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1.
Column experiments were conducted for examining the effectiveness of the cationic hydrogel on Cr(VI) removal from groundwater and soil. For in-situ groundwater remediation, the effects of background anions, humic acid (HA) and pH were studied. Cr(VI) has a higher preference for being adsorbed onto the cationic hydrogel than sulphate, bicarbonate ions and HA. However, the adsorbed HA reduced the Cr(VI) removal capacity of the cationic hydrogel, especially after regeneration of the adsorbents, probably due to the blockage of adsorption sites. The Cr(VI) removal was slightly influenced by the groundwater pH that could be attributed to Cr(VI) speciation. The 6-cycle regeneration and reusability study shows that the effectiveness of the cationic hydrogel remained almost unchanged. On average, 93% of the adsorbed Cr(VI) was recovered in each cycle and concentrated Cr(VI) solution was obtained after regeneration. For in-situ soil remediation, the flushing water pH had an insignificant effect on the release of Cr(VI) from the soils. Multiple-pulse flushing increased the removal of Cr(VI) from the soils. In contrast, more flushing water and longer operation may be required to achieve the same removal level by continuous flushing.  相似文献   

2.
Mak MS  Lo IM 《Chemosphere》2011,84(2):234-240
This study investigated the removal kinetics and mechanisms of Cr(VI) and As(V) by Fe(0) in the presence of fulvic acid (FA) and humic acid (HA) by means of batch experiments. The focus was on the involvements of FA and HA in redox reactions, metal complexation, and iron corrosion product aggregation in the removal of Cr(VI) and As(V) removal by Fe(0). Synthetic groundwater was used as the background electrolyte to simulate typical groundwater. The results showed faster Cr(VI) removal in the presence of HA compared to FA. Fluorescence spectroscopy revealed that no redox reaction occurred in the FA and HA. The results of the speciation modeling indicate that the free Fe(II) concentration was higher in the presence of HA, resulting in a higher removal rate of Cr(VI). However, the removal of As(V) was inhibited in the HA solution. Speciation modeling showed that the concentration of dissolved metal-natural organic matter (metal-NOM) complexes significantly affected the aggregation of the iron corrosion products which in turn affected the removal of As(V). The aggregation was found to be induced by gel-bridging of metal-NOM with the iron corrosion products. The effects of metal-NOM on the aggregation of the iron corrosion products were further confirmed by TEM studies. Larger sizes of iron corrosion products were formed in the FA solution compared to HA solution. This study can shed light on understanding the relationships between the properties of NOM (especially the content of metal-binding sites) and the removal of Cr(VI) and As(V) by Fe(0).  相似文献   

3.
Yang JK  Lee SM 《Chemosphere》2006,63(10):1677-1684
The removal efficiencies of Cr(VI) and HA, using a TiO(2)-mediated photocatalytic process, were investigated with variations in the pH, TiO(2) dosage and Cr(VI)/HA ratio. During the photocatalytic reaction, the total removal of Cr(VI) occurred through adsorption onto TiO(2), as well as its reduction to Cr(III). However, oxidation and adsorption were identified as important removal processes for the treatment of HA. Due to the anionic type adsorption onto TiO(2) and its acid-catalyzed photocatalytic reduction, the removal of Cr(VI) decreased with increasing pH, while that of HA increased with increasing pH. The TiO(2) dosage was also an important parameter for the removal of Cr(VI). As the TiO(2) dosage was increased to 2.5 g l(-1), the removal of Cr(VI) was continuously enhanced, but decreased at dosages above 3 g l(-1) due to the increased blockage of the incident UV light used for the photocatalytic reaction. The removal of Cr(VI) was greatly enhanced when the system contained both HA and Cr(VI) compared to Cr(VI) alone. Also, the removal of HA was greatly enhanced when the system contained both HA and Cr(VI) compared to HA alone. The removal of Cr(VI) was continuously enhanced as the HA concentration gradually increased; however, no further increase was observed above 20 mg l(-1) HA due to the increased absorption of the UV light. This result supports that the photocatalytic reaction, with illuminated TiO(2), could be applied to more effectively treat wastewater containing both Cr(VI) and HA than that containing a single species only.  相似文献   

