铁(氢)氧化物介导的溶解性有机质、无机磷的固定及相互作用研究进展

铁(氢)氧化物介导的溶解性有机质(DOM)和无机磷(DIP)的固定在水生态系统中普遍存在,对碳、磷元素的生物地球化学循环有重要的影响. 铁(氢)氧化物主要通过吸附和共沉淀两种过程固定DOM和DIP,且铁(氢)氧化物、DOM和DIP三者存在复杂的相互作用. 本文主要从铁(氢)氧化物对DOM和DIP的固定,铁(氢)氧化物、DOM和DIP之间的相互影响等方面综述了相关研究进展,梳理了铁(氢)氧化物、DOM和DIP在吸附和共沉淀过程中的相互作用机制与影响因素. DOM的存在会通过占据铁(氢)氧化物表面吸附点位、络合、抑制铁水解沉淀等途径影响铁(氢)氧化物对DIP的固定; 且不同机制与DOM的不同性质如分子大小、芳香组分、羧基官能团含量等有关. 而DIP的存在会改变铁(氢)氧化物对DOM的固定分馏过程,改变溶液中DOM的组分和性质. 在明晰三者相互作用基础上,探讨了铁(氢)氧化物介导的DOM和DIP的固定过程对湖泊内源磷释放和碳埋藏的可能影响,并对未来的研究方向进行了展望.     

Amount and reactivity of dissolved organic matter export are affected by land cover change from old-growth to second-growth forests in headwater ecosystems

Headwater forest ecosystems of the western USA generate a large portion of the dissolved organic matter (DOM) transported in streams across North America. Land cover changes that alter forest structure and species composition affect the quantity and composition of DOM transferred to aquatic ecosystems. Clear-cut harvesting affects ~1% of the forest area of North America annually, leaving most western forests in varying stages of regrowth and the total area of old-growth forest is decreasing. The consequences of this widespread management practice on watershed carbon cycling remain unknown. We investigated the role of land cover change, because of clear-cut harvesting, from mixed-species old-growth to lodgepole pine-dominated second-growth forest on the character and reactivity of hillslope DOM exports. We evaluated inputs of DOM from litter leachates and export of DOM collected at the base of trenched hillslopes during a 3-year period (2016–2018) at the Fraser Experimental Forest in north-central Colorado, USA. Dissolved organic carbon and total dissolved nitrogen were higher in lateral subsurface flow draining old- versus second-growth forest. Fluorescence spectroscopy showed that the DOM exported from the old-growth forest was more heterogeneous and aromatic and that proteinaceous, microbially processed DOM components were more prevalent in the second-growth forest. Biological oxygen demand assays revealed much lower microbial metabolism of DOM in litter leachate and subsurface exports from the old-growth forest relative to second growth. Old-growth and second-growth forests are co-mingled in managed ecosystems, and our findings demonstrate that land cover change from a mixture of conifer species to lodgepole pine dominance influences DOM inputs that can increase the reactivity of DOM transferred from terrestrial to aquatic ecosystems.     

草源型可溶性有机物降解过程中活性氧物种产生过程

活性氧物种(ROS)参与天然水体系统中的光化学反应、氧化还原反应,是影响水体中有机污染物的迁移、转化、环境归宿及生态效应的重要因素.然而目前对草源型可溶性有机物(DOM)分解过程中ROS的产生过程并不清楚.本文通过室内模拟实验首先构建了室内测定3种ROS(~3CDOM~*、~1O_2、·OH)的方法,进而分析草源植物——苔草(Carex tristachya)残体浸出液中DOM光降解过程中ROS的产生过程.结果表明:ROS累积含量的产生随着DOM的降解逐渐升高在3种自由基含量中,~3CDOM*的产生含量最多,·OH产生含量低于另外2种ROS两个数量级.CDOM含量与~3CDOM~*、~1O2、·OH浓度呈现正相关关系,尤其与~3CDOM~*和~1O_2浓度的显著性水平最高,·OH次之.ROS浓度与水质指标呈现出不同的线性相关关系,与硝态氮浓度呈负相关关系,而与亚硝态氮浓度呈现正相关关系,并且亚硝态氮对ROS浓度影响效果极显著.同时类蛋白荧光峰值强度的衰减与ROS累积含量呈现极显著负相关关系,脱明在DOM的光降解过程中蛋白质小分子的降解是产生ROS很重要的一个部分.综上通过对草源型DOM光降解过程中ROS产生过程的研究,增加了对湖泊生态系统中水生植物产生ROS的过程、迁移、转化、归宿及其作用机制的认识.     

