Jovana B. Veselinovi?, Danuta Leszczynska, Jerzy Leszczynski. Monte Carlo based QSAR models for toxicity of organic chemicals to Daphnia magna. Environmental Toxicology and Chemistry: Volume 35, Issue 11, pages 2691–2697, November 2016. DOI: 10.1002/etc.3466
详情请见http://onlinelibrary.wiley.com/doi/10.1002/etc.3466/full
     

Microbial hydrolysis of polysaccharides and organic phosphates in the Northern Adriatic Sea

g -glucosidase and alkaline phosphatase, two ectoenzymes involved in the microbial decomposition of polysaccharides and organic phosphates, were evaluated in water samples collected from two areas of the Northern Adriatic Sea during the multidisciplinary Prisma II research project. The distribution of g -glucosidase and alkaline phosphatase is reported together with that of leucine aminopeptidase, an enzyme involved in the degradation of protein compounds. The data obtained showed the prevalence of g -glucosidase in summer months in the northern area, located in front of the Po delta, while in winter it is higher in the southern area (in front of Ancona). Phosphatase activity during February, 1998 had a maximum of 107 r nml m 1 h m 1 at a coastal station in the northern area; this enzyme appeared to be mainly associated with phytoplankton because the increase in alkaline phosphatase was associated with the increase of phytoplankton biomass, measured by chlorophyll a content. The relations between the microbial activities and environmental parameters are discussed.     

Herbicides interactions with cow manure and field soil organic matter

The direct interaction of the herbicide metazachlor ‐chosen as an example‐ with the soil organic matter has been studied by laboratory incubation of old and young cow manures containing metazachlor. The extraction efficiencies of solvents of increasing polarities indicated the formation of association compounds by bonds weaker than covalent between metazachlor and the organic matter: electron donor‐acceptor complexes, hydrogen bonding complexes, and complexes by both bonding types. Laboratory incubation of metazachlor in soil of low organic matter content indicated that the soil mineral part only had a diluting effect on the soil organic matter capacity to adsorb metazachlor. Similar association compounds were observed in the soil of a cauliflower field crop. Their concentrations were greater in the plots treated with organic fertilizers than in the organic fertilizers untreated plots. The free‐ unbound metazachlor was faster metabolized than the one bound to the soil organic matter, explaining why the organic fertilizer treatments slow down the herbicide soil biodegradation during the main first crop period. Inclusion of metazachlor in the field soil humic acids lattice ‐another kind of herbicide association compound with the soil organic matter‐ occurred at crop end when most of the metazachlor was metabolized; the soil concentrations of this kind of association compound thus was low, so that the release after crop of metazachlor in the environment has no practical significance.