Effect of nutrient amendments on indigenous hydrocarbon biodegradation in oil-contaminated beach sediments

Nutrient amendment to oil-contaminated beach sediments is a critical factor for the enhancement of indigenous microbial activity and biodegradation of petroleum hydrocarbons in the intertidal marine environment. In this study, we investigated the stimulatory effect of the slow-release fertilizers Osmocote (Os; Scotts, Marysville, OH) and Inipol EAP-22 (Ip; ATOFINA Chemicals, Philadelphia, PA) combined with inorganic nutrients on the bioremediation of oil-spiked beach sediments using an open irrigation system with artificial seawater over a 45-d period. Osmocote is comprised of a semipermeable membrane surrounding water-soluble inorganic N, P, and K. Inipol, which contains organic N and P, has been used for oil cleanup on beach substrate. Nutrient concentrations and microbial activity in sediments were monitored by analyzing sediment leachates and metabolic dehydrogenase activity of the microbial biomass, respectively. Loss of aliphatics (n-C12 to n-C33, pristane, and phytane) was significantly greater (total loss between 95 and 97%) in oil-spiked sediments treated with Os alone or in combination with other nutrient amendments, compared with an unamended oil-spiked control (26% loss) or sediments treated with the other nutrient amendments (28-65% loss). A combination of Os and soluble nutrients (SN) was favorable for the rapid metabolic stimulation of the indigenous microbial biomass, the sustained release of nutrients, and the enhanced biodegradation of petroleum hydrocarbons in leached, oil-contaminated sediments.     

Biodegradation of polycyclic aromatic hydrocarbons in oil-contaminated beach sediments treated with nutrient amendments

Microbial biodegradation of polycyclic aromatic hydrocarbons (PAHs) during the process of bioremediation can be constrained by lack of nutrients, low bioavailability of the contaminants, or scarcity of PAH-biodegrading microorganisms. This study focused on addressing the limitation of nutrient availability for PAH biodegradation in oil-contaminated beach sediments. In our previous study, three nutrient sources including inorganic soluble nutrients, the slow-release fertilizer Osmocote (Os; Scotts, Marysville, OH) and Inipol EAP-22 (Ip; ATOFINA Chemicals, Philadelphia, PA), as well as their combinations, were applied to beach sediments contaminated with an Arabian light crude oil. Osmocote was the most effective nutrient source for aliphatic biodegradation. This study presents data on PAH biodegradation in the oil-spiked beach sediments amended with the three nutrients. Biodegradation of total target PAHs (two- to six-ring) in all treatments followed a first-order biodegradation model. The biodegradation rates of total target PAHs in the sediments treated with Os were significantly higher than those without. On Day 45, approximately 9.3% of total target PAHs remained in the sediments amended with Os alone, significantly lower than the 54.2 to 58.0% remaining in sediment treatments without Os. Amendment with Inipol or soluble nutrients alone, or in combination, did not stimulate biodegradation rates of PAHs with a ring number higher than 2. The slow-release fertilizer (Os) is therefore recommended as an effective nutrient amendment for intrinsic biodegradation of PAHs in oil-contaminated beach sediments.     

Temporal and spatial distributions of sediment total organic carbon in an estuary river

Understanding temporal and spatial distributions of naturally occurring total organic carbon (TOC) in sediments is critical because TOC is an important feature of surface water quality. This study investigated temporal and spatial distributions of sediment TOC and its relationships to sediment contaminants in the Cedar and Ortega Rivers, Florida, USA, using three-dimensional kriging analysis and field measurement. Analysis of field data showed that large temporal changes in sediment TOC concentrations occurred in the rivers, which reflected changes in the characteristics and magnitude of inputs into the rivers during approximately the last 100 yr. The average concentration of TOC in sediments from the Cedar and Ortega Rivers was 12.7% with a maximum of 22.6% and a minimum of 2.3%. In general, more TOC accumulated at the upper 1.0 m of the sediment in the southern part of the Ortega River although the TOC sedimentation varied with locations and depths. In contrast, high concentrations of sediment contaminants, that is, total polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs), were found in sediments from the Cedar River. There was no correlation between TOC and PAHs or PCBs in these river sediments. This finding is in contradiction to some other studies which reported that the sorption of hydrocarbons is highly related to the organic matter content of sediments. This discrepancy occurred because of the differences in TOC and hydrocarbon source input locations. It was found that more TOC loaded into the southern part of the Ortega River, while almost all of the hydrocarbons entered into the Cedar River. This study suggested that the locations of their input sources as well as the land use patterns should also be considered when relating hydrocarbons to sediment TOC.     

