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1.
C Taylor  T Viraraghavan 《Chemosphere》1999,39(10):1583-1593
A bench-scale investigation (soil pan testing) was conducted with the objective of studying degradation rates of diesel contaminated soil (2500 and 10,000 ppm by weight of total petroleum hydrocarbons (TPH) to dry weight of soil) under different treatment conditions over a 17 week testing period. The greatest degradation of the diesel contaminated soil was obtained with the addition of nutrients (Co = 10,000 ppm of TPH; k = 0.19 week-1). 'k' for soil not amended with nutrients was 0.07 week-1. The control cell (C0 = 2500 ppm TPH), with sodium azide (to suppress degradation) was compared with an experimental cell of 2500 ppm initial concentration of TPH without nutrient amendment. The control cell exhibited a relatively low uniform degradation (k = 0.08 week-1) of TPH over the duration of the experiment with reasonable first-order kinetic regression statistics.  相似文献   

2.
Composting of contaminated soil in biopiles is an ex situ technology, where organic matter such as bark chips are added to contaminated soil as a bulking agent. Composting of lubricating oil-contaminated soil was performed in field scale ( [Formula: see text] m(3)) using bark chips as the bulking agent, and two commercially available mixed microbial inocula as well as the effect of the level of added nutrients (N,P,K) were tested. Composting of diesel oil-contaminated soil was also performed at one level of nutrient addition and with no inoculum. The mineral oil degradation rate was most rapid during the first months, and it followed a typical first order degradation curve. During 5 months, composting of the mineral oil decreased in all piles with lubrication oil from approximately 2400 to 700 mg (kg dry w)(-1), which was about 70% of the mineral oil content. Correspondingly, the mineral oil content in the pile with diesel oil-contaminated soil decreased with 71% from 700 to 200 mg (kg dry w)(-1). In this type of treatment with addition of a large amount of organic matter, the general microbial activity as measured by soil respiration was enhanced and no particular effect of added inocula was observed.  相似文献   

3.
Yu DY  Kang N  Bae W  Banks MK 《Chemosphere》2007,66(5):799-807
Although alkanes are relatively less reactive to chemical oxidation compared to alkenes, the chemical oxidation of alkanes has not been adequately explored in the context of environmental remediation efforts. Laboratory-scale column experiments were therefore conducted with soil artificially contaminated by diesel fuel as a surrogate for alkanes of environmental relevance. Particular attention was paid to saturated hydrocarbons refractory to volatilization. Reaction conditions involve 1485mgkg(-1) of the initial concentration of diesel range organics (DRO) and a constant ozone concentration of 119+/-6mgl(-1) at the flow rate of 50mlmin(-1). The observed removal of DRO reached 94% over 14h of continuous ozone injection. Ozone oxidation demonstrated effective removal of non-volatile DRO in the range of C(12)-C(24). Each alkane compound displayed comparable degradation kinetics, suggesting virtually no selectivity of ozone reactions with alkanes in soil. A pseudo-first order kinetic model closely simulated the removal kinetics, yielding a reaction rate constant of 0.213 (+/-0.021)h(-1) and a half-life of 3.3 (+/-0.3)h under the experimental conditions used in this study. An estimate of ozone demand was 32mg of O(3) (mgDRO)(-1).  相似文献   

4.
Mesocosm studies using sub-Antarctic soil artificially contaminated with diesel or crude oil were conducted in Kerguelen Archipelago (49 degrees 21' S, 70 degrees 13' E) in an attempt to evaluate the potential of a bioremediation approach in high latitude environments. All mesocosms were sampled on a regular basis over six months period. Soils responded positively to temperature increase from 4 degrees C to 20 degrees C, and to the addition of a commercial oleophilic fertilizer containing N and P. Both factors increased the hydrocarbon-degrading microbial abundance and total petroleum hydrocarbons (TPH) degradation. In general, alkanes were faster degraded than polyaromatic hydrocarbons (PAHs). After 180 days, total alkane losses of both oils reached 77-95% whereas total PAHs never exceeded 80% with optimal conditions at 10 degrees C and fertilizer added. Detailed analysis of naphthalenes, dibenzothiophenes, phenanthrenes, and pyrenes showed a clear decrease of their degradation rate as a function of the size of the PAH molecules. During the experiment there was only a slight decrease in the toxicity, whereas the concentration of TPH decreased significantly during the same time. The most significant reduction in toxicity occurred at 4 degrees C. Therefore, bioremediation of hydrocarbon-contaminated sub-Antarctic soil appears to be feasible, and various engineering strategies, such as heating or amending the soil can accelerate hydrocarbon degradation. However, the residual toxicity of contaminated soil remained drastically high before the desired cleanup is complete and it can represent a limiting factor in the bioremediation of sub-Antarctic soil.  相似文献   

