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1.
The sorption of ionizable benzotriazole (BTA) to corncob biochars pyrolyzed at different temperature (i.e., 300 oC, 500 oC and 800 oC) was investigated in this study. Biochars produced at higher temperature showed higher surface area, micropore volume and aromaticity. Consequently, the sorption of BTA changed from absorption to adsorption for biochars pyrolyzed at 300 oC and 800 oC, respectively. Solution pH affected speciation of BTA and surface charge properties of biochars. For BTA0, H-bond, partition and micropore filling are dominant sorption mechanisms. For BTA-, it is suggested that negative charge-assisted H-bond plays an important role in sorption. Corncob biochar pyrolyzed at high temperature (e.g., 800 oC) showed the highest sorption affinity for BTA. Ca2+ in solution enhanced BTA- and BTA0 sorption through cation-bridge and surface complexation.  相似文献   

2.
Batch kinetics and isotherm studies were carried out to evaluate the sorption of phenol by pyrolyzed and activated Jordanian oil-shale. The effects of contact time, initial sorbate concentration, sorbent concentration, temperature, pH and inorganic salts (NaCl and KCl), on the adsorption process by different sorbents were considered. Chemically activated oil shale, pretreated with ZnCl 2, gave the highest uptake of phenol. The isotherm experimental data fit well to Freundlich and Redlich-Paterson models and to a less extent to the Langmuir model. The increase in the initial sorbate concentration resulted in an increase in the uptake. Three kinetics models, namely the Morris-Weber model, the Lagergren model, and the pseudo-second-order model (PSOM), were applied to represent the experimental results for pyrolyzed and ZnCl 2-oil shale sorbents. Pyrolyzed oil shale was prepared using a fluidized bed reactor at 520 °C in the presence of nitrogen. Physical activation was carried out by treating the resulted pyrolyzed oil shale with CO 2 at 830 °C, while chemical activation of oil shale was carried out using KOH and ZnCl 2 as impregnating agents.  相似文献   

3.
Thermally carbonization biochar produced from a traditional Chinese herbal medicine waste (Astragalus mongholicus residue) was investigated for its performance in ciprofloxacin adsorption. Batch sorption experiments were conducted, and scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and Brunauer–Emmett–Teller surface area analyses were employed to characterize the biochar. The results demonstrated that thermal activation process improves the adsorbent characteristics. Biochar produced at 800 °C had the best adsorption capacity, a better pore structure and the largest surface areas. The adsorption process fit well to a pseudo-second-order kinetics model. The adsorption isothermal model results revealed that the adsorption process of ciprofloxacin is described better by the Freundlich isotherm and the type of adsorption is a chemical process. The maximum adsorption of ciprofloxacin occurred at pH 7. The present research demonstrated that A. mongholicus biochar might be an attractive and cost-effective adsorbent with good adsorption performance for removing ciprofloxacin from water solution.  相似文献   

4.
Aquifer thermal energy storage in urban and industrial areas can lead to an increase in subsurface temperature to 70 °C and more. Besides its impacts on mineral and sorption equilibria and chemical reaction kinetics in an aquifer, temperature sensitively influences microbial activity and thus redox processes, such as sulphate reduction. Microorganism species can only operate within limited temperature ranges and their adaptability to temperature is a crucial point for the assessment of the environmental consequences of subsurface heat storage. Column experiments with aquifer sediment and tap water at 10, 25, 40, and 70 °C showed that under the constant addition of acetate sulphate reduction could be initiated after 26–63 pore volumes exchanged at all temperatures. Fastest initiation of sulphate reduction with the highest reduction rates was found at 40 °C. Maximum rate constants during experimental run-time were 0.56 h?1 at 40 °C and 0.33, 0.36, and 0.25 h?1 at 10 and, 25, and 70 °C, respectively. Hence, microbial activity was enhanced by a temperature increase to 40 °C but was significantly lowered at 70 °C. At 25 °C methane was found in solution, indicating the presence of fermenting organisms; at 10, 40, and 70 °C no methane production was observed. It could be shown that redox processes in an aquifer generally can adapt to temperatures significantly higher than in situ temperature and that the efficiency of the reduction process can be enhanced by temperature increase to a certain limit. Enhancement of sulphate reduction in an aquifer due to temperature increase could also allow enhanced degradation of organic ground water contaminants such as BTEX, where sulphate is an important electron acceptor.  相似文献   