The impact of urbanization on tropical mangroves (Fortaleza,Brazil): Evidence from PAH distribution in sediments

This investigation represents the first environmental diagnosis of the distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in sediments from a tropical mangrove in Fortaleza, northeastern Brazil. Sediment cores from six sampling stations in the Cocó and Ceará Rivers were retrieved in June-July 2006 to determine 17 priority PAHs. The total PAH concentrations (Σ_PAHs) ranged from 3.04 to 2234.76 μg kg^?1(Cocó River) and from 3.34 to 1859.21 μg kg^?1 (Ceará River). These levels are higher than those of other cities with more industrial development. PAH concentrations did not reach probable effect levels (PELs). However, from 4.5 to 87.5% of individual PAH concentrations can occasionally cause adverse biological effects for aquatic organisms. The PAH molecular ratios indicate that the PAHs in the sediment core were derived mainly from petroleum, wood, and charcoal combustion (pyrogenic source), and that atmospheric deposition and urban runoff may serve as important pathways for PAH input to the sediment. Clearly, the Σ_PAHs in sediments collected in the Cocó and Ceará Rivers indicate that ongoing pollution is more severe than past pollution.     

Landscape metrics and estuarine sediment contamination in the mid-Atlantic and southern New England regions

In a previously published study, quantitative relationships were developed between landscape metrics and sediment contamination for 25 small estuarine systems within Chesapeake Bay. These analyses have been extended to include 75 small estuarine systems across the mid-Atlantic and southern New England regions of the USA. Because of the different characteristics and dynamics of the estuaries across these regions, adjustment for differing hydrology, sediment characteristics, and sediment origins were included in the analysis. Multiple linear regression with stepwise selection was used to develop statistical models for sediment metals, organics, and total polycyclic aromatic hydrocarbons (PAHs). The landscape metrics important for explaining the variation in sediment metals levels (R2 = 0.72) were the percent area of nonforested wetlands (negative contribution), percent area of urban land, and point source effluent volume and metals input (positive contributions). The metrics important for sediment organics levels (R2 = 0.5) and total PAHs (R2 = 0.46) were percent area of urban land (positive contribution) and percent area of nonforested wetlands (negative contribution). These models included silt-clay content (metals) or total organic C (organics, total PAHs) of sediments and grouping by estuarine hydrology, suggesting the importance of sediment characteristics and hydrology in mitigating the influence of the landscape metrics on sediment contamination levels. The overall results from this study are indicative of how statistical models can be developed relating landscape metrics to estuarine sediment contamination for distributions of land cover and point source discharges.     

极端环境下的石油烃生物降解及其在生物修复中的应用

文章综合论述了微生物在高温、低温、高盐等极端条件下对石油烃的生物降解过程,研究了生物降解在生物修复中的应用效果。同时,还介绍了对于强酸、强碱及高压条件下石油烃生物降解的研究状况,论述了研究石油烃生物降解对开发和丰富微生物资源的重要性。     