5.
针对柴油污染土壤生物修复技术效率低的问题,通过构建高效降解菌群修复柴油污染的土壤,采用组合优化和正交实验构建最佳组合与接种比例的菌群,并研究其柴油降解特性。结果表明,通过筛选、鉴定并命名的4株柴油降解菌为Bacillus sp. VOC18-L1、Enterococcus faecalis-L2、Lysinibacillus-L3、Rhodococcus equi-L4;当4株菌接种比例为3∶1∶3∶4,pH = 7.0,30 ℃,转速150 r·min−1时,柴油降解的效果最佳,14 d对7.0 mL·L−1的柴油降解率达到89.0%。通过气相色谱质谱联用仪(GC-MS)检测柴油降解产物,发现该混合菌株能将柴油中的烷烃降解为短链烷烃,最终转化为小分子物质。同时利用KEGG数据库获得代谢丰度图并初步预测每种菌的功能,根据微生物多样性测试结果,进一步证明了混合菌对柴油完全降解的效果优于单种菌种。通过人工构建的微生物菌群可以有效地应用于柴油污染土壤的修复。  相似文献   

6.
The biodegradation of aliphatic and aromatic hydrocarbons by natural soil microflora and seven fungi species, including imperfect strains and higher level lignolitic species, is compared in a 90-day laboratory experiment using a natural, not-fertilized soil contaminated with 10% crude oil. The natural microbial soil assemblage isolated from an urban forest area was unable to significantly degrade crude oil, whereas pure fungi cultures effectively reduced the residues by 26-35% in 90 days. Normal alkanes were almost completely degraded in the first 15 days, whereas aromatic compounds (phenanthrene and methylphenanthrenes) exhibited slower kinetics. Aspergillus terreus and Fusarium solani, isolated from oil-polluted areas, produced the more efficient attack of aliphatic and aromatic hydrocarbons, respectively. Overall, imperfect fungi isolated from polluted soils showed a somewhat higher efficiency, but the performance of unadapted, indigenous, lignolitic fungi was comparable, and all three species, Pleurotus ostreatus, Trametes villosus and Coriolopsis rigida, effectively degraded aliphatic and aromatic components. The simultaneous, multivariate analysis of 22 parameters allowed the elucidation of a clear reactivity trend of the oil components during biodegradation: lower molecular weight n-alkanes > phenanthrene > 3-2-methylphenanthrenes > intermediate chain length n-alkanes > longer chain length n-alkanes > isoprenoids approximately 9-1-methylphenanthrenes. Irrespective of the individual degrading capacities, all fungi species tested seem to follow this decomposition sequence.  相似文献   

7.
Phytoremediation is a promising technique for cleaning petroleum contaminated soils. In this study, the effects of two grass species (Festuca arundinacea Schreb. and Festuca pratensis Huds.), infected (E(+)) and non-infected (E(-)) by endophytic fungi (Neotyphodium coenophialum and Neotyphodium uncinatum, respectively) on the degradation of petroleum hydrocarbons in an aged petroleum contaminated soil was investigated. Plants were grown in the soil for 7 months and unplanted soil considered as control. At the end of the experiment, total and oil-degrading bacteria, dehydrogenase activity, water-soluble phenols, total petroleum hydrocarbons (TPH) and polycyclic aromatic hydrocarbons (PAHs) contents were measured in the soil. The results demonstrated that E(+) plants contained more root and shoot biomass than E(-) plants and created higher levels of water-soluble phenols and dehydrogenase activity in the soil, while there was no significant difference in bacterial counts of planted soils. Planting stimulated total and oil-degrading bacterial numbers, dehydrogenase activity and the soil content of water-soluble phenols. Regardless of endophyte infection, PAH and TPH removal in the rhizosphere of plants were 80-84 and 64-72% respectively, whereas the removals in controls were 56 and 31%, respectively. It was revealed that TPHs in retention time range of n-alkanes with C(10)-C(25) chain lengths and TPH were more degraded in the rhizosphere of E(+) plants compared to E(-) ones. Thus, grasses infected with endophytic fungi could be more efficient for removal of TPH from oil-contaminated soils.  相似文献   