4.
The combination of zero-valent iron (Fe0) and iron oxide-coated sand (IOCS) was used to remove Cr(VI) and As(V) from groundwater in this study. The efficiency and the removal mechanism of Cr(VI) and As(V) by using this combination, with the influence of humic acid (HA), were investigated using batch experiments. Results showed that, compared to using Fe0 or IOCS alone, the Fe0-IOCS can perform better on the removal of both Cr(VI) and As(V). Metal extraction studies showed that As(V) was mainly removed by IOCS and iron corrosion products while Cr(VI) was mainly removed by Fe0 and its corrosion products. Competition was found between Cr(VI) and As(V) for the adsorption sites on the iron corrosion products. HA had shown insignificant effects on Cr(VI) removal but some effects on As(V) removal kinetics. As(V) was adsorbed on IOCS at the earlier stage, but adsorbed/coprecipitated with the iron corrosion products at the later stage.  相似文献   

5.
The humic acid (HA) fraction of a food and vegetable residues compost (CM) was taken as indicator to trace the fate of CM organic matter in four years CM amended soil. (1)H and (13)C NMR spectroscopy were used to investigate the nature of the HA isolates from CM, control soil (S(4)) and amended soil. The result indicated a significant structural difference between CM HA and S(4) HA, and supported the presence of both HA fractions in soil at the end of the amendment trials. However, the nature and content of CM HA in soil did not fully explain the increase of soil cation exchange capacity (CEC) after amendment. All CM humic fractions (i.e., fulvic acid, humic acid and humin) were found to contribute to the change of the soil organic matter composition. It is concluded that although CM HA is a suitable indicator of the survival of compost organic matter in soil during amendment, all three humic fractions should be monitored and analyzed to fully understand changes in the composition and properties of amended soil.  相似文献   

6.
Sachs S  Bernhard G 《Chemosphere》2008,72(10):1441-1447
An artificial humic substance-kaolinite-associate (HSKA) was synthesized as a model substance for natural clays containing organic matter in clay formations, soils, and sediments. The U(VI) sorption onto this model substance was studied in batch experiments as a function of pH and compared to the U(VI) sorption onto kaolinite in absence and presence of separately added humic acid (HA). The HSKA has a TOC content of 4.9 mg g(-1). It was found that the humic matter associated with kaolinite exhibits an immobilizing as well as an mobilizing effect on U(VI). Between pH 3 and 5, humic matter causes an increase of the U(VI) sorption onto kaolinite, whereas at pH above 5 the release of humic matter from the associate into the solution and the formation of dissolved uranyl humate complexes reduces the U(VI) sorption. The U(VI) sorption onto the synthetic HSKA differs from that of U(VI) in the system U(VI)/HA/kaolinite with comparable amounts of separately added HA. Separately added HA causes a stronger mobilizing effect on U(VI) than humic matter present in HSKA. This can be attributed to structural and functional dissimilarities of the humic substances.  相似文献   

7.
Soil organic matter (SOM) is generally believed not to influence the sorption of glyphosate in soil. To get a closer look on the dynamics between glyphosate and SOM, we used three approaches: I. Sorption studies with seven purified soil humic fractions showed that these could sorb glyphosate and that the aromatic content, possibly phenolic groups, seems to aid the sorption. II. Sorption studies with six whole soils and with SOM removed showed that several soil parameters including SOM are responsible for the strong sorption of glyphosate in soils. III. After an 80 day fate experiment, ∼40% of the added glyphosate was associated with the humic and fulvic acid fractions in the sandy soils, while this was the case for only ∼10% of the added glyphosate in the clayey soils. Glyphosate sorbed to humic substances in the natural soils seemed to be easier desorbed than glyphosate sorbed to amorphous Fe/Al-oxides.  相似文献   