三峡库区典型次级支流表层沉积物中PAHs的分布特征及来源分析

本文表征了三峡库区典型次级支流(梁滩河)表层沉积物中18种多环芳烃(PAHs)的浓度,并对其分布特征和污染来源进行了探讨。18种PAHs的总浓度(∑18 PAHs)范围为198.5～4349 ng/g-dw(干重),平均浓度为1441ng/g,中值为1160 ng/g。与其他地区沉积物污染情况相比,梁滩河沉积物中PAHs浓度处于中等偏低的污染程度,支流污染程显著高于干流,流经城镇的右支污染程度显著高于流经农村或人口较少的左支和主干流。大部分采样点以高环(4～6环)PAHs污染为主。PAHs源解析结果表明,梁滩河表层沉积物中PAHs污染以燃烧源为主,主要源于化石燃料和生物质的不完全燃烧。沉积物中苯并[a]芘的毒性当量因子(TEF)值为39.38～384.37 ngTEQ/g,平均值110.94 ngTEQ/g。生态风险评价的结果表明,右支流的两个采样点R3和R4点沉积物中PAHs可能存在生物负效应影响,R4点的高风险可能与附近白市驿机场污染有关。     

Incidence of adverse biological effects within ranges of chemical concentrations in marine and estuarine sediments

Matching biological and chemical data were compiled from numerous modeling, laboratory, and field studies performed in marine and estuarine sediments. Using these data, two guideline values (an effects range-low and an effects range-median) were determined for nine trace metals, total PCBs, two pesticides, 13 polynuclear aromatic hydrocarbons (PAHs), and three classes of PAHs. The two values defined concentration ranges that were: (1) rarely, (2) occasionally, or (3) frequently associated with adverse effects. The values generally agreed within a factor of 3 or less with those developed with the same methods applied to other data and to those developed with other effects-based methods. The incidence of adverse effects was quantified within each of the three concentration ranges as the number of cases in which effects were observed divided by the total number of observations. The incidence of effects increased markedly with increasing concentrations of all of the individual PAHs, the three classes of PAHs, and most of the trace metals. Relatively poor relationships were observed between the incidence of effects and the concentrations of mercury, nickel, total PCB, total DDT and p,p′-DDE. Based upon this evaluation, the approach provided reliable guidelines for use in sediment quality assessments. This method is being used as a basis for developing National sediment quality guidelines for Canada and informal, sediment quality guidelines for Florida. The methods and guidelines presented in this report do not necessarily represent the policy of the National Oceanic and Atmospheric Administration, Environment Canada, or Florida Department of Environmental Protection.     

微生物对石油烃类的降解机理

文章分析了生物降解需要的条件、环境因素对石油烃微生物降解的影响,石油烃类的有氧降解机理、有氧降解方式,石油烃类的厌氧降解机理、厌氧降解过程中某些无机含氧化合物作受氢体的递氢过程,石油烃类化合物微生物降解难易程度,提出了以后应进一步重视原油的生物降解应用于我国微生物采油的研究。     

西溪湿地底泥质量现状与生态风险初步评价

为了解西溪湿地底泥质量现状,2012年9月采集保护区内不同干扰类型的底泥样本,测试了底泥中重金属和POPs中PCBs、OCPs和PAHs的含量,并对湿地底泥污染进行了生态风险初步评价。结果表明,底泥中未检出PCBs和OCPs,但检测出14种EPA优控PAHs,总PAHs的浓度范围为115.9～217.8 ng·g^-1,低于潜在生态风险的效应区间低值ERL,其中列入中国＂水中优先控制污染黑名单＂的7种PAHs均有检出并且其总量占∑PAHs 1/2左右（平均为50.08%）;底泥中8种重金属含量平均值低于《土壤环境质量标准》（GB 15618—1995）的二级标准,但Hg、Zn、Pb、Ni含量在多个位点已超过一级标准;分别采用土壤背景值和国家一级标准为参比值对湿地底泥中重金属进行单因子污染风险指数评价,发现分别有7种和4种元素的污染指数大于1;综合分析不同干扰类型的底泥质量,发现底泥疏浚能有效降低有机质含量、全氮和PAHs含量,但对全磷、重金属含量则无明显效果,封闭水体的干塘措施能显著减少污泥量和有机物含量。研究结果表明,西溪湿地底泥中高环PAHs和重金属污染水平可能对西溪湿地生物具有潜在的生物毒性作用及不利的生态影响效应,其疏浚底泥农用则无生态风险。     

Sequential accelerated solvent extraction of polycyclic aromatic hydrocarbons with different solvents: performance and implication