8.
The influence of oil concentration on hydrocarbon biodegradation in a sandy sediment was studied in polyvinyl chloride reactors (0.45 x 0.28 x 0.31 m) containing 76.8 kg of beach sand in natura, where the upper layer was artificially contaminated with petroleum. The oil-degrading microorganisms used consisted of a mixed culture named ND, obtained from landfarming and associated with indigenous microorganisms. On the 28th day of the process, the degradation in reactors containing sandy sediment contaminated with light Arabian oil and presenting an initial oil content of 14, 21 or 28 g kg-1 reached the following levels (%): 33.7, 32.9 and 28.9 for oil and grease; up to 88.3, 35.3 and 13.0 for C14-C26 n-alkanes; and 100, 61.3 and 59.4 for pristane, respectively. Phytane removal (37.1%) was only detected in the reactor contaminated with the lowest oil concentration studied. These results, together with the expressive bacterial growth observed (from 10(6) to 10(11) cfu g-1) give strong support to the argument that biodegradation was the dominant component of the remediation process. Susceptibility to biodegradation was inversely proportional to increasing oil contamination. The degradation of branched alkane: pristane was not repressed by the presence of n-alkanes.  相似文献   

9.
Contamination of soil with hydrocarbons occurs frequently when petroleum ducts are damaged. Restoration of those contaminated soils might be achieved by applying readily available organic material. An uncontaminated clayey soil sampled in the vicinity of a duct carrying diesel which ruptured recently, was contaminated in the laboratory and amended with or without maize or biosolids while production of carbon dioxide (CO(2)), dynamics of ammonia (NH(4)(+)), nitrates (NO(3)(-)), and total petroleum hydrocarbons (TPH) were monitored. The fastest mineralization of diesel, as witnessed by production of CO(2), was found when biosolids were added, but the amount mineralized after 100 days, approximately 88%, was similar in all treatments. Approximately 5 mg of the 48 mg TPH kg(-1) found in the sterilized soil at the beginning of the experiment could not be accounted for after 100 days. The concentration of TPH in the unsterilized soil decreased rapidly in all treatments, but the rate of decrease was different between the treatments. The fastest decrease was found in the soil amended with biosolids and approximately 30 mg TPH kg(-1) or 60% could not be accounted for within 7 days. The decrease in concentration of TPH at the onset of the incubation was similar in the other treatments. After 100 days, the concentration of TPH was similar in all soils and appear to stabilize at 19 mg TPH kg(-1) soil. It was concluded that biosolids accelerated the decomposition of diesel and TPH due to its large nutrient content, but after 100 days the amount of diesel mineralized and the residual concentration of TPH was not affected by the treatment applied.  相似文献   

10.
Influence of salinity on bioremediation of oil in soil   总被引:11,自引:0,他引:11  
Spills from oil production and processing result in soils being contaminated with oil and salt. The effect of NaCl on degradation of oil in a sandy-clay loam and a clay loam soil was determined. Soils were treated with 50 g kg(-1) non-detergent motor oil (30 SAE). Salt treatments included NaCl amendments to adjust the soil solution electrical conductivities to 40, 120, and 200 dS m(-1). Soils were amended with nutrients and incubated at 25 degrees C. Oil degradation was estimated from the quantities of CO(2) evolved and from gravimetric determinations of remaining oil. Salt concentrations of 200 dS m(-1) in oil amended soils resulted in a decrease in oil mineralized by 44% for a clay loam and 20% for a sandy-clay loam soil. A salt concentration of 40 dS m(-1) reduced oil mineralization by about 10% in both soils. Oil mineralized in the oil amended clay-loam soil was 2-3 times greater than for comparable treatments of the sandy-clay loam soil. Amending the sandy-clay loam soil with 5% by weight of the clay-loam soil enhanced oil mineralization by 40%. Removal of salts from oil and salt contaminated soils before undertaking bioremediation may reduce the time required for bioremediation.  相似文献   