8.
岳佳妮  肖峰  李一鸣 《环境工程学报》2023,17(10):3333-3341
为了解不同有机物对含藻水体混凝过程的影响,以含铜绿微囊藻水体作为实验对象,考察牛血清蛋白(BSA)和腐殖酸(HA)2种有机物及其质量浓度对含藻水体浊度、藻类有机物的去除效果以及絮体形成、破碎、再絮凝的影响。结果表明,少量的BSA对混凝反应起促进作用,当BSA的投加量超过1 mg·L−1转为抑制作用,因为投加量升高时,BSA抢占混凝剂活性位点,抑制混凝反应。HA不利于混凝反应的进行,因为HA中的官能团优先与混凝剂结合,从而导致混凝效果变差。提高混凝药剂投加量可缓解有机物质量浓度增加对混凝效果的影响。当BSA投加量为5 mg·L−1,PACl投加量为0.06 mmol·L−1时,能达到出水浊度小于1 NTU,藻细胞去除率大于90 %的混凝效果,HA添加量为5 mg·L−1,PACl投加量为0.12 mmol·L−1时,也能达到相同的混凝效果。混凝更容易去除分子质量较大的BSA和HA,而对小分子亲水性有机物的去处效果较差,如藻类有机物或HA中小分子有机物。少量的BSA和HA增加了混凝絮体的生成速率和初始粒径。本研究结果可为天然水体混凝除藻工艺优化运行提供参考。  相似文献   

9.
Adani F  Ricca G  Tambone F  Genevini P 《Chemosphere》2006,65(8):1300-1307
Humic acid consists of a recalcitrant (unhydrolysed fraction) (the core) and labile (hydrolysable fraction) fraction. Core-humic acid (core-HA) isolation was performed by treating source material with apolar and polar solvents (organic solvents+acid hydrolysis) before alkaline extraction. Leonardite, soil Ah horizont and dry blood were chosen for this study because of their different origin and degree of humification. Chemical analysis (elemental analysis, total acidity, E(4):E(6)), spectroscopic analysis (DRIFT and (1)H NMR), and complete mass balance were used to investigate the effect of purifying humic acids. The results obtained showed that purification produced a slight modification of Leonardite humic acids as was expected for these highly humified organic matrices. On the other hand, about 500 g kg(-1) of soil humic acids were lost by purification. The fractions lost mainly consisted of carbohydrates. Dry blood showed the presence of humic acids that contrasted with its origin, thus indicating the limitations of the common analytical methods used for HA extraction. Nevertheless, in practice, purification caused the complete disappearance (914 g kg(-1) of HA was lost) of these HAs. The results obtained in this work suggest that the HA fraction isolated (named core-HA) effectively represents the HA structure proposed by the existing literature, since the purification proposed was able to eliminate the adsorbed organic molecules (interference materials) coating the HA structure.  相似文献   

10.
Zhang T  Wu YX  Huang XF  Liu JM  Xia B  Zhang WH  Qiu RL 《Chemosphere》2012,88(6):730-735
Soil washing is one of the few permanent treatment alternatives for removing metal contaminants. Ethylenediaminetetraacetic acid and its salts (EDTA) is very effective at removing cationic metals and has been utilized globally. However it is ineffective for anionic metal contaminants or metals bound to soil organic matter. The simultaneous removal of cationic and anionic metal contaminants by soil washing is difficult due to differences in their properties. The present study evaluated the potential of a washing process using two synthesized EDTA-derivatives, C6HEDTA (2,2′-((2-((carboxymethyl)(2-(hexanoyloxy)ethyl)amino)ethyl)azanediyl)diacetic acid) and C12HEDTA (2,2′-((2-((carboxymethyl) (2-(dodecanoyloxy)ethyl)amino)ethyl)azanediyl)diacetic acid), which consist of a hydrophilic polycarboxylic moiety and a hydrophobic moiety with a monoalkyl ester group. A series of equilibrium batch experiments at room temperature were conducted to investigate the efficacy of C6HEDTA and C12HEDTA as extractants for both oxyanion Cr(VI) and cationic Cu(II). Results showed that either C6HEDTA or C12HEDTA can extract both Cr(VI) and Cu(II) from humic acid simultaneously. However, C6HEDTA was less effective for Cr(VI) probably because it has no surface activities to increase solubility of humic acid, like C12HEDTA. Extraction of Cr(VI) was mainly attributed to the decreased surface tension and enhanced solubility of organic matter. Extraction of Cu(II) was attributed to both the Cu(II) chelation and enhanced solubility of humic acid. It was demonstrated that the hydrophilic polycarboxylic moiety of C12HEDTA chelates cations while the monoalkyl ester group produces surface active properties that enhance the solubility of humic acid.  相似文献   