Sixteen USEPA priority polycyclic aromatic hydrocarbons (PAHs) extracted by Soxhlet extraction (S-PAHs) with dichloromethane and routine accelerated solvent extraction (A-PAHs) with 1:1 toluene/methanol, respectively, were investigated in 24 soil samples from two cities in the center of the Pearl River Delta, South China. Polycyclic aromatic hydrocarbons, methylphenanthrene and perylene, in two soils, two sediments, and an immature oil shale were also sequentially extracted by accelerated solvent extraction (ASE) with each of four different organic solvents for three times. The A-PAHs' concentrations are 2.41 times the S-PAHs' concentrations. For sequential three ASEs, PAHs in the first extract account for 56 to 67% of their total concentrations in the sequential three extractions and toluene displays the best extraction performance among the four solvents. Diagnostic ratios of PAHs in Soxhlet extraction, routine ASE, and sequential ASE with each solvent for a given sample are very similar, suggesting their identical petrogenic and pyrogenic sources in the soils and sediments. But the PAH ratios for the shale have an obvious petrogenic origin. The perylene/5-ring PAH ratios indicate a diagenetic source, especially in the shale and sediments. The correlation analysis shows that A-PAHs/S-PAHs is better associated with the contents of total organic carbon (TOC) than those of black carbon (BC). The above results indicate the significant petrogenic origin of PAHs and the important effect of organic matter on their extraction and distribution in the investigated field soils/sediments.     

Phytoremediation of aged petroleum sludge: effect of inorganic fertilizer

Phytoremediation is a promising new technology that uses higher plants to enhance biodegradation. Nutrient availability is an important factor governing the success of phytoremediation and can be regulated through the addition of fertilizer. A greenhouse study was conducted to assess the importance of nitrogen and phosphorus for the phytoremediation of petroleum sludge. Degradation of total petroleum hydrocarbons (TPH) was quantified for six fertilization rates and three vegetation treatments: bermuda grass [Cynodon dactylon (L.) Pers.], tall fescue (Festuca arundinacea Schreb.), and an unvegetated control. During the first 6 mo of the experiment, TPH declined by an average of 49% with no significant differences between treatments. After 1 yr, TPH degradation was significantly greater in both vegetated treatments with a mean TPH reduction of 68% for bermuda, 62% for fescue, and 57% for the unvegetated control. Degradation of TPH in the fescue and bermuda treatments was significantly lower in the treatments in which no fertilizer was added or N and P were added simply to maintain plant growth compared with the higher rates of fertilization. For this short-term, greenhouse experiment, optimal remediation was obtained by fertilization that produced a C to N to P ratio of 100:2:0.2.     

9,10-Phenanthrenequinone photoautocatalyzes its formation from phenanthrene, and inhibits biodegradation of naphthalene

Polycyclic aromatic hydrocarbons (PAHs) have earned considerable attention due to their widespread environmental distribution and toxicity. In the environment, PAHs decompose by a variety of biotic and abiotic pathways. In both polar and nonpolar environments, phenanthrene (Phe, a common, three-ring PAH) is converted by sunlight to more polar products such as 9,10-phenanthrenequinone (PheQ) and subsequent oxidation products such as the corresponding open-ring dicarboxylic acid product. Biodegradation of phenanthrene also usually leads to oxidative metabolites, and eventually ends in mineralization. Our experimental objective was to investigate the photodegradation of phenanthrene and determine the effect of reaction products such as PheQ on microbial biodegradation of two- and three-ring PAHs. Abiotic experiments were performed to examine the photolytic breakdown of Phe; Phe was converted to PheQ, which catalyzed its own formation. In biodegradation experiments PheQ (0.04-4 mg/L) caused marked inhibition of naphthalene (Nap) biodegradation by a Burkholderia species; Phe did not. Only 20% of the naphthalene was degraded in the presence of PheQ compared with 75% in the control culture with no PheQ added. No PAH-degrading cultures were able to use PheQ as sole carbon source; however, the Phe-degrading enrichment culture dominated by a Sphingomonas species was able to degrade PheQ cometabolically in the presence of Phe. These results may explain why photooxidized phenanthrene-containing mixtures can resist biodegradation.     