11.
This study evaluated the use of sugarcane filter cake and nitrogen, phosphorus and potassium (NPK) fertilization in the bioremediation of a soil contaminated with diesel fuel using a completely randomized design. Five treatments (uncontaminated soil, T1; soil contaminated with diesel, T2; soil contaminated with diesel and treated with 15 % (wt) filter cake, T3; soil contaminated with diesel and treated with NPK fertilizer, T4; and soil contaminated with diesel and treated with 15 % (wt) filter cake and NPK fertilizer, T5) and four evaluation periods (1, 60, 120, and 180 days after the beginning of the experiment) were used according to a 4?×?5 factorial design to analyze CO2 release. The variables total organic carbon (TOC) and total petroleum hydrocarbons (TPH) remaining in the soil were analyzed using a 5?×?2 factorial design, with the same treatments described above and two evaluation periods (1 and 180 days after the beginning of the experiment). In T3 and T5, CO2 release was significantly higher, compared with the other treatments. Significant TPH removal was observed on day 180, when percent removal values were 61.9, 70.1, 68.2, and 75.9 in treatments T2, T3, T4, and T5, respectively, compared with the initial value (T1).  相似文献   

12.
In-vessel composting of polycyclic aromatic hydrocarbons (PAHs) present in contaminated soil from a manufactured gas plant site was investigated over 98 days using laboratory-scale in-vessel composting reactors. The composting reactors were operated at 18 different operational conditions using a 3-factor factorial design with three temperatures (T, 38 degrees C, 55 degrees C and 70 degrees C), four soil to green waste ratios (S:GW, 0.6:1, 0.7:1, 0.8:1 and 0.9:1 on a dry weight basis) and three moisture contents (MC, 40%, 60% and 80%). PAH losses followed first order kinetics reaching 0.015 day(-1) at optimal operational conditions. A factor analysis of the 18 different operational conditions under investigation indicated that the optimal operational conditions for degradation of PAHs occurred at MC 60%, S:GW 0.8:1 and T 38 degrees C. Thus, it is recommended to maintain operational conditions during in-vessel composting of PAH-solid waste close to these values.  相似文献   

13.
为研究RL强化MI修复原油污染土壤的效果,通过盆栽实验,测定了修复过程中微生物、脱氢酶、原油降解率和正构烷烃等变化.结果表明,提取RL具有良好表面和乳化活性.修复过程中微生物数目、脱氢酶和石油降解率具有相关性.RL+MI联合修复对原油的降解效果最显著,第14、21和28天的降解率分别达67.6%、78.6%和81.3%,较MI和RL处理分别提高了22%~24%和32%~38%;细菌、放线菌和霉菌最高生物量分别比CK提高约20、5.8和4.7倍;GC-MS示修复14 d后∑C21-/∑C22+(1.334)和Pr/Ph(1.152)均大于CK,说明降解早期具有高碳正构烷烃、奇数烷烃的降解优势以及对类异戊二烯烷烃的降解.  相似文献   

14.
强化生物通风修复过程中柴油衰减规律及其影响因素研究   总被引:1,自引:0,他引:1  
强化生物通风技术对于修复因地下储油罐泄漏引起的土壤污染具有很大的应用前景。通过室内土柱模拟柴油泄漏污染土壤,从土柱中总石油烃(total petroleum hydrocarbon,TPH)剖面分布随时间的变化及降解模式角度,分析了其自然衰减和强化生物通风过程。结果表明:初始柴油浓度直接影响着各柱在自然衰减和强化生物通风过程中柱内的残余TPH平衡分布曲线的形状和浓度峰值位置;在前期自然衰减过程中(约1个月),当土壤中的柴油浓度为5 000~40 000 mg油/kg土时,整个柱内TPH变化的主要原因是重力扩散迁移的结果;当土壤中的柴油浓度≤5 000 mg油/kg土时,其TPH的变化不仅是重力扩散迁移作用的结果,生物降解作用也存在;通风约2个月后,抽提作用对于保持土柱上部柴油浓度稳定变化的意义较为突出。  相似文献   

