基于液相31P核磁共振(NMR)技术的巢湖沉积物中有机磷形态研究

利用改进的沉积物有机磷提取方法和液相31P核磁共振(NMR)分析方法,研究了巢湖表层沉积物有机磷形态.结果表明:西部湖区表层沉积物总磷含量高于东部湖区,其平均含量分别为(1089.82±108.14) mg·kg-1和(497.80±51.59) mg·kg-1;东部湖区沉积物中有机磷百分含量(31.88％±2.41％)高于西部湖区(20.86％±1.65％);表层沉积物主要磷份组成包括膦酸盐(Phon-P)、正磷酸盐(Ortho-P)、磷酸单酯(Mono-P)、磷脂(Lipid-P)、DNA(DNA-P)、焦磷酸盐(Pyro-P);磷酸单酯为有机磷的主要组分,平均含量占总磷的22.12％±5.32％;磷酸单酯和DNA百分含量东部湖区大于西部湖区,磷酸单酯百分含量分别为25.99％±2.29％和16.30％±1.06％,DNA百分含量分别为5.61％±0.24％和3.85％±1.01％.31P核磁共振技术可以有效的应用于巢湖等富营养化湖泊沉积物磷形态分析;巢湖表层沉积物以无机磷为主,有机磷种类丰富,以磷酸单酯为主.     

基于能源-环境情景模拟的北京市大气污染对居民健康风险评价研究

保护居民健康是北京市能源系统优化管理和大气污染治理的重要目标.本研究基于北京市的社会经济发展目标并结合相关节能减排和环保要求,针对全市2010-2020年间的能源消费分别设计了高、中、低3种约束情景,通过LEAP模型预测了全市至2020年的能源消费量与S02、NOx、PM10和PM2.5等4种主要大气污染物的排放强度,并采用泊松回归模型对3种情景下主城区居民受环境空气中这4种大气污染物的暴露危害所导致的健康风险进行了评估.结果显示:相对低约束情景,高约束情景至2020年可避免与S02、NOx、PM10和PM2.5污染相关的死亡危害分别为2663、6359、4720和4104人·a-1,而且在高约束情景下煤炭消费比重每下降1％,可相应地避免约1400人·a-1的污染急性死亡.由此建议北京市实施更加严格的节能和减排措施,严控煤炭消费总量,进一步优化能源结构,最大程度地降低能源消费导致的大气污染所产生的居民健康风险.     

饮用水水源地严格管理水质的对策分析——对实行严格水资源管理问题上的看法和建议

2012年1月国务院发布了《关于实行最严格水资源管理制度的意见》,这是众所关注的要事,实行了最严格水资源管理的原则精神以及确定县级以上政府负总责的规定.但对如何严格管理的技术路线和对策措施上,特针对现实中存在的主要问题提出以下3点看法和建议:①达到地面水环境质量Ⅱ类水质的饮用水水源地不一定未受污染;②保护区内企业车间排水口符合第一类污染物最高允许排放浓度规定是满足饮用水水源地要求的必要条件;③《地面水环境质量标准》(GB 3838-2002)对第一类污染物规定的Ⅱ类水质,是否体现了水环境背景值有较大存疑.     

垦殖对湿地土壤有机碳垂直分布及可溶性有机碳截留的影响

通过测定和计算兴凯湖地区沼泽湿地及由其垦殖而来的旱田和水田土壤剖面有机碳含量和密度及土壤剖面不同深度土壤溶液中可溶性有机碳含量,分析了垦殖对兴凯湖周边沼泽湿地土壤有机碳垂直分布及土壤剖面截留可溶性有机碳的影响.结果表明,垦殖显著影响湿地0～40 cm土壤有机碳含量,大豆田和水稻田0～10、10～20、20～30、30～40 cm土壤有机碳含量与湿地相比分别降低了79.07%和82.01%、79.01%和82.28%、79.86%和92.90%、37.49%和78.05%;40 cm以下土层土壤有机碳含量垦殖前后差异不显著.大豆田和水稻田有机碳密度相比沼泽湿地分别降低了25.50%和47.35%,但三者1 m深土壤中大部分的有机碳均是储存在0～50 cm土层中.垦殖前后土壤有机碳含量与深度之间的关系均可用指数函数来描述,垦殖改变了土壤有机碳含量但并未改变其随土壤深度的变化规律.垦殖为大豆田土壤剖面对可溶性有机碳的截留效果较湿地和水稻田更明显,沼泽湿地和水稻田对可溶性有机碳的截留效果大致相当.     