5.
Because of their physicochemical properties, biochars can be used as sorption materials for removal of toxic substances. The purpose of the present study was to determine whether biochar obtained from cones of larch (Larix decidua Mill. subsp. decidua) and spruce (Picea abies L. H. Karst) could be used as a sorbent for Cd2+, Pb2+ and Co2+ in aqueous solutions. So far, this feedstock had not been tested in this respect. The material was subjected to pyrolysis at 500 and 600 °C for the duration of 5, 10 and 15 min. The obtained pyrolysates were found to differ in terms of pH and the contents of the essential macroelements. The different values of these parameters were determined for varying temperature, duration of the pyrolysis process and type of feedstock. Sorption capacities of the biochars for removal of Cd2+, Pb2+ and Co2+ were examined using simulated contamination of aqueous solutions with salts of these metals. The findings showed the highest, nearly complete, removal for Pb2+ were maximum 99.7%, and almost three times lower value for Cd2+ and Co2+ (respectively, 35.7 and 24.8%). It was demonstrated that pyrolysis of conifer cones produced optimum sorption capacities when the process was conducted at a temperature of 500 °C for the duration of 5 min. It was shown that products of spruce cone pyrolysis were characterized by better sorption capacity in comparison with products of larch cone pyrolysis. The properties of conifer cone biochar create the possibility of using it as an adsorbent in water and wastewater treatment as well as in production of filters and activated carbon.  相似文献   

6.
This study describes the development of scallop shell synthesized ceramic biomaterial for phosphorus removal from water. The synthesized biomaterial was characterized by scanning electron microscope, Brunauer–Emmett–Teller and X-ray diffractometer methods. The influences of contact time, initial phosphate concentration, initial solution pH, co-existing ions and temperature for phosphorus removal were investigated by batch experiments. The results indicated that the equilibrium data can be fitted by the Langmuir isotherm model at temperatures ranging from 15 to 55 °C, with the maximum sorption capacity of 13.6 mg/g. Sorption kinetics followed a pseudo-second-order kinetic equation model. The sorption process was optimal at a wide range of solution pH (above 2.4), with a relatively high sorption capacity level. Phosphorus sorption was slightly impeded by the presence of F?, HCO3 ? and NH4 + ions, and significantly inhibited by Cl?, SO4 2? and NO3 ? ions. Sorption process appeared to be controlled by a chemical precipitation processes. The mechanism may be attributed to ion complexation during subsequent sorption of phosphorus on scallop shell synthesized ceramic biomaterial.  相似文献   

7.
The subsurface migration of methyl tertiary butyl ether (MTBE) and benzene towards a drinking-water production site in Belgium was monitored for 9 years. A large gasoline spill at a nearby fuel station had caused a 500-m long and 50-m-wide pollution plume of MTBE (10?30 mg/L) and benzene (2?10 mg/L). In order to prevent any intrusion of pollutants into the drinking-water supply, a conceptual model was used to design a pump-and-treat system that intercepted the gasoline-contaminated groundwater emanating from the spill. The contaminated soil in the spill zone was excavated. A numerical mass transport model was developed to evaluate the ongoing plume containment. The model describes the subsurface MTBE migration and was regularly updated, based on groundwater monitoring data and the measured mass of MTBE extracted with the pump-and-treat system. With continued interception pumping, the MTBE plume can be remediated in 14 years. Without it, MTBE and benzene concentrations up to 600 μg/L could have reached the drinking-water production site and the plume would persist for 9 years longer. Source zone treatment combined with plume interception pumping is a suitable risk-based remediation strategy for the containment of MTBE and benzene groundwater pollution.  相似文献   