The Analysis of the Seasonal,Spatial, and Compositional Distribution of Humic Substances in a Subtropical Shallow Lake

The spatial and temporal distribution of humic substances in aquatic ecosystems can have important effects on ecosystem productivity, negatively impacting primary productivity while positively impacting secondary productivity. In the present investigation, a large shallow lake ecosystem was studied to determine the spatial and seasonal variation of the composition and concentration of humic substances. Concentrations of total dissolved organic matter, humic acid, and fulvic acid were found to display significant spatial distributions (1.3…13.5 mg/L, DOM; 0.1…5.4 mg/L, HA). The distribution is described by using mapping techniques and the analysis of the spatial distribution of the lake. An analysis of the seasonal variations also indicated the dependence of the occurrence of these compounds on meteorological and hydrological conditions. To identify the potential sources of these organic materials, an analysis was made of the ratio of humic and fulvic acid fractions and total DOM. It was found that areas of high DOM concentration coincided with the areas of highest HA percentage of total DOM. Furthermore using the ratio of the normalised concentrations of HA, FA, and residual DOM (< 5000 g/mol) it was found that areas dominated by each are spatially distinct. This confirms the hypothesis that in these shallow lakes, photodegradation and bacterioplankton activity will create a residence time dependent zonation of each component of the total DOM.     

溶解性有机质与水生生物的直接相互作用研究进展

溶解性有机质广泛存在于天然水体中,具有重要的生态与环境意义.然而在环境科学领域内,天然水体中的溶解性有机质长期以来仅仅被作为惰性的吸附剂对待,其自身的与生物的直接作用却一直被忽视.近年来,越来越多的研究证据表明溶解性有机质自身即具有生物效应.它能在生物表面吸附.并影响细胞膜的电化学性质与膜渗透性,能被生物吸收,进而诱导...     

Application of generalized contaminant retardation factor to a multi‐phase system

In this study, a generalized contaminant retardation factor applicable to a multiphase system where various types of colloids exist simultaneously with contaminants is derived and incorporated into an equilibrium model which is successfully applied to experimental data for which phenanthrene was used as hydrophobic organic contaminants and dissolved organic matter (DOM) or bacteria as mobile carriers. Based on the parameter values for the experimental data regarding the association of phenanthrene with solid matrix, DOM and various bacterial isolates, numerical experiments are performed to examine the transport behaviour of hydrophobic organic contaminants in various types of the multiphase system. Numerical experiments demonstrate that the extent of contaminant transport enhancement depends on the adsorption affinity of the colloid, its concentration and its mobility, and that the importance of a third phase to contaminant transport needs to be evaluated carefully with respect to the relevance of experimental conditions applied to realistic environmental conditions. Copyright © 2003 John Wiley & Sons, Ltd.     

Effects of varying estuarine conditions on the sorption of phenanthrene to sediment particles of Yangtze Estuary

The sorption of phenanthrene on the Yangtze Estuary sediment was studied under varying conditions of particle size, sediment organic contents, salinity, and dissolved organic matter (DOM) concentrations. Small sediment particles showed higher trapping capacity for phenanthrene due to the higher organic contents associated. The organic carbon-based partition coefficient of phenanthrene to the Yangtze Estuary sediment was obtained as 7120 L/kg, lower than the values for other soils or sediments reported in previous studies. The magnitude and direction of the salt effect were complicated by the specific DOM studied. The sediment sorption capacity was greatly increased in saline water in the absence of DOM but decreased in the presence of DOM. Given the conditions in the Yangtze Estuary, the equilibrium sorption of phenanthrene would be decreased with increasing salinity. Overall, the nature and content of both sediment-bound and dissolved organic matter dominate the sorption of hydrophobic organic contaminants in the estuary.     