Investigation of low-molecular weight organic acids and their spatiotemporal variation characteristics in Hongfeng Lake, China

The identities and concentrations of low-molecular-weight organic acids (LMWOAs) were determined by ion chromatography throughout a 20-m water column in Hongfeng Lake, China. The spatiotemporal variations of LMWOAs and their contributions to dissolved organic matter (DOM) in a research period of 24 hr were also investigated. The results demonstrated that five LMWOAs (lactic, acetic, pyruvic, sorbic, oxalic acid) were detected, and their total concentration and proportion in DOC were 6.55 μmol/L and 7.47%. Their average levels were 2.50, 0.65, 2.35, 0.96 and 0.09 μmol/L, respectively. LMWOAs were higher during daytime (10:00-18:00 on Jun 13, 2008) than nighttime (21:00-6:00 the next morning), in particular 4.99 μmol/L high in the epilimnion ( 1 m water depth), reflecting the fact that direct import from terrigenous sources and photochemical production from humic materials were dominant during LMWOAs’ origin and accumulation. The same factors caused LMWOAs to be 0.63 μmol/L in the epilimnion higher than in the hypolimnion. The rapid decrease of total organic acid (TOA) up until 18:00 mainly resulted from bio-uptake and mineralization in the hypolimnion (>1 m water depth). Pyruvic acid increased with time in the epilimnion and decreased in the hypolimnion, largely related to the two contrary processes of continuous degradation and synthesis of macromolecular organic matter during life materials’ cycle mediated by organisms. Simultaneously, plankton behavior and thermal stratification played a pivotal role in LMWOAs’ behavior in the water column, causing decreasing and increasing profiles. The distribution of LMWOAs represents an interesting resource for biogeochemical research of DOM in aquatic ecosystems.     

Homogeneous and heterogeneous reactions of anthracene with selected atmospheric oxidants

The reactions of gas-phase anthracene and suspended anthracene particles with O3 and O3-NO were conducted in a 200-L reaction chamber, respectively. The secondary organic aerosol (SOA) formations from gas-phase reactions of anthracene with O3 and O3-NO were observed. Meanwhile, the size distributions and mass concentrations of SOA were monitored with a scanning mobility particle sizer (SMPS) during the formation processes. The rapid exponential growths of SOA reveal that the atmospheric lifetimes of gas-phase anthracene towards O3 and O3-NO are less than 20.5 and 4.34 hr, respectively. The particulate oxidation products from homogeneous and heterogeneous reactions were analyzed with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). Gas chromatograph/mass spectrometer (GC/MS) analyses of oxidation products of anthracene were carried out for assigning the time-of-flight (TOF) mass spectra of products from homogeneous and heterogeneous reactions. Anthrone, anthraquinone, 9,10- dihydroxyanthracene, and 1,9,10-trihydroxyanthracene were the ozonation products of anthracene, while anthrone, anthraquinone, 9-nitroanthracene, and 1,8-dihydroxyanthraquinone were the main products of anthracene with O3-NO.     

Identification of key factors governing chemistry in groundwater near the water course recharged by reclaimed water at Miyun County, Northern China

Reclaimed water was successfully used to recover the dry Chaobai River in Northern China, but groundwater may be polluted. To ensure groundwater protection, it is therefore critical to identify the governing factors of groundwater chemistry. Samples of reclaimed water, river and groundwater were collected monthly at Chaobai River from January to September in 2010. Fifteen water parameters were analyzed. Two kinds of reclaimed water were different in type (Na-Ca-Mg-Cl-HCO3 or Na-Ca-Cl-HCO3 ) and concentration of nitrogen. The ionic concentration and type in river were similar to reclaimed water. Some shallow wells near the river bed had the same type (Na-Ca-Mg-Cl-HCO3 ) and high concentration as reclaimed water, but others were consistent with the deep wells (Ca-Mg-HCO3 ). Using cluster analysis, the 9 months were divided into two periods (dry and wet seasons), and all samples were grouped into several spatial clusters, indicating different controlling mechanisms. Principal component analysis and conventional ionic plots showed that calcium, magnesium and bicarbonate were controlled by water-rock interaction in all deep and some shallow wells. This included the dissolution of calcite and carbonate weathering. Sodium, potassium, chloride and sulfate in river and some shallow wells recharged by river were governed by evaporation crystallization and mixing of reclaimed water. But groundwater chemistry was not controlled by precipitation. During the infiltration of reclaimed water, cation exchange took place between (sodium, potassium) and (calcium, magnesium). Nitrification and denitrification both happened in most shallow groundwater, but only denitrification in deep groundwater.     