11.
程爱华  郑蕾 《环境工程学报》2018,12(10):2892-2898
以活性污泥与生物铁作为修复剂,对比时间、pH、污泥投加量、Cr(VI)初始浓度对活性污泥、生物铁去除土壤中Cr(VI)的影响;考察生物铁对土壤中Cr(VI)的还原率;采用SEM、XRD、XPS对生物铁修复前后的Cr(VI)污染土壤进行表征分析。实验结果表明:在土壤中,生物铁对Cr(VI)的修复效果优于活性污泥,当pH为6.0,Cr(VI)初始浓度为300 mg·kg-1,生物铁和活性污泥的投加量均为19.57 mg·g-1,修复时间为45 d时,土壤中Cr(VI)经活性污泥与生物铁修复后浓度分别为31.42、19.69 mg·kg-1,去除率分别为89.52%、94.12%。生物铁修复土壤Cr(VI)以还原作用为主,吸附为辅。Cr(VI)污染土壤被生物铁修复后出现了FeOOH、Fe3O4以及Fe3O4与FeCr2O4的混合物,部分Cr(VI)被还原为Cr(III),铁被氧化为Fe2+、Fe3+。  相似文献   

12.
Park D  Yun YS  Park JM 《Chemosphere》2005,60(10):1356-1364
The biomass of the brown seaweed, Ecklonia sp., is capable of reducing Cr(VI) to Cr(III). However, very little is known about the mechanism of Cr(VI) reduction by the biomass. The aims of the present investigation were to enhance the Cr(VI)-reducing capacity of the biomass using various chemical treatments and to elucidate the mechanisms governing Cr(VI) reduction. Among the various chemical treatments, acid-treatment showed the best performance with regards the improvement of Cr(VI) removal from the aqueous phase, while organic solvent-treatment significantly improved the removal efficiency of total Cr in the equilibrium state. Based on FTIR study, the biomass was subjected to chemical modification of its amino and carboxyl groups, to examine their roles in the Cr(VI) removal from the aqueous phase. Methylation of the amino group significantly decreased the Cr(VI) removal rate, but amination of the carboxyl group significantly increased the Cr(VI) removal rate. Meanwhile, esterification of the carboxyl group and carboxylation of the amino group decreased the Cr(VI) removal rate, but the former showed a more negative effect than the latter. These findings indicated that the amino and carboxyl groups take part in the Cr(VI) removal from the aqueous phase. In conclusion, mechanisms for direct and indirect Cr(VI) removal are proposed, and some aspects for the application of this biomass to Cr(VI) detoxification are discussed.  相似文献   

13.
为了增加混凝出水中Cr(VI)的去除率,使用铁表面改性的石英砂进行了不同条件下的Cr(VI)吸附实验,实验结果表明,在实验pH值(2.0~13.0) 范围内,表面附着的铁具有较高的稳定性。铁表面改性后石英砂的等电点向碱性范围内移动,有助于吸附去除带负电的Cr(VI)。随着吸附时间的增加,改性石英砂对Cr(VI)的去除能力逐渐提高。Cr(VI)的浓度逐渐减少,改性石英砂对Cr(VI)的吸附动力下降,110 min后,吸附基本达到平衡。腐殖酸对于Cr(VI)在改性滤料表面吸附的影响主要体现在与Cr(VI)的竞争吸附和对Cr(VI)的还原作用。随着Cr(VI)浓度的增加,Cr(VI)的去除率呈现先增大后降低的趋势,当Cr(VI)浓度为2.0 mg/L时去除率达到最高。未改性的石英砂对于混凝沉后水中的剩余Cr(VI)无明显的去除作用。当使用改性砂柱对AS混凝出水进行过滤时,30 min之内Cr(VI)的去除率仍然能够达到接近100%。当体系中无腐殖酸存在, Al30做混凝剂时,Cr(VI)在较短的时间(20 min)通过滤柱。  相似文献   