Organically Bound Nutrients in Dissolved Organic Matter Fractions in Seepage and Pore Water of Weakly Developed Forest Soils

Previous field and laboratory studies showed that organically bound nutrients can contribute largely to the export of N, P, and S from soil into aquatic systems. One possible determinant for the losses of dissolved organic nutrients leaving the soil environment could be their distribution between dissolved organic matter (DOM) fractions of different mobility in soil. To elucidate the potential influence of DOM fractions under varying flow conditions on the vertical translocation of organically bound nutrients, we determined the concentrations and fluxes of dissolved organic C (DOC) and nutrients (DON, DOP, DOS) in soil water under a Scots pine (Pinus sylvestris L.) and a European beech (Fagus sylvatica L.) forest. We sampled seepage water from the organic forest floor layer and the mineral subsoil using zero‐tension lysimeters and soil pore water using tension lysimeters and suction cups. DOM in soil water was fractionated into hydrophilic and hydrophobic compounds by XAD‐8 at pH 2. We found that the organic forest floor layers were large sources for DOC, DON, DOP, and DOS. The dissolved organic nutrients were mainly concentrated in the hydrophilic DOM fraction which proved to be more mobile in mineral soil pore water than the hydrophobic one. Consequently, the concentrations and fluxes of dissolved organic nutrients decreased less with depth than those of DOC. Concentrations as well as fluxes in subsoil pore water of DOC and dissolved organic nutrients in the studied weakly developed soils were high as compared with literature data on deeply developed forest soils. Under conditions of rapid water flow through the strongly structured mineral soil at the beech site, almost no retention of DOM took place and thus the influence of the distribution of organically bound nutrients between the DOM fractions on the export of DON, DOP, and DOS was negligible.     

Diurnal variability in riverine dissolved organic matter composition determined by in situ optical measurement in the San Joaquin River (California,USA)

Dissolved organic matter (DOM) concentration and composition in riverine and stream systems are known to vary with hydrological and productivity cycles over the annual and interannual time scales. Rivers are commonly perceived as homogeneous with respect to DOM concentration and composition, particularly under steady flow conditions over short time periods. However, few studies have evaluated the impact of short term variability (<1 day) on DOM dynamics. This study examined whether diurnal processes measurably altered DOM concentration and composition in the hypereutrophic San Joaquin River (California) during a relatively quiescent period. We evaluated the efficacy of using optical in situ measurements to reveal changes in DOM which may not be evident from bulk dissolved organic carbon (DOC) measurement alone. The in situ optical measurements described in this study clearly showed for the first time diurnal variations in DOM measurements, which have previously been related to both composition and concentration, even though diurnal changes were not well reflected in bulk DOC concentrations. An apparent asynchronous trend of DOM absorbance and chlorophyll‐a in comparison to chromophoric dissolved organic matter (CDOM) fluorescence and spectral slope S_290–350 suggests that no one specific CDOM spectrophotometric measurement explains absolutely DOM diurnal variation in this system; the measurement of multiple optical parameters is therefore recommended. The observed diurnal changes in DOM composition, measured by in situ optical instrumentation likely reflect both photochemical and biologically‐mediated processes. The results of this study highlight that short‐term variability in DOM composition may complicate trends for studies aiming to distinguish different DOM sources in riverine systems and emphasizes the importance of sampling specific study sites to be compared at the same time of day. The utilization of in situ optical technology allows short‐term variability in DOM dynamics to be monitored and serves to increase our understanding of its processing and fundamental role in the aquatic environment. Copyright © 2007 John Wiley & Sons, Ltd.     