Petroleum hydrocarbons and limiting nutrients in <Emphasis Type="Italic">Macura reptantia</Emphasis>, <Emphasis Type="Italic">Procambarus clarkii</Emphasis> and benthic sediment from Qua Iboe Estuary,Nigeria

The levels of total petroleum hydrocarbons in two commonly consumed benthopelagic shellfishes, Macura reptantia and Procambarus clarkii, harvested from benthic sediment of Qua Iboe Estuary were determined using a gas chromatography with flame-ionization detector. Seventy-two (72) samples each of benthic sediment and the shellfishes were collected monthly between June 2003 and February 2004 covering the peak periods of the wet and dry seasons. Concentrations of hydrocarbons were highly variable and ranged between 5.00 and 232.00 μg/g dry weight of benthic sediment, 3.05 and 11.30 μg/g dry weight of M. reptantia, 1.62 and 9.00 μg/g dry weight of P. clarkii. Pearson’s correlation analysis of total hydrocarbon concentrations in subtidal sediments with levels in the fauna species yielded positive significant (P < 0.05) correlations in M. reptantia (r = 0.737) and P. clarkii (r = 0.924). This is indicative of a long term and chronic accumulation of hydrocarbons in the estuarine ecosystem, reflecting the potential for exposure of the resident biota and the risk to human health.     

Effects of plants on the removal of hexavalent chromium in wetland sediments

The effect of two wetland plants, Typha latifolia L. (cattail) and Phragmites australis (Cav.) Trin. ex Steud (common reed), on the fate of Cr(VI) in wetland sediments was investigated using greenhouse bench-scale microcosm experiments. The removal of Cr(VI) was monitored based on the vertical profiles of aqueous Cr(VI) in the sediments. The Cr(VI) removal rates were estimated taking into account plant transpiration, which was found to significantly concentrate dissolved species in the sediments. After correcting for evapotranspiration, the actual Cr(VI) removal rates were significantly higher than would be inferred from uncorrected profiles. On average, the Cr(VI) removal rates were 0.005 to 0.017 mg L(-1) d(-1), 0.0003 to 0.08 mg L(-1) d(-1), and 0.004 to 0.13 mg L(-1) d(-1) for the control, T. latifolia, and P. australis microcosms, respectively. The fate of the removed Cr(VI) was examined by determining the quantity and chemical speciation of the Cr in the sediment and plant materials. Chromium(III) was the dominant form of Cr in both the sediment and plants, and precipitation of Cr(III) in the sediment was the major pathway responsible for the disappearance of aqueous Cr(VI) from the pore water. Incubation results showed that abiotic reduction was the primary mechanism underlying Cr(VI) removal in the microcosm sediments. Organic compounds produced by plants, including root exudates and mineralization products of dead roots, are thought to be the factor that is either directly or indirectly responsible for the gap between Cr(VI) removal efficiencies in the sediments of the vegetated and unvegetated microcosms.     

Nitrogen and phosphorus flux rates from sediment in the lower St. Johns River estuary

Internal cycling of nutrients from the sediment and water column can be an important contribution to the total nutrient load of an aquatic ecosystem. Our objective was to estimate the internal nutrient loading of the Lower St. Johns River (LSJR). Dissolved reactive phosphorus (DRP) and ammonium (NH(4)-N) flux from sediments were measured under aerobic and anaerobic water column conditions using intact cores, to estimate the overall contribution of the sediments to P and N loading to the LSJR. The DRP flux under aerobic water column conditions averaged 0.13 mg m(-2) d(-1), approximately 37 times lower than that under anaerobic conditions (4.77 mg m(-2) d(-1)). The average NH(4)-N released from the anaerobic cores (18.03 mg m(-2) d(-1)) was also significantly greater than in the aerobic cores for all sites and seasons, indicating the strong relationship between nutrient fluxes and oxygen availability in the water column. The mean annual internal DRP load was estimated to be 330 metric tons (Mg) yr(-1), 21% of the total P load to the river, while the mean annual internal load of NH(4)-N was determined to be 2066 Mg yr(-1), 28% of the total N load to the LSJR estuary. As water resource managers reduce external loading to the LSJR the frequency of anaerobic events should decline, thereby reducing nutrient fluxes from the sediment to the water column, reducing the internal loading of DRP and NH(4)-N. Results from this study demonstrate that the internal flux of nutrients from sediments may be a significant portion of the total load and should be accounted for in the total nutrient budget of the river for successful restoration.     

