Modeling batch leaching behavior of arsenic and selenium from bituminous coal fly ashes

Correctly predicting the leaching potential of arsenic (As) and selenium (Se) is critical for assessing the environmental impact of coal fly ash. This study investigated the impacts of several key environmental factors, including pH, leaching time, and ash washing on the batch leaching behavior of As and Se from bituminous coal fly ashes. The experimental results demonstrated that As and Se leaching from fly ash increased beyond the minimal leaching pH ranges. Increasing leaching time increased As leaching but decreased Se leaching in the alkaline pH condition. A speciation-based adsorption model was used to quantify the batch leaching data, and determine the intrinsic leaching parameters including the total batch leachable mass and the adsorption constant of As or Se. The modeling approach was validated by correctly predicting the independent batch leaching data in a broad pH range and a different L/S condition. Experimental and modeling results also demonstrated that ash washing and ash aging (longer leaching time) did not change the adsorption constants of As and Se on the ash surface. However, ash washing could increase the availability of As and Se for leaching.     

污泥-烟煤基活性炭的制备及其对苯酚的吸附性能

以石化企业在污水处理过程中产生的干化剩余污泥为原料,大同烟煤作辅助添加料,采用化学活化法制备污泥-烟煤基活性炭,探讨了活化剂（ZnCl2）用量、活化温度、活化时间等条件对所制备的活性炭性能的影响。以活性炭的碘吸附值为衡量指标,当污泥：烟煤（质量比）=1：1时获得制备污泥-烟煤活性炭的最佳工艺条件为：浸渍液为ZnCl2：原料（质量比）=2：1,活化温度550℃,活化时间30 min,在该条件下制备的活性炭的碘吸附值为990 mg·g-1,比表面积为836 m2·g-1,产率为46.6%。同时,以苯酚为目标污染物,考察了所制备的污泥-烟煤基活性炭对苯酚的去除效果,结果表明：污泥-烟煤基活性炭投加量为2.0 g·L-1时,4 h后达到吸附平衡,离子强度对吸附容量没有显著的影响,溶液pH在4~10范围内对苯酚有较好吸附,pH=6时苯酚吸附容量为138.9 mg·g-1。与同类吸附剂相比,制备的污泥-烟煤基活性炭可高效吸附水溶液中的苯酚。     

Upgraded modified forms of bituminous coal for the removal of safranin-T dye from aqueous solution

Natural bituminous coal was used as a precursor in the synthesis of different modified products. The modification of coal was performed by treating it with nitric acid (N-coal), coating its surface by zinc oxide nanoparticles (Z-coal), and converting it into porous graphite (PG). The effect of modification processes on the structures, morphologies, and optical properties was followed by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectrum (FT-IR), and UV/VIS spectrophotometer analysis. The surface of N-coal grains becomes smoother than the surface of raw coal grains due to the removal of the associated impurities and the formation of nitrogen function groups. For Z-coal, the whole surface of coal grains appears to be completely covered by agglomerated ZnO nanoparticles of massive density and irregular shapes. The average crystallite size of the formed ZnO is ~22.2 nm and density of dislocations is 2.029 × 10^?3 dislocation/nm². Also, the removal of safranin-T dye by natural bituminous coal and its modified forms was investigated as a function of contact time, adsorbent mass, initial dye concentration, and pH value. At pH 8, the PG showed higher efficiency (96%) than Z-coal (93.5%), N-coal (74.5%), and natural coal (62%) after 2 h for 0.1 g on 100 mg/L dye. The obtained results are well fitted by pseudo-second-order kinetic than by intraparticle diffusion and Elovich kinetic models for the adsorption by N-coal, Z-coal, and PG, whereas the adsorption by raw coal is well fitted with both pseudo-second-order and Elovich kinetic models. The Langmuir isotherm model fits well the equilibrium adsorption isotherm of safranin by raw coal and its modified forms. The values of maximum adsorption capacity were calculated for raw coal, N-coal, Z-coal, and PG to be 21.3, 27.4, 32.46, and 33.67 mg/g, respectively. A monolayer model with one energy and a monolayer model with two energies as advanced equilibrium models were investigated for more physical interpretation of the adsorption process. The calculated parameters (number of adsorbed molecules per site and number of receptor sites per unit mass) reflected the role of modification processes in the adsorption behavior of safranin.