沉积物中有机质的环境行为研究进展

水体沉积物是重金属,有毒有机化合物等环境污染物及C,N,P等营养元素的汇和释放源,而有机质对灾些污染物和营养元素在沉积物中的迁移,转化等地球化学行为中起着至关重要的作用,本文就近期有关沉积物中有机质的环境地球化学行为为方面的研究进行了综述,重点评述了有关沉积物中有机质本身的来源,性质,迁移和矿化及其环境效应等方面的研究进展。     

Variation in the photochemical lability of dissolved organic matter in a large boreal watershed

Boreal watersheds contain a vast quantity of terrestrially derived dissolved organic matter (DOM) originating from wetland and forest soils, yet variation in the potential for photochemical transformation of boreal aquatic DOM sources remains poorly understood. Laboratory solar radiation exposure experiments were conducted on DOM samples collected in three seasons, across nine sites, representing contrasting catchment composition and watershed position to assess variation in the photochemical lability of boreal DOM source and stable carbon isotopic signature (δ¹³C) of photomineralized DOM. Dissolved organic carbon (DOC) loss rates during laboratory exposure were lowest in summer, suggesting that DOM may have been more photo-degraded during summer. DOM from upstream portions of forested stream sites and wetland-influenced sites was more photolabile relative to downstream portions and the river DOM, suggesting potential losses in photolabile DOM downstream and in the lower reaches of the watershed. Increased a₂₅₄:a₃₅₀ and spectral slope following sample exposure suggest photoproduction of low molecular weight (LMW) CDOM and/or a higher photoreactivity of high molecular weight versus LMW compounds. Photomineralization of nitrogen was regulated by organic nitrogen concentration and resulted in NH₄ ⁺-photoproduction rates between 0.01 and 0.3?μM N?h^?1 and ecologically significant increases in NH₄ ⁺ for these waters. The δ¹³C of the photomineralized DOM was positively correlated to initial DOC concentration and generally lower when initial DOC concentrations were lower, suggesting variation in photomineralized DOM δ¹³C may be a result of kinetic isotope fractionation. Results from this study demonstrate significant variation in the photochemical lability of boreal watershed sources of DOM. Such variation suggests landscape and environmental change has the potential to alter the biogeochemical role photochemical transformations play in downstream portions of boreal watersheds.     

Denitrification in a Laurentian Great Lakes coastal wetland invaded by hybrid cattail (Typha × glauca)

Wetland ecosystems maintain and improve water quality through the process of denitrification, an increasingly important ecosystem service due to global N pollution. Invasive plants have the potential to disrupt denitrification by altering the environmental conditions that facilitate this process. Great Lakes coastal wetlands are experiencing widespread invasion by highly productive hybrid cattail with largely uncertain biogeochemical effects. Through field and controlled mesocosm studies, we sought to determine the effects of cattail invasion through time on denitrification rates and associated environmental factors in a Great Lakes coastal wetland. In the field, we found that cattail density correlated with increased denitrification and a suite of environmental and plant community characteristics and denitrification rates were positively correlated with NH₄ ⁺, sediment organic matter, reduced water levels, and cattail stand age. Through our controlled mesocosm study, we documented conditions 1- and 5-year following invasion and found that denitrification rates and soil organic matter increased in year 5, and cattail and year-since-invasion altered plant communities and soil NH₄ ⁺. Only a weak correlation between denitrification rates and cattail treatments was noted, however, owing to high replicate variability. Our results indicate that with increasing cattail residence time, one ecosystem service, biodiversity, was negatively impacted, while two other services, denitrification and sediment carbon accumulation, were enhanced. Thus, this highly invaded wetland still provides valuable services to aquatic ecosystems and to society. A holistic perspective is therefore critical when evaluating invasive species impacts in which negative impacts are weighed against other ecosystem services, which may be stimulated.     