8.
Impacts of subsurface heat storage on aquifer hydrogeochemistry   总被引:3,自引:3,他引:0  
The use of shallow aquifers for subsurface heat storage in terms of energy management and building climatisation can lead to a temperature rise in the aquifer to 70 °C and above. The influence of temperature changes on individual mineral and sorption equilibria, reaction kinetics and microbial activity is largely known. However, the impact of heating to temperatures as high as 70 °C on the aquifer overall system has not been quantified yet. Temperature-related changes in sediment ion exchange behaviour, dimension and rates of mineral dissolution and precipitation as well as microbially enhanced redox processes were studied in column experiments using aquifer sediment and tap water at 10, 25, 40, and 70 °C. At 70 °C, a change in sediment sorption behaviour for cations and organic acids was postulated based on temporal changes in pH, magnesium, and potassium concentration in the experimental solution. No clear changes of pH, TIC and major cations were found at 10–40 °C. Redox zoning shifted from oxic conditions towards nitrate and iron(III) reducing conditions at 25 and 40 °C and sulphate reducing conditions at 70 °C. This was attributed to (a) a temperature-related increase in microbial reduction activity, and (b) three times higher release of organic carbon from the sediment at 70 °C compared to the lower temperatures. The findings of this study predict that a temperature increase in the subsurface up to 25 °C and above can impair the usability of ground water as drinking and process water, by reducing metal oxides and thus possibly releasing heavy metals from the sediment. Generally, at 70 °C, where clear cation and organic carbon desorption processes were observed and sulphate reducing conditions could be achieved, a site-specific assessment of temperature effects is required, especially for long-term operations of subsurface heat storage facilities.  相似文献   

9.
Atomic layer deposition (ALD) thin film coating was applied to improve the hydrophilia of biochar derived from black willow. 2 (2Al, 0.82 wt% Al2O3), 5 (5Al, 1.40 wt% Al2O3), and 10 (10Al, 2.36 wt% Al2O3) cycles of alumina ALD were applied. The biochars were characterized by inductively coupled plasma–atomic emission spectroscopy, nitrogen adsorption and desorption, scanning electron microscopy, and Fourier transform infrared spectroscopy. The adsorbents were utilized for the removal of methylene blue (MB) from an aqueous solution to evaluate their adsorption capacities. The 5Al biochar showed the highest adsorption capacity, compared to the uncoated biochar and other Al2O3 coated biochars, due to its improved hydrophilia. The amount of MB adsorbed onto the 5Al biochar was almost three times that adsorbed onto the uncoated biochar during the first hour of adsorption experiments. Adsorption isotherms were modeled with the Langmuir and Freundlich isotherms. The data fit well with the Langmuir isotherm, and the maximum adsorption capacities were found to be 26.8 and 35.0 mg/g at 25 °C for the uncoated biochar and 5Al biochar, respectively. The adsorbed MB amount per square meter achieved 1.3 mg/m2 onto the 5Al biochar, and it was twice the amount on the uncoated biochar. The experimental data were analyzed by pseudo-first-order and pseudo-second-order kinetics models of adsorption. The pseudo-second-order model better describes adsorption kinetic data for the uncoated biochar and 5Al biochar than the pseudo-first-order model does.  相似文献   

10.
Qatar economy has been growing rapidly during the last two decades during which waste generation and greenhouse gas emissions increased exponentially making them among the main environmental challenges facing the country. Production of biochar from municipal solid organic wastes (SOWs) for soil application may offer a sustainable waste management strategy while improving crop productivity and sequestering carbon. This study was conducted to (1) investigate the physicochemical parameters of biochars for SOW, (2) select the best-performing biochars for soil fertility, and (3) evaluate the potential benefits of these biochars in lowering greenhouse gases (GHGs) during soil incubation. Biochars were produced from SOW at pyrolysis temperatures of 300–750 °C and residence times of 2–6 h. Biochars were characterized before use in soil incubation to select the best-performing treatment and evaluation of potential GHG-lowering effect using CO2 emission as proxy. Here, soil–biochar mixtures (0–2%w/w) were incubated in greenhouse settings for 120 days at 10% soil moisture. Soil properties, such as pH, EC, TC, and WHC, were significantly improved after soil amendment with biochar. Two biochars produced from mixed materials at 300–500 °C for 2 h and used at 0.5–1% application rate performed the best in enhancing soil fertility parameters. A significant decrease in CO2 emission was observed in vials with soil–biochar mixtures, especially for biochars produced at 500 °C compared the corresponding raw materials which exhibited an exponential increase in the CO2 emission. Hence, application of biochar to agricultural soils could be beneficial for simultaneously improving soil fertility/crop productivity while sequestering carbon, thereby reducing anthropogenic emissions of GHGs.  相似文献   