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Graphical abstract High volatile bituminous coal and its modified forms have been used for the removal of Safranin-T dye from aqueous solution.

     

An adsorption diffusion model for removal of para-chlorophenol by activated carbon derived from bituminous coal

Batch adsorption experiments were carried out to study the adsorptive removal and diffusion mechanism of para-chlorophenol (p-CP) onto Calgon Filtrasorb 400 (F400) activated carbon. The external mass transfer resistance is negligible in the adsorption process carried out under different conditions in batch operation. Intraparticle diffusion model plots were used to correlate the batch p-CP adsorption data; three distinct linear sections were obtained for every batch operation. The textural properties of F400 activated carbon showed that it has a large portion of supermicropores, which is comparable to the size of the p-CP molecules. Due to the stronger interactions between p-CP molecules and F400 micropores, p-CP molecules predominantly diffused and occupied active sites in micropore region by hopping mechanism, and eventually followed by a slow filling of mesopores and micropores. This hypothesis is proven by the excellent agreement of the intraparticle diffusion model plots and the textural properties of F400 activated carbon.     

The formation of chlorodibenzo-p-dioxins by air oxidation and chlorination of bituminous coal

A well characterized bituminous coal was subjected to high temperature air oxidation and chlorination. After an extensive cleanup procedure, the reaction products were analyzed for chlorinated dibenzo-p-dioxins by gas chromatography-mass spectrometry. Substantial quantities of chlorodibenzo-p-dioxins, some of which are known to be highly toxic, were observed with chlorination by hydrogen chloride and chlorine gas.     

药渣与煤共热解动力学模型及逸出气红外特性分析

利用TG-FTIR对红霉素药渣、烟煤及共热解过程及热解产物进行分析,研究了添加药渣对烟煤热解过程的影响。在40种固相反应机制函数中,采用Freeman-Carroll积分法推断药渣、烟煤单独热解及共热解过程的最佳反应机理函数,结果显示,药渣单独热解及共热解过程符合Avrami-Erofeev方程(n=4)模型,而烟煤的3个热解阶段分别符合反Jander方程、Avrami-Erofeev方程(n=4)、Jander方程三维扩散(n=2)模型;对共热解lnA与E分析,表明共热解过程存在动力学补偿效应。对共热解逸出气的红外分析表明:药渣单独热解及共热解过程除CO2、CO气体逸出外,还有部分醛类、酮类、羧酸类、酯类等小分子物质逸出,而烟煤单独热解气体主要成分为CO2、CO和CH4;药渣的添加使可燃气体逸出增多,有利于热解气溢出到燃烧后期燃烧室的预混燃烧,扩散混合条件大大改善。     

粉煤灰沸石负载铈掺杂TiO2对水体中蒽的去除

采用溶胶-凝胶法在80℃条件下制备了锐钛矿型稀土铈掺杂Ti02负载粉煤灰沸石光催化剂(以下简称光催化剂).利用X射线衍射(XRD)、扫描电镜(SEM)对光催化剂进行了表征,同时考察了稀土铈掺杂量、光催化剂投加量、溶液pH以及蒽初始浓度对其光降解过程的影响,并研究了蒽的光降解动力学特性.结果表明,稀土铈掺杂量为0.50％(质量分数)、pH偏碱性时蒽的光降解效果最佳.光催化反应符合Langmuir-Hinshelwood动力学模型,蒽的光降解过程符合一级反应动力学模型,反应速率常数为0.0173min-i.     

Molecular simulation and experimental studies on CO2 and N2 adsorption to bituminous coal

Environmental Science and Pollution Research - A coal fire is one of the most serious disasters in coal mining. To improve the efficiency of an inert gas for extinguishing the fire, the adsorption...     