三峡库区土地利用对河流溶解性有机质的多时空尺度影响

三峡库区拥有目前世界上规模最大的水利枢纽工程,自投入使用以来,为长江流域提供了丰富的水源及电力,促进了经济的发展,但同时也对该区域的生态环境造成了严重的冲击。澎溪河流域作为三峡库区长江流域干流的典型回水区和消落带,是众多学者研究三峡库区生态环境变化的重点区域。为探究不同时空尺度下土地利用对河流溶解性有机质（DOM）的影响,以澎溪河流域为研究对象,基于紫外-可见光谱分析和三维荧光光谱矩阵-平行因子分析,结合河段缓冲区、河岸带缓冲区及子流域3种空间尺度的二级土地利用类型,解析了旱雨季水体DOM的组成及来源特征,并采用相关分析和冗余分析方法探讨了3种空间尺度下土地利用方式对旱雨季水体DOM的多时空尺度影响。结果表明：（1）旱季水体DOM荧光组分以陆源类腐殖质所占比例更大,雨季水体DOM荧光组分以富里酸贡献为主。（2）流域内陆源输入和内源产生对水体DOM丰度均有贡献,雨季较旱季水体DOM的陆源性更强,自生源特征较弱。（3）土地利用在雨季和子流域尺度下对水体DOM的影响更显著,其中,雨季子流域尺度下,土地利用指数对水体DOM参数的解释率为90.35%。（4）不同土地利用方式对水体DOM产生的影响...     

Interactions between climate change and contaminants

There is now general consensus that climate change is a global threat and a challenge for the 21st century. More and more information is available demonstrating how increased temperature may affect aquatic ecosystems and living resources or how increased water levels may impact coastal zones and their management. Many ecosystems are also affected by human releases of contaminants, for example from land based sources or the atmosphere, which also may cause severe effects. So far these two important stresses on ecosystems have mainly been discussed independently. The present paper is intended to increase awareness among scientists, coastal zone managers and decision makers that climate change will affect contaminant exposure and toxic effects and that both forms of stress will impact aquatic ecosystems and biota. Based on examples from different ecosystems, we discuss risks anticipated from contaminants in a rapidly changing environment and the research required to understand and predict how on-going and future climate change may alter risks from chemical pollution.     

POTENTIAL EFFECTS OF CLIMATE CHANGE ON FRESHWATER ECOSYSTEMS OF THE NEW ENGLAND/MID-ATLANTIC REGION

Numerous freshwater ecosystems, dense concentrations of humans along the eastern seaboard, extensive forests and a history of intensive land use distinguish the New England/Mid-Atlantic Region. Human population densities are forecast to increase in portions of the region at the same time that climate is expected to be changing. Consequently, the effects of humans and climatic change are likely to affect freshwater ecosystems within the region interactively. The general climate, at present, is humid continental, and the region receives abundant precipitation. Climatic projections for a 2 × CO₂ atmosphere, however, suggest warmer and drier conditions for much of this region. Annual temperature increases ranging from 3–5°C are projected, with the greatest increases occurring in autumn or winter. According to a water balance model, the projected increase in temperature will result in greater rates of evaporation and evapotranspiration. This could cause a 21 and 31% reduction in annual stream flow in the southern and northern sections of the region, respectively, with greatest reductions occurring in autumn and winter. The amount and duration of snow cover is also projected to decrease across the region, and summer convective thunderstorms are likely to decrease in frequency but increase in intensity. The dual effects of climate change and direct anthropogenic stress will most likely alter hydrological and biogeochemical processes, and, hence, the floral and faunal communities of the region's freshwater ecosystems. For example, the projected increase in evapotranspiration and evaporation could eliminate most bog ecosystems, and increases in water temperature may increase bioaccumulation, and possibly biomagnification, of organic and inorganic contaminants. Not all change may be adverse. For example, a decrease in runoff may reduce the intensity of ongoing estuarine eutrophication, and acidification of aquatic habitats during the spring snowmelt period may be ameliorated. Recommendations for future monitoring efforts include: (1) extending and improving data on the distribution, abundance and effect of anthropogenic stressors (non-point pollution) within the region; and (2) improving scientific knowledge regarding the contemporary distribution and abundance of aquatic species. Research recommendations include: (1) establishing a research centre(s) where field studies designed to understand interactions between freshwater ecosystems and climate change can be conducted; (2) projecting the future distribution, activities and direct effects of humans within the region; (3) developing mathematical analyses, experimental designs and aquatic indicators that distinguish between climatic and anthropogenic effects on aquatic systems; (4) developing and refining projections of climate variability such that the magnitude, frequency and seasonal timing of extreme events can be forecast; and (5) describing quantitatively the flux of materials (sediments, nutrients, metals) from watersheds characterized by a mosaic of land uses. © 1997 John Wiley & Sons, Ltd.     