Influence of dissolved organic matter character on mercury incorporation by planktonic organisms：An experimental study using oligotrophic water from Patagonian lakes

Ligands present in dissolved organic matter （DOM） form complexes with inorganic divalent mercury （Hg^2＋） affecting its bioavailability in pelagic food webs. This investigation addresses the influence of a natural gradient of DOM present in Patagonian lakes on the bioaccumulation of Hg^2＋ （the prevailing mercury species in the water column of these lakes） by the algae Cryptomonas erosa and the zooplankters Brachionus calyciflorus and Boeckella antiqua. Hg^2＋ accumulation was studied through laboratory experiments using natural water of four oligotrophic Patagonian lakes amended with^197Hg^2＋. The bioavailability of Hg^2＋ was affected by the concentration and character of DOM. The entrance of Hg^2＋ into pelagic food webs occurs mostly through passive and active accumulation. The incorporation of Hg^2＋ by Cryptomonas, up to 27% of the Hg^2＋ amended, was found to be rapid and dominated by passive adsorption, and was greatest when low molecular weight compounds with protein-like or small phenolic signatures prevailed in the DOM. Conversely, high molecular weight compounds with a humic or fulvic signature kept Hg^2＋ in the dissolved phase, resulting in the lowest Hg^2＋ accumulation in this algae. In Brachionus and Boeckella the direct incorporation of Hg from the aqueous phase was up to 3% of the Hg^2＋ amended. The dietary incorporation of Hg^2＋ by Boeckella exceeded the direct absorption of this metal in natural water, and was remarkably similar to the Hg^2＋ adsorbed in their prey. Overall, DOM concentration and character affected the adsorption of Hg^2＋ by algae through competitive binding, while the incorporation of Hg^2＋ into the zooplankton was dominated by trophic or dietary transfer.     

Electrochemical and spectroscopic characteristics of dissolved organic matter in a forest soil profile

Dissolved organic matter （DOM） represents one of the most mobile and reactive organic compounds in ecosystem and plays an important role in the fate and transport of soil organic pollutants, nutrient cycling and more importantly global climate change. Electrochemical methods were first employed to evaluate DOM redox properties, and spectroscopic approaches were utilized to obtain information concerning its composition and structure. DOM was extracted from a forest soil profile with five horizons. Differential pulse voltammetry indicated that there were more redox-active moieties in the DOM from upper horizons than in that from lower horizons. Cyclic voltammetry further showed that these moieties were reversible in electron transfer. Chronoamperometry was employed to quantify the electron transfer capacity of DOM, including electron acceptor capacity and electron donor capacity, both of which decreased sharply with increasing depth. FT-IR, UV-Vis and fluorescence spectra results suggested that DOM from the upper horizons was enriched with aromatic and humic structures while that from the lower horizons was rich in aliphatic carbon, which supported the findings obtained by electrochemical approaches. Electrochemical approaches combined with spectroscopic methods were applied to evaluate the characteristics of DOM extracted along a forest soil profile. The electrochemical properties of DOM, which can be rapidly and simply obtained, provide insight into the migration and transformation of DOM along a soil profile and will aid in better understanding of the biogeochemical role of DOM in natural environments.     

Speciation of organic phosphorus in a sediment profile of Lake Taihu II. Molecular species and their depth attenuation

The understanding of organic phosphorus(P) dynamics in sediments requires information on their species at the molecular level,but such information in sediment profiles is scarce.A sediment profile was selected from a large eutrophic lake,Lake Taihu(China),and organic P species in the sediments were detected using solution phosphorus-31 nuclear magnetic resonance spectroscopy(31 P NMR) following extraction of the sediments with a mixture of 0.25 mol/L NaOH and 50 mmol/L EDTA(NaOH-EDTA) solution.The results showed that P in the NaOH-EDTA extracts was mainly composed of orthophosphate,orthophosphate monoesters,phospholipids,DNA,and pyrophosphate.Concentrations of the major organic P compound groups and pyrophosphate showed a decreasing trend with the increase of depth.Their half-life times varied from 3 to 27 years,following the order of orthophosphate monoesters > phospholipids DNA > pyrophosphate.Principal component analysis revealed that the detected organic P species had binding phases similar to those of humic acid-associated organic P(NaOH-NRP HA),a labile organic P pool that tends to transform to recalcitrant organic P pools as the early diagenetic processes proceed.This demonstrated that the depth attenuation of the organic P species could be partly attributed to their increasing immobilization by the sediment solids,while their degradation rates should be significantly lower than what were suggested in previous studies.