Long-term variation of PM2.5 levels and composition at rural, urban, and roadside sites in Hong Kong: Increasing impact of regional air pollution

Long-term study of air pollution plays a decisive role in formulating and refining pollution control strategies. In this study, two 12-month measurements of PM_2.5 mass and speciation were conducted in 00/01 and 04/05 to determine long-term trend and spatial variations of PM_2.5 mass and chemical composition in Hong Kong. This study covered three sites with different land-use characteristics, namely roadside, urban, and rural environments. The highest annual average PM_2.5 concentration was observed at the roadside site (58.0±2.0 μg m⁻³ (average±2σ) in 00/01 and 53.0±2.7 μg m⁻³ in 04/05), followed by the urban site (33.9±2.5 μg m⁻³ in 00/01 and 39.0±2.0 μg m⁻³ in 04/05), and the rural site (23.7±1.9 μg m⁻³ in 00/01 and 28.4±2.4 μg m⁻³ in 04/05). The lowest PM_2.5 level measured at the rural site was still higher than the United States’ annual average National Ambient Air Quality Standard of 15 μg m⁻³. As expected, seasonal variations of PM_2.5 mass concentration at the three sites were similar: higher in autumn/winter and lower in summer. Comparing PM_2.5 data in 04/05 with those collected in 00/01, a reduction in PM_2.5 mass concentration at the roadside (8.7%) but an increase at the urban (15%) and rural (20%) sites were observed. The reduction of PM_2.5 at the roadside was attributed to the decrease of carbonaceous aerosols (organic carbon and elemental carbon) (>30%), indicating the effective control of motor vehicle emissions over the period. On the other hand, the sulfate concentration at the three sites was consistent regardless of different land-use characteristics in both studies. The lack of spatial variation of sulfate concentrations in PM_2.5 implied its origin of regional contribution. Moreover, over 36% growth in sulfate concentration was found from 00/01 to 04/05, suggesting a significant increase in regional sulfate pollution over the years. More quantitative techniques such as receptor models and chemical transport models are required to assess the temporal variations of source contributions to ambient PM_2.5 mass and chemical speciation in Hong Kong.     

Nitrate reductase for nitrate analysis in water

Nitrate analysis in water is one of the most frequently applied methods in environmental chemistry. Current methods for nitrate are generally based on toxic substances. Here, we show that a viable alternative method is to use the enzyme nitrate reductase. The key to applying this Green Chemistry solution for nitrate analysis is plentiful, inexpensive, analytical grade enzyme. We demonstrate that recombinant Arabidopsis nitrate reductase, expressed in the methylotrophic yeast Pichia pastoris, is a highly effective catalyst for nitrate analysis at 37°C. Recombinant production of enzyme ensures consistent quality and provides means to meet the needs of environmental chemistry.     

硝酸盐浓度及投加方式对反硝化除磷的影响

采用SBR反应器，详细研究了硝酸盐浓度及其投加方式对反硝化除磷过程的影响。结果表明，缺氧环境下的反硝化吸磷速率与作为电子受体的硝酸盐浓度有很大的关系，硝酸盐浓度越高．吸磷速率越快。当硝酸盐浓度较低．不足以氧化反硝化聚磷菌细胞内的PHB从而导致体系反硝化除磷效率的下降。相同浓度的硝酸盐，采用流加的方式可以获得比一次性投加更高的反硝化吸磷速率。缺氧环境下，反硝化脱氮量与磷的吸收量成良好的线性关系．借助于反硝化聚磷菌，反硝化脱氮与除磷可在一种环境中完成，有效解决了废水中COD不足的问题．同时达到了节省能源和降低污泥产量的目的。     

含氮杂环化合物吡啶缺氧降解过程中硝酸还原酶活性研究

在实验室中，采用摇床试验，在保证缺氧的条件下。研究了含氮杂环化合物吡啶缺氧反硝化降解过程中，硝酸还原酶的适宜作用条件、吡啶降解过程中硝酸还原酶活性变化情况及吡啶和硝态氮等的降解情况。结果表明，C／N对吡啶缺氧反硝化降解具有重要意义，pH和温度均对硝黧还原酶活性具有一定影响。硝酸还原酶的适宜作用条件为：温度25—30℃，pH7．5。吡啶降解过程中，硝酸还原酶活性由低到高逐渐提高，最后达到一个相对稳定的数值。在适宜的碳氮比条件下，吡啶起始浓度越高，硝酸还原酶最后稳定活性越高。     

Nitrate removal from aqueous solutions by magnetic cationic hydrogel: Effect of electrostatic adsorption and mechanism

Excessive nitrate(NO_3~-) is among the most problematic surface water and groundwater pollutants.In this study,a type of magnetic cationic hydrogel(MCH) is employed for NO_3~-adsorption and well characterized herein.Its adsorption capacity is considerably pHdependent and achieves the optimal adsorption(maximum NO_3~--adsorption capacity is95.88±1.24 mg/g) when the pH level is 5.2-8.8.The fitting result using the homogeneous surface diffusion model indicates that the surface/film diffusion controls the adsorption rate,and NO_3~-approaches the center of MCH particles within 30 min.The diffusion coefficient(D_s) and external mass transfer coefficient(k_F) in the liquid phase are1.15 × 10~(-6) cm~2/min and 4.5 × 10~(-6) cm/min,respectively.The MCH is employed to treat surface water that contains 10 mg/L of NO_3~-,and it is found that the optimal magnetic separation time is 1.6 min.The high-efficiency mass transfer and magnetic separation of MCH during the adsorption-regeneration process favors its application in surface water treatment.Furthermore,the study of the mechanism involved reveals that both-N~+(CH_3)_3 groups and NO_3~-are convoluted in adsorption via electrostatic interactions.It is further found that ion exchange between NO_3~-and chlorine occurs.     