14.
为揭示Tessier连续提取法应用于土壤总铬(TCr)和六价铬[Cr(Ⅵ)]结合态分析的适用性,通过液相和土壤相实验,分别研究了提取液自身还原性组分及土壤残留还原剂在各个提取步骤中导致的Cr(Ⅵ)-Cr(Ⅲ)转化问题。结果表明,提取液中还原性组分会在铁锰氧化物结合态和有机结合态的检测中导致Cr(Ⅵ)被还原为Cr(Ⅲ),可还原的Cr(Ⅵ)最大量分别为50.88和0.54 mg;经还原修复后的铬污染土壤中残留还原剂会在可交换态和碳酸盐结合态的检测中导致Cr(Ⅵ)的还原。提取过程中Cr(Ⅵ)-Cr(Ⅲ)的转化限制了Tessier连续提取法在铬污染土壤中的应用。当用于了解铬污染土壤TCr、Cr(Ⅵ)结合态的分布时,Cr(Ⅵ)铁锰氧化物结合态和有机结合态检测结果均显著低于真实值,TCr结合态的检测结果重现性较差。当用于评价修复后土壤中Cr(Ⅵ)结合态变化时,可交换态、碳酸盐结合态、铁锰氧化物结合态和有机结合态的检测结果均可能显著低于真实值。研究可为利用Tessier连续提取法准确评估铬污染土壤修复效果提供参考。  相似文献   

15.
Zhang W  Zhuang L  Tong L  Lo IM  Qiu R 《Chemosphere》2012,86(8):809-816
Cr(VI) was often reported to oxidize soil organic matter at acidic environments due to its high ORP, probably thus changing cationic metal species bound to soil organic matter, and influencing their electro-migration patterns. However, such an effect on the electro-migration was not confirmed in most previous studies. Therefore, this study applied a fixed voltage direct current field on an aged electroplating contaminated clayed soil, with a special interest in the direct or indirect influence of Cr(VI) on the electro-migration of other coexisting metals. After 353 h electrokinetic process, 81% of Zn, 53% of Ni and 22% of Cu in the original soil were electro-migrated into the electrolyte, and most of the remaining concentrated near the cathode. The Cr(VI) oxidized some soil organic matter along its migration pathway, with a pronounced reaction occurred near the anode at low pHs. The resulting Cr(III) reversed its original movement, and migrated towards the cathode, leading to the occurrence of a second Cr concentration peak in the soil. Metal species analyses showed that the amount of metals bound to soil organic matter significantly decreased, while a substantial increase in the Cr species bound to Fe/Mn (hydro-)oxides was observed, suggesting an enhancement of cationic metal electro-migration by the reduction of Cr(VI) into Cr(III). However, the Cr(VI) may form some stable lead chromate precipitates, and in turn demobilize Pb in the soil, as the results showed a low Pb removal and an increase in its acid-extractable and residual fractions after electrokinetic remediation.  相似文献   

16.
Murphy V  Hughes H  McLoughlin P 《Chemosphere》2008,70(6):1128-1134
Dried biomass of the macroalgae Fucus vesiculosus and Fucus spiralis (brown), Ulva spp. (comprising Ulva linza, Ulva compressa and Ulva intestinalis) and Ulva lactuca (green), Palmaria palmata and Polysiphonia lanosa (red) were studied in terms of their chromium biosorption performance. Metal sorption was highly pH dependent with maximum Cr(III) and Cr(VI) sorption occurring at pH 4.5 and pH 2, respectively. Extended equilibrium times were required for Cr(VI) binding over Cr(III) binding (180 and 120min, respectively) thus indicating possible disparities in binding mechanism between chromium oxidation states. The red seaweed P. palmata revealed the highest removal efficiency for both Cr(III) and Cr(VI) at low initial concentrations. However, at high initial metal concentrations F. vesiculosus had the greatest removal efficiency for Cr(III) and performed almost identically to P. lanosa in terms of Cr(VI) removal. The Langmuir Isotherm mathematically described chromium binding to the seaweeds where F. vesiculosus had the largest q(max) for Cr(III) sorption (1.21mmol g(-1)) and P. lanosa had the largest Cr(VI) uptake (0.88mmol g(-1)). P. palmata had the highest affinity for both Cr(III) and Cr(VI) binding with b values of 4.94mM(-1) and 8.64mM(-1), respectively. Fourier transform infrared analysis revealed interactions of amino, carboxyl, sulphonate and hydroxyl groups in chromium binding to Ulva spp. The remaining seaweeds showed involvement of these groups to varying degrees as well as ether group participation in the brown seaweeds and for Cr(VI) binding to the red seaweeds.  相似文献   