11.
Retention behaviour of natural clayey materials at different temperatures   总被引:2,自引:1,他引:1  
The water retention capacity of geomaterials, and especially clayey soils, is sensitive to temperature changes as the physical mechanisms of retention, such as capillarity or adsorption, are affected by it. It is therefore a major issue to be able to define temperature-dependent behaviour of materials, especially for geo-energy and geo-environmental applications involving non-isothermal conditions. This paper presents results of experiments conducted on two representative materials: a hard clay (Opalinus clay) and a plastic clay (Boom clay), both of which have been considered as buffer materials for underground radioactive waste disposal, in Switzerland and Belgium, respectively. Two new devices were developed for this purpose to permit the analysis of water retention behaviour at different temperatures. The behaviour of these two materials at ambient (20 °C) and high temperature (80 °C) was observed and described through the evolution of the degree of saturation, the water content and the void ratio with respect to suction. It appears that the retention capability of the clays reduces significantly with an increase in temperature; on the other hand, the change in temperature had less of an effect on the total volume variation.  相似文献   

12.
It has been widely accepted in scientific communities that water confined in porous materials gradually freezes from large pores to small pores at subfreezing temperatures (< 0 °C), though we still describe a soil as frozen or unfrozen in engineering practice and daily life. Therefore, it is more accurate to say “how frozen” instead of “whether frozen.” This gradual freezing process is temperature-dependent because water in pores of different sizes has different energy levels, which requires different temperatures for its phase transition, leading to a relationship between unfrozen water content and temperature in soils. However, the understanding of this relationship, i.e., the Phase Composition Curves (PCC), is still incomplete, especially in the low-temperature range. We still lack answers to even the most fundamental questions for frozen soils and their PCCs: (1) How much pore water could be frozen? (2) How do capillarity and adsorption control the freezing of pore water? This study investigates two basic physical mechanisms, i.e., unfreezable threshold and adsorption, for their dominant roles in the low-temperature range of the PCC. To quantify the effects of the unfreezable threshold, molecular dynamics simulation was employed to identify the unfreezable threshold of cylindrical pores. The simulation results, for the first time, revealed that the unfreezable threshold corresponds to a pore diameter of 2.3 ± 0.1 nm and is independent of the wettability of the solid substrates. Combining this unfreezable threshold with a modified Gibbs–Thomson equation, a mathematical model was proposed to predict the melting temperature in pores of different sizes, which considers both unfreezable threshold and adsorption. Comparisons of the results calculated with the new model and other two conventional equations against experimental results indicated that the model can improve conventional equations which have been used for centuries by including the two mechanisms, which significantly improved our understanding of frozen soils.  相似文献   

13.
《Applied Geochemistry》2002,17(5):649-656
Adsorption of Mo on to hydrous TiO2 (anatase) particles was investigated. Batch experiments were conducted at 19 and 90 °C over a pH range of 2 to 12 and Mo concentrations ranging from approximately 10−6 to 10−4 M. The extent of sorption was strongly dependent on pH and surface loading. Maximum sorption was observed in the acidic pH range at low surface loading. Adsorption behavior was described using the empirical Langmuir adsorption model. A constant capacitance surface complexation model was also used to fit the adsorption isotherms using a ligand exchange reaction for a hydroxyl surface site on anatase. Comparison of experimental data at two different temperatures (19 and 90 °C) indicates that Mo sorption in the acidic pH range decreases with increasing temperature.  相似文献   