15.
Gagni S  Cam D 《Chemosphere》2007,67(10):1975-1981
In the last decade, a refinery plant located in Lido Adriano, East Ravenna (Italy) has been subject to mineral oil contamination. The mineral crude oil, extracted from the offshore in Adriatic sea, consisted of 78% aliphatics, cyclic alkanes and saturated polycyclic hydrocarbons, 9% aromatics, polycyclic aromatic hydrocarbons (PAHs) and alkylated derivatives, and 13% of tars/asphaltenes. Analysis of soil after 10 years of natural attenuation revealed a complete depletion of linear (n-C(9)-C(24)), light aromatics (C1-C3/benzenes) and PAHs (C2/naphthalene, C1/phenanthrene); besides a substantial degradation of isoprenoids prystane and phytane, branched and cyclic alkanes. The remaining contaminants which withstood to natural degradation was saturated polycyclic hydrocarbons (perhydro-PAH derivatives), unsaturated polycyclic hydrocarbons (tetrahydro, dihydro-PAH derivatives), terpanes, steranes and unidentified compounds. Such residues resulted in 80% reduction of its concentration after two months of laboratory treatment. Samples were extracted by organic solvents, separated by silica/alumina gel column chromatography and analyzed by gas chromatography-mass selective detector (GC-MSD). Identification and quantification of aliphatic, cyclic alkanes, typical PAHs, terpanes and steranes were carried out to chromatograms of M/Z=85, 83, individual M/Zs, M/Z=191 and 217, respectively. The present work shows that, among numerous biomarkers present in the source oil, stigmastane and two isomers of hopane showed invariable concentrations after laboratory experiments that mimic natural biodegradation in the field, so they can be used as conserved internal biomarkers. These are very useful tools to assess alterations in less stable classes of saturated compounds contained in petroleum. Marked degradation of perhydro, tetrahydro, dihydro-PAH derivatives in the laboratory treatment has been evidenced.  相似文献   

16.
采用原位强化生物修复技术对某区块石油污染土壤进行为期16个月的生物修复,考察了处置后污染土壤理化性质、微生物学特性以及石油烃组成的纵向分布特征。实验结果表明,经过修复后各土层的石油烃去除率是表层土IN-3(50.42%)中层土IN-2(23.54%)底层土IN-1(10.51%);IN-1处于缺氧环境,存在硫酸盐还原和反硝化作用,使得土壤pH值从7.86±0.03降低至7.27±0.03,土壤总氮从2.53±0.13 g/kg降低至0.77±0.04 g/kg;厌氧菌的种群数量是IN-1(10.43±0.71×104CFU/g)IN-3(6.74±0.39×104CFU/g)IN-2(5.15±0.42×104CFU/g),放线菌数量与石油烃含量显著负相关(r=-0.989,p=0.0110.05);IN-3对饱和份和芳香份的降解率最高,分别达到了70.27%和54.52%,远高于IN-2和IN-1;模拟蒸馏结果表明,IN-3正构烷烃得到了很大程度的去除,缺氧的IN-1对正构烷烃去除得较少;厌氧菌数量与胶质和沥青质去除率之间成正相关关系,对于污染源较为分散的污染区域,采用原位生物强化修复时可以考虑引入厌氧修复。  相似文献   

17.
为了探究堆置法处理油污土壤的作用效果,采用单因素实验确定石油初始浓度、温度、土壤含水量、有机质含量、土壤C/N、菌剂浓度相关因素的水平取值范围。以石油烃降解率为评价指标,再通过正交实验进一步优化相关参数,确定最佳条件。结果表明:以石油初始浓度2%、温度35℃、土壤C/N 10∶1为控制变量;以菌剂浓度(X)、有机质含量(Y)、土壤含水量(Z)为变化因素设计正交实验组合L9(34)。可以得出,堆置法处理油污土壤的最佳水平组合为X2Y2Z3,即菌剂浓度5×109 cfu·kg-1,有机质含量为5%,土壤含水量为60%。  相似文献   

18.
Composting for the removal of polycyclic aromatic hydrocarbons (PAH) from soil was assessed as a treatment option at a former tar contaminated site, alongside conventional land treatment. The key objective of the study was to illustrate differences in the extent of removal of the different PAH compounds undergoing biological treatment. Soil composting led to more extensive PAH removal than did 2 variations on the land treatment process. Soil composting was substantially more effective in removing benzo(a)anthracene, chrysene, benzo(b+k)fluoranthene, benzo(a)pyrene, dibenz(ah)anthracene, indenopyrene and benz (gih)perylene, than the land treatment processes. The extents of removal of these higher molecular weight PAH were at least 50% over the 7 month treatment period where composting was used, whereas degradation did not exceed 5% for each of these PAH compounds in the land treatments over the same period. Implications from the study for the practical and effective composting of PAH compounds in soil, are (1) moisture in the soil-compost mix should be kept constant, (2) fresh organic matter should be used and (3) efforts need to be made to ensure soil is properly homogenized, both prior to and during soil mixing.  相似文献   