17.
18.
Ke L  Wong TW  Wong AH  Wong YS  Tam NF 《Chemosphere》2003,52(9):1581-1591
Vegetated (with Kandelia candel seedlings) and non-vegetated mangrove microcosms were employed to remove pyrene from contaminated sediments, and the effects of adding 6.7% humic acid (HA) on such removal were investigated. At the end of 6-month treatment, residual pyrene concentrations in surface sediments (0-2 cm) of the contaminated microcosms reduced from an initial 5.82 to 0.63 microg g(-1) dw, and the reduction was less in HA amended microcosms with the residual pyrene concentration remained at 3.12 microg g(-1) dw. The pyrene removal percentages in microcosms with HA amendment were 29% for surface aerobic sediments and 41% for bottom (anaerobic) sediments, while the respective removal percentages in microcosms without HA amendment were 89% (surface sediments) and 53% (bottom sediments). Microcosms planted with K. candel seedlings had a significantly higher pyrene removal when compared to the non-vegetated ones, and the average removal percentages were 70.9% and 61.4%, respectively. However, when humic acid was added, no significant difference was found between vegetated and non-vegetated microcosms in pyrene removal, both had less than 40% removal, probably because plant growth in humic acid amended contaminated microcosms, in terms of total biomass, was reduced by 50%. Roots of K. candel could accumulate pyrene from contaminated microcosms, and pyrene concentrations in roots harvested from microcosms with and without humic acid addition were 6.01 and 3.46 microg g(-1) dw, respectively. These results suggest that the addition of HA to contaminated sediments decreased the mangrove microcosm's ability to remove pyrene as pyrene was more tightly bound to the organic matter and plant growth was reduced.  相似文献   

19.
A novel process, enhanced direct injection-well recharge system (EnDir), can overcome the technical difficulties during the application of conventional surface spreading and has been developed to recharge groundwater with reclaimed water. In this study, removal and transformation of dissolved organic matter (DOM) in the system were investigated in laboratory-scale experiments. Results demonstrated that dissolved organic carbon and trihalomethane formation potential values could be reduced from 6.54 +/- 1.30 mg/L and 267.9 +/- 24.3 microg/L to 1.59 +/- 0.64 mg/L and 104.5 +/- 10.2 microg/L, respectively, as a result of DOM biodegradation in the aerobic short-term vadose soil treatment. Fluorescence spectra showed that aromatic protein-like substances and soluble microbial byproducts could be removed, to a great extent, in the soil system. Despite different removal efficiencies of DOM in different molecular weight fractions, the residual DOM was composed mainly of fulvic acid-like and humic acid-like substances, with molecular weights of 500 Da to 1 kDa.  相似文献   

20.
Polycyclic aromatic hydrocarbons (PAHs) are one of the main classes of contaminants in the terrestrial environment. Aside from total organic carbon, the ratio among the different organic matter fractions [dissolved organic matter, fulvic acid (FA), humic acid (HA) and humin] can also affect the mobility of these hydrocarbons in soils. In this study the effect of the whole organic carbon pool has been compared with that of HA and FA on the translocation of four PAHs (biphenyl, fluorene, phenanthrene and pyrene) in soil columns. Oxidized and untreated soil columns with and without HA or FA, were prepared, spilled with hydrocarbons and leached with a 0.01 M CaCl2 solution. The influence of HA and FA on PAH translocation was investigated through determinations of the PAH contents and total organic carbon (TOC) in the layers of the columns. All molecules were moved vertically by the percolating solutions, their concentrations decreasing with depths. The nonoxidized soil tended to retain more PAHs (96%) than the oxidized one (60%), confirming that organic matter plays an important role in controlling PAH leaching. The whole organic matter pool reduced the translocation of pollutants downward the profile. The addition of HA enhanced this behaviour by increasing the PAH retention in the top layers (7.55 mg and 4.00 mg in the top two layers, respectively) while FA increased their mobility (only 2.30 and 2.90 mg of PAHs were found in the top layers) and favoured leaching. In fact, in the presence of HA alone, the higher amounts of PAHs retained at the surface and the good correlation (r2=0.936) between TOC and hydrocarbon distribution can be attributed to a parallel distribution of PAHs and HA, while in the presence of FA, the higher mobility of PAHs can be attributed to the high mobility of the humic material, as expected by its extensive hydrophilic characteristics.  相似文献   

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