14.
The carbon molecular sieves (CMSs) prepared by carbonaceous materials as precursors are effective in CO2/N2 separation. However, selectivity of these materials is too low, since hydrocarbon cracking for developing the desired microporosity in carbonaceous materials has not been done effectively. Hence, in this study, cobalt and nickel impregnation on the precursor was conducted to introduce catalysts for hydrocarbon cracking. Cobalt and nickel impregnation, carbonization under N2 atmosphere, and chemical vapor deposition (CVD) by benzene were conducted on the extruded mixtures of activated carbon and coal tar pitch under different conditions to prepare CMSs. The best CMS prepared by carbon deposition on the cobalt-impregnated samples exhibited CO2 adsorption capacity of 54.79 mg/g and uptake ratio of 28.9 at 0 °C and 1 bar. In terms of CO2 adsorption capacity and uptake ratio, CMSs prepared by carbon deposition on non-impregnated and cobalt-impregnated samples presented the best results, respectively. As benzene concentration and CVD time increased, equilibrium adsorption capacity of CO2 decreased, and uptake ratio increased. Cobalt was found to be the best catalyst for benzene cracking in the CVD process.  相似文献   

15.
Aquifer thermal energy storage may result in increases in the groundwater temperature up to 70 °C and more. This may lead to geochemical and microbiological alterations in the aquifer. To study the temperature effects on the indigenous microbial community composition, sediment column experiments at four different temperatures were carried out and the effluents were characterized geochemically and microbiologically. After an equilibrium phase at groundwater temperature of 10 °C for 136 days, one column was kept at 10 °C as a reference and the others were heated to 25, 40 and 70 °C. Genetic fingerprinting and quantitative PCR revealed a change in the bacterial community composition and abundance due to the temperature increase. While at 25 °C only slight changes in geochemical composition and gene copy numbers for bacteria were observed, increasing concentrations of total organic carbon in the 40 °C column were followed by a strong increase in bacterial abundance. Thermophilic bacteria became dominant at 70 °C. Temporary sulfate reduction took place at 40 and 70 °C and this correlated with an increased abundance of sulfate-reducing bacteria (SRB). Furthermore, a coexistence of SRB and sulfur-oxidizing bacteria (SOB) at all temperatures indicated an interaction of these physiological groups in the sediments. The results show that increased temperatures led to significant shifts in the microbial community composition due to the altered availability of electron donors and acceptors. The interplay of SRB and SOB in sedimentary biofilms facilitated closed sulfur cycling and diminished harmful sulfur species.  相似文献   

16.
In the present research, coal fly ash, a waste by-product of thermal power plant, has been segregated to obtain hollow and spherical cenospheres which combined with activated carbon in different ratio for effectual remediation of wastewater. Fabricated cenospheres activated carbon (CNAC) composites were characterized by ATR-FTIR, SEM, XRD, BET and CILAS for functionality, surface modification, crystallinity, surface area, pore volume, pore size and particle size analysis, respectively. Batch adsorption has been applied to appraised maximum removal of Disperse Orange 25 (DO) and Disperse Blue 79:1 (DB) dyes at varying solution pH 2 to 12, adsorbent dose 0.1 g cenospheres + 0.1 g AC to 1.0 g cenospheres + 1.0 g AC, dye concentration 10 to 100 mg/L, agitation speed 80 to 240 rpm and contact time 5 to 300 min at three different temperatures (25, 35 and 45 °C). The maximum percentage removal was found to be 79 and 76% for DO and DB dyes, respectively, at optimized condition. Langmuir isotherm showed good interaction with adsorption data, and the obtained maximum equilibrium adsorption capacity was found to be 90.91 mg/g for DO and 83.33 mg/g for DB at 45 °C. Eventually, the negative ?G° (? 7.513 for DO and ? 7.767 for DB) has suggested the feasibility of dyes adsorption on CNAC composites.  相似文献   

17.
The use of renewable energy can be enhanced by utilising groundwater reservoirs for heating and cooling purposes. The urbanisation effect on the peak heating and peak cooling capacity of groundwater in a cold groundwater region was investigated. Groundwater temperatures were measured and energy potentials calculated from three partly urbanised aquifers situated between the latitudes of 60° 25′N and 60° 59′N in Finland. The average groundwater temperature below the zone of seasonal temperature fluctuations was 3–4 °C higher in the city centres than in the rural areas. The study demonstrated that due to warmer groundwater, approximately 50–60 % more peak heating power could be utilized from populated areas compared with rural areas. In contrast, approximately 40–50 % less peak cooling power could be utilised. Urbanisation significantly increases the possibility of utilising local heat energy from groundwater within a wider region of naturally cold groundwater. Despite the warming in urban areas, groundwater still remains attractive as a source of cooling energy. More research is needed in order to determine the long-term energy capacity of groundwater, i.e. the design power, in urbanised areas of cold regions.  相似文献   