Assessment of sources and transformation of nitrate in the alluvial-pluvial fan region of north China using a multi-isotope approach

A multi-isotope approach and mixing model were combined to identify spatial and seasonal variations of sources,and their proportional contribution to nitrate in the Hutuo River alluvial-pluvial fan region.The results showed that the NO_3~- concentration was significantly higher in the Hutuo River valley plain(178.7 mg/L) region than that in the upper and central pluvial fans of the Hutuo River(82.1 mg/L and 71.0 mg/L,respectively)and in the river(17.0 mg/L).Different land use types had no significant effect on the groundwater nitrate concentration.Based on a multi-isotope approach,we confirmed that the main sources of groundwater nitrate in different land use areas were domestic sewage and manure,followed by soil nitrogen,ammonia fertilizer,nitrate fertilizer and rainwater,and there were no significant spatial or seasonal variations.Combining δ~(15)N-NO_3,δ~(18)O-NO_3~- and δ~(37)Cl results can increase the accuracy of traceability.Nitrification could be the most important nitrogen migration and transformation process,and denitrification did not significantly affected the isotopic composition of the nitrate.The SIAR model outputs revealed that the main nitrate pollution sources in groundwater and river water were domestic sewage and manure,accounting for 55.9%-61.0% and 22.6%(dry season),50.3%-60.4% and 34.1%(transition season),42.7%-47.6% and 35.6%(wet season 2016) and 45.9%-46.7% and 38.4%(wet season 2017),respectively.This work suggests that the random discharge and disposal of domestic sewage and manure should be the first target for control in order to prevent further nitrate contamination of the water environment.     

Adsorption mechanisms of PFOA onto activated carbon anchored with quaternary ammonium/epoxide-forming compounds: A combination of experiment and model studies

When wood-based activated carbon was tailored with quaternary ammonium/epoxide (QAE) forming compounds (QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid (PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before half-breakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.     

农业排水沟渠硝态氮吸收动力学特征及相关性分析

为揭示农业排水沟渠NO_3~--N吸收动态变化特征,选择溴化钠(Na Br)为保守示踪剂、硝酸钾(KNO3)为添加营养盐,于2016年10月至2017年4月在合肥地区某一源头溪流开展5次示踪试验,并以TASCC方法和Michaelis-Menten(M-M)方程模拟NO_3~--N吸收动力学特征,结果表明,背景浓度条件下排水沟渠完全混合子渠段U_(amb)和V_(f-amb)的变化范围分别为11.40~69.13μg·(m~2·s)~(-1)[均值为34.45μg·(m~2·s)-1]、0.07~0.43 mm·s~(-1)(均值为0.24 mm·s~(-1)),相应地Sw-amb变化范围为92.51~405.74 m(均值为199.06 m),明显小于排水沟渠长度(也就是2.5 km),表明沟渠具有较强的NO_3~--N滞留潜力.M-M方程较好地拟合了NO_3~--N吸收动力学特征,参数Umax变化范围为158~1 280μg·(m~2·s)~(-1)[均值为631.13μg·(m~2·s)~(-1)],Km变化范围为0.16~5.52 mg·L~(-1)(均值为1.46 mg·L~(-1)).相关分析表明,Sw-amb与NO_3~--Namb呈显著负相关、Uamb与NO_3~--Namb呈极显著正相关,其它螺旋指标与NO_3~--N背景浓度的相关性均不明显;水文因素对NO_3~--N滞留影响也不显著,而沟渠槽道地貌特征指标Фw、ФA与大部分螺旋指标都呈显著相关性,表明槽道地貌特征对NO_3~--N滞留影响相对较为重要.     

稳定同位素追踪水体中的氮来源的研究现状

氮是水体中的主要污染物之一。近几十年来,随着工农业的发展,使得水体中氮的污染呈上升趋势,并在今后可能会持续,最根本的解决方法是找到源头,从根本上切断污染途径以达到消除氮源的污染。在查阅相关文献的基础上,阐述了水中用同位素追踪研究氮的来源的研究进展和存在的问题,对于评价氮的污染现状、污染控制和环境管理具有十分重要的意义。     

The fate of nitrogen in a moderately alkaline and calcareous soil amended with biosolids and urea

The determination of nitrogen (N) based loading rates for land application of biosolids is challenging and site specific. Over loading may contribute to environmental, agricultural, or human health problems. The objective of this study was to monitor N mineralization and losses in a moderately alkaline and calcareous desert soil amended with either anaerobically digested (AN) or lime-stabilized (LS) biosolids, and irrigated with and without urea enriched water. For Experiment 1, N inputs, leaching and residuals in soil were evaluated in an open soil column system. For Experiment 2, ammonia (NH₃) emissions were evaluated in a closed soil column system. In Experiment 1, AN and LS biosolids increased soil ON (organic N) by three and two fold, respectively. Respective net N mineralization of ON from biosolids alone was 90% and 62% without urea, and 71% and 77%, respectively with added urea. Nitrogen leaching losses and residuals in amended soil did not account for all N inputs into the soil/biosolids system. In Experiment 2, NH₃ emissions were not significantly different among treated soils with or without added urea, except LS amended soil receiving urea. Ammonia losses did not account for unaccounted N in Experiment 1. We concluded that deep placement and rapid mineralization of AN biosolids promoted anaerobic soil conditions and denitrification, in addition to the high denitrification potential of desert soil. LS biosolids showed greater potential than AN biosolids for safe and beneficial land application to desert soils regardless of biosolids placement and the inclusion of N rich irrigation water.