19.
The efficiency of rhizosphere biodegradation of petroleum hydrocarbons heterogeneously distributed in soils is dependent on the ability of plant roots to prospect into contaminated zones. Rhizobox experiments were conducted to study the influence of diesel contaminated layers on the spatial distribution and the development of the roots of perennial ryegrass. Root distribution and root and shoot development were monitored over time. The final root and above ground biomass and the final TPH concentration were determined. The spatial distribution of the contaminant as well as the irrigation method used affected root distribution, plant development and TPH degradation and therefore ryegrass remediation potential. The results show that roots colonise fully uncontaminated soil and grow preferentially between zones of contamination. Conversely, when no immediate uncontaminated soil is available, roots grow through contaminated zones in order to prospect for uncontaminated soil.  相似文献   

20.
Background, Aims and Scope In oil spill investigations, one of the most important steps is a proper choice of approaches that imply an investigation of samples taken from different sedimentary environments, samples of oil contaminants taken in different periods of time and samples taken at different distances from the oil spill. In all these cases, conclusion on the influence of the environment, microorganisms or migration on the oil contaminants' composition can be drawn from the comparison of chemical compositions of the investigated contaminants. However, in case of water contaminants, it is very important to define which part of organic matter has been analyzed. Namely, previous investigations showed that there were some differences in chemical composition of the same oil contaminant depending on the intensity of its contact with ground water. The aim of this work is to define more precisely the interactions between oil contaminant and water, i.e. the influence of the intensity of interaction between the oil contaminant and water on its chemical composition. The study was based on a comparison of four fractionated extracts of an oil pollutant, after they had been analyzed in details. Methods Oil polluted surface water (wastewater canal, Pančevo, Serbia) was investigated. The study was based on a comparison of four extracts of an oil contaminant: extract 1 (decanted part), and extracts 2, 3 and 4 (extracted by shaking for 1 minute, 5 minutes and 24 hours, respectively). The fractionated extracts were saponified with a solution of KOH in methanol, and neutralized with 10% hydrochloric acid. The products were dissolved in a mixture of dichloromethane and hexane, and individually fractionated by column chromatography on alumina and silica gel (saturated hydrocarbon, aromatic, alcohol and fatty acid fractions). n-Alkanes and isoprenoid aliphatic alkanes, polycyclic alkanes of sterane and triterpane types, alcohols and fatty acids were analyzed using gas chromatography (GC) and gas chromatography-mass spectrometry (GC-MS). δ13CPDB values of individual n-alkanes in the aliphatic fractions were determined using gas chromatography-isotope ratio monitoring-mass spectrometry (GC-irmMS). Results and discussion. Extracts 1 and 2 are characterized by uniform distribution of n-alkanes, whereas extract 3 is characterized by an even-numbered members dominating the odd-ones, and extract 4 showed a bimodal distribution. Extract 1 is characterized by the least negative δ13CPDB values of C19-C26 n-alkanes. Sterane and triterpane analysis confirmed that all extracts originated from the same oil contaminant. n-Fatty acids, C19-C24, in all extracts are very low, being somewhat higher in extract 4. Even-numbered n-alcohols, C12–C16, were identified in the highest concentration in extract 3. It was assumed that algae were responsible for the composition of extract 3. Furthermore, a possible reason for higher concentrations of C19–C26 n-alkanes and C19–C24 fatty acids in extract 4 is the formation of inclusion compounds with colloidal micelles formed between the oil contaminant's NSO-compounds and water. Conclusion It was undoubtedly confirmed that there were specific differences in the compositions of the different extracts depending on the intensity of the interaction between the oil contaminant and the surface water. Recommendation and Outlook. When comparing the composition of oil contaminants from different water samples (regardless of the ultimate investigation goal) it is necessary to compare the extracts isolated under the same conditions, in other words, extracts that were in the same or very similar interaction with water.  相似文献   

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