18.
Arsenic in groundwater is a serious environmental problem. The contamination of groundwater with arsenic has been of utmost concern worldwide. Steel slag is a solid waste generated from steel production. Although steel slags have been used for arsenic removal from water, this process has not been systematically or integratively researched. In this study, the arsenic removal capacity and mechanism were investigated for carbon steel slag, stainless steel slag and Fe-modified stainless steel slag based on an in-depth study. The study also evaluated the potential utilization of different steel slag for regeneration. The maximum adsorption of arsenic on carbon steel slag, stainless steel slag and Fe-modified stainless steel slag was 12.20, 3.17 and 12.82 mg g?1 at 25 °C, respectively. The modification of stainless steel slag by FeC13 can generate more pore structures and larger surface areas, and 300 °C treatment produces the best regeneration efficiency. The ΔG values were negative for all of the steel slags, indicating the spontaneous nature of the adsorption process. The solution pH was a critical parameter for the removal of arsenic for steel slags. Under highly alkaline solution conditions, the mechanism of arsenic removal by carbon steel slag and stainless steel slag can be attributed to chemisorption, including chemical precipitation and coordination reactions, and under weakly alkaline solution conditions, electrostatic interaction and specific adsorption are the arsenic removal mechanisms by Fe-modified stainless steel slag. Regeneration of the Fe-modified stainless steel slag was better achieved than that of the other steel slags in the application of high-temperature treatment.  相似文献   

19.
An activated carbon-impregnated cellulose filter was fabricated, and the capacity to remove dust and volatile organic compounds was evaluated in a laboratory. The adsorption capacities for benzene, toluene, ethyl benzene and m-xylene gases were compared by an adsorption isotherm test conducted as a preliminary test, showing that m-xylene and benzene were the most and least favorable for adsorption onto activated carbon, respectively. Cellulose filters were made with four levels of activated carbon contents, and dust removal was performed with all of the filters showing 99 % and higher efficiencies stable with a small variation during the experiment. Activated carbon content of 5 g in the unit filter area (125 g/m2) was found optimum for benzene, toluene, ethylbenzene and m-xylene removal, as it appeared that higher than 5 g activated carbon content was unnecessary for the improvement of its capacity. With increasing benzene, toluene, ethylbenzene and m-xylene loading, the highest removal rates were determined as 0.33–0.37 mg/cm2 s for as short as 0.0046 s of air filter residence time. The rapid removal was possible because of the high surface area of the activated carbon-impregnated cellulose filter provided by powdered activated carbon, which is distinguished from the granular form in conventional activated carbon towers. As fixed within a cellulose scaffolding structure, the powdered activated carbon performed excellent benzene, toluene, ethylbenzene, and m-xylene adsorption (98.9–100 %), and at the same time, particular matters were removed in average 99.7 % efficiency after being filtered through the cellulose filter sheet.  相似文献   

20.
Open burning of waste at dumpsites sites may alter many physical and chemical properties of underlining soil layers including its ability to retard the migration of potential contaminants, such as lead, through the vadose zone. In this study, lead sorption onto soil samples from Irbid that were subjected to high temperatures has been investigated. These samples were collected from ground surface and heated to temperatures of 25, 70, 100, 200, 225, 250, 275, 300, 400, and 550°C. Based on these temperatures the soil was divided into ten different groups. Each group was first characterized by conducting a set of experiments to estimate the Atterberg limits (liquid limit, plastic limit, and plasticity index), the organic carbon content, and a set of batch experiments to study lead adsorption. Results indicate that the LL, PL, total organic carbon are slightly affected by high temperatures less than 200°C, show an abrupt change between temperature from 200 and 300°C, and then slight change above 300°C. Sorption of lead onto heated samples, however, was not significantly changed. This may be explained by the fact that adsorption of heavy metals mainly occurs onto the soil mineral parts which are slightly affected by the temperature range used in this study.  相似文献   

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