Effects of precipitation on summer epilimnion thickness in tropical lakes

This study aimed to evaluate the importance of physical, chemical and biological factors (e.g., chlorophyll-a, and carbon) in the regulation of the summer epilimnion thickness (Zmix) of the tropical lakes focusing on trends of the current environmental variability. We sampled a set of tropical lakes from the middle Rio Doce lacustrine system (Minas Gerais, Brazil) for two consecutive summers. Besides Zmix, we analyzed the visible light attenuation (Kd_PAR), dissolved organic carbon (DOC), chlorophyll-a (Chl-a), total suspended solids (TSS), and fetch. We also analyze the quality of the dissolved organic matter (DOM) through colored dissolved organic matter (CDOM), spectral slope (S), DOC-specific absorbance (SUVA) and the ratio between the absorbance at 250 nm and 365 nm (E_250:365). Our results showed quite different results during the two years studied. In the summer of 2012, when there was higher rainfall, variations in Zmix were correlated to the optical factors associated with DOM quality, while in the drier summer of 2013 Chl-a, TSS and fetch were the variables that more explained Zmix. It suggests that DOM regulates the Zmix in the rainy periods in the studied tropical lakes and that control is determined by the balance between the DOM input (runoff) and output (such as photodegradation) of the aquatic systems. In reduced rain conditions (summer 2013), the factors responsible by chemistry photodegradation of DOM were predominant, and the organic matter was no longer controlling Zmix, which was driven by internal mixing, productivity, and the wind (Chl-a, TSS and fetch). In this study we showed how changes in precipitation might cause shifts in the factors that regulate the epilimnion thickness in tropical lakes.     

Continuous fluorescence assessment of organic matter variability on the Bournbrook River,Birmingham, UK

Continuous monitoring of dissolved organic matter (DOM) character and concentration at hourly resolution is rare, despite the importance of analysing organic matter variability at high‐temporal resolution to evaluate river carbon budgeting, river water health by detecting episodic pollution and to determine short‐term variations in chemical and ecological function. The authors report a 2‐week experiment performed on DOM sampled from Bournbrook, Birmingham, UK, an urban river for which spectrophotometric (fluorescence, absorbance), physiochemical (dissolved organic carbon [DOC], electrical conductivity, pH) and isotopic (D/H) parameters have been measured at hourly frequency. Our results show that the river had sub‐daily variations in both organic matter concentration and characteristics. In particular, after relatively high‐magnitude precipitation events, organic carbon concentration increased, with an associated increase in intensity of both humic‐like and tryptophan‐like fluorescence. D/H isotopic ratio demonstrates different hydrological responses to different rainfall events, and organic matter character reflects this difference. Events with precipitation < 2 mm typically yielded isotopically heavy water with relatively hydrophilic DOM and relatively low specific absorbance. Events with precipitation > 2 mm had isotopically lighter water with higher specific absorbance and a decrease in the proportion of microbially derived to humic‐like fluorescence. In our heavily urbanized catchment, we interpret these signals as one where riverine DOM is dominated by storm sewer‐derived ‘old’ organic matter at low‐rainfall amounts and a mixed signal at high‐precipitation amounts where ‘event’ surface runoff‐derived organic matter dominate during storm sewer and combined sewer overflow routed DOM. Copyright © 2009 John Wiley & Sons, Ltd.