Genotoxicity is unrelated to total concentration of priority carcinogenic polycyclic aromatic hydrocarbons in soils undergoing biological treatment

A solid-phase microbiological assay was used to determine the changes in genotoxicity associated with sequestration or biodegradation of carcinogenic compounds in contaminated soils. The concentration of six carcinogenic polycyclic aromatic hydrocarbons (PAHs) did not change in 59 d in sterile soil, but the genotoxicity declined markedly. In a soil undergoing bioremediation in the field for 147 d or biodegradation in the laboratory for 180 d, the concentrations either changed little or declined at different rates, but the genotoxicity increased followed by a decline. The genotoxicity of a second soil declined as a result of biological treatment. The data show that genotoxicity of contaminated soils may be unrelated to the concentration of carcinogenic PAHs because of aging or new mutagens formed during biological treatment.     

Selenium distribution and fluxes in intertidal wetlands, San Francisco Bay, California

Selenium (Se) concentrations exceeding ecological guidelines for sediments and suspended particulate matter (SPM) have been observed in the northern reach of the San Francisco Bay estuary. Longterm availability of elevated Se in wetland sediments depends in part on the fluxes controlling Se distribution. The relative contribution of sedimentary vs. post-depositional Se fluxes in two San Francisco Bay intertidal wetlands was estimated. Selenium concentrations on surface wetland sediments were compared with levels on SPM, and with previously established background levels in San Francisco Bay sediments. Sediment Se fluxes to the wetlands were measured directly using sediment traps. Although dissolved Se concentrations are higher than particulate Se concentrations in San Francisco Bay water, sediment input into the system provides the major flux of Se. Strong correlation between Se and C on SPM (r2 = 0.81) indicates the importance of organic particulate deposition. Dependence on sediment texture was qualitatively established by measuring Se on particle-size separates. Normalization to Al showed that 65% of Se spatial variability is related to sediment texture. Selenium is further enriched in the marsh via post-depositional inputs, probably due to in situ adsorption from overlying water and chemical reduction. According to sediment flux measurements, enrichment in the marsh is equivalent to 20 to 25% of the particulate Se flux, thereby defining the marsh as a Se sink. These findings highlight the need for more intensive monitoring of SPM as the major source of Se to intertidal wetlands.     

苯和菲在含水层的典型介质中迁移转化研究

石油烃污染会对人类生存的环境造成严重危害,地下水系统中石油烃污染物的研究已受到国内外的高度重视。本文针对某石油烃污染场地的污染状况及水文地质条件,利用模拟柱实验研究石油烃中常见组分苯和菲在典型含水层中的迁移转化,实验结果表明,苯和菲在4种含水层介质中(粉砂、中砂、粗砂、砾砂)受到的迁移阻滞作用都是随着粒径的减小而增大。菲在4种介质中的迁移速率要小于苯,说明4种介质对菲的阻滞作用要大于苯。通过检测各模拟柱出水中Fe2+、Fe3+、NH4+-N和NO3--N浓度的变化可知,在苯和菲的砾砂模拟柱中,由于水流速度快,试验周期短,模拟柱内各项指标变化较小,生物作用较弱;而在苯和菲的粗砂、中砂和粉砂模拟柱中,NO3--N浓度减少,NH4+-N和Fe3+含量增加,说明微生物开始利用NO3--N和Fe3+降解苯和菲,微生物对苯和菲在粗砂、中砂和粉砂中的迁移转化过程有显著的作用。