Ca-Fe基磁性纳米复合材料对水体中磷的结晶回收

人类活动导致大量的不可再生的磷资源流失到水环境中造成水体富营养化,磷的结晶回收对废水治理、地表水管理和可持续发展具有重要意义。采用微波-冷却-回流和超声的方法制备Ca-Fe 基磁性纳米复合材料(CaCO₃-Fe₃O₄),通过批量吸附实验法系统探究了体系pH、接触时间、磷的初始浓度、共存离子等因素对复合材料去除水体中磷的影响规律。结果表明,CaCO₃-Fe₃O₄纳米磁性复合材料在pH=3.0~6.0内对磷表现出良好的去除效果,对磷的最大去除容量为189.21 mg·g⁻¹。复合材料对水体中的磷主要通过吸附-结晶耦合机制去除,在高浓度含磷废水中,磷以CaHPO₄·2H₂O的形式被回收。综合考虑磁分离的简易性、磷的去除容量和环境友好性,所制备的Ca-Fe基磁性复合材料在磷资源回收领域具有潜在的应用价值。     

A comparative study on the recovery of polycyclic aromatic hydrocarbons from fly ash and lignite coal

The recovery of polycyclic aromatic hydrocarbons (PAHs) from lignite coal burnt in Greek power stations and the fly ash produced is examined comparatively using Soxhlet, ultrasonic and accelerated solvent extraction procedures with various organic solvents. Soxhlet using toluene/methanol mixture and accelerated solvent extraction/toluene were found to be the most efficient methods for fly ash PAHs, yielding average recoveries of about 80%. The accelerated solvent extraction/toluene procedure was superior for lignite PAHs, yielding 96% average recovery, whereas ultrasonic and Soxhlet extraction yielded relatively lower recoveries (75% and 67%, respectively).     

利用电渗析浓缩飞灰水洗液并回收工业盐

为回收飞灰中含有的大量可溶性盐,并利于飞灰后续填埋、水泥窑协同处置或建材利用,采用不同的液固比水洗飞灰并利用循环式电渗析装置浓缩飞灰水洗液,依据Na⁺、K⁺//Cl⁻—H₂O 三元水盐体系相图通过蒸发结晶回收浓缩液中的盐。结果表明,以4 L·kg⁻¹的液固比二级水洗飞灰后,可将飞灰中的可溶性氯质量分数降到《生活垃圾焚烧飞灰污染控制技术规范(试行)》(HJ 1134-2020)规定的限值之下。将飞灰一级水洗液加入电渗析装置的淡液室和浓液室,对比淡液室∶浓液室=2∶1 (V/V) 1次电渗析浓缩和淡液室∶浓液室=1∶1 (V/V) 2次电渗析浓缩2种工况可知,后者的浓缩倍数和淡液回用率(2.28倍、62%)比前者（2.03倍、54%）略高,但后者能耗是前者的1.37倍。因此,1次电渗析更适合用于飞灰水洗液的浓缩提盐。提高飞灰水洗液中盐质量浓度,可以提高电渗析浓缩速率。浓缩液蒸发结晶可得到纯度为92.2%的工业氯化钾和融雪剂,并可将飞灰中洗出的68%的钾回收为工业氯化钾。本研究结果可为电渗析浓缩飞灰水洗液并回收盐的工业应用提供参考。     

Removal of PAHs from water using an immature coal (leonardite)

It has been studied an immature coal (leonardite) as an adsorbent for removing PAHs [fluorene, pyrene, benzo(k)fluoranthene, benzo(a)pyrene and benzo(g,h,i)perylene] from water. To determine the efficiency of leonardite as an adsorbent of PAHs, factors such as pH, contact time and equilibrium sorption were evaluated in a series of batch experiments. There were no significant differences in the removal percentages for the various pH values studied, except for fluorene. The adsorption of fluorene was higher at lower pH values. The equilibrium time was reached at 24h. At this time, more than 82% of the pyrene, benzo(k)fluoranthene, benzo(a)pyrene and benzo(g,h,i)perylene had been removed. During the first 2h, the adsorption rate increased rapidly. After that time, however, there was a minor decrease. Equilibrium data were fitted to Freundlich models to determine the water-leonardite partitioning coefficient. Physical adsorption caused by the aromatic nature of the compounds was the main mechanism that governed the removal process. The polarity of the humic substances in leonardite may also have influenced the adsorption capacity.     

气水比对污泥水中以鸟粪石形式回收氮磷的影响

污泥水富含氮磷,其回流经常造成污水处理厂出水水质的不稳定。以模拟污泥水为对象,采用套筒式流化床结晶装置,通过曝气吹脱CO2提高pH值并添加镁盐的方式以促进污泥水中鸟粪石的结晶,研究气水比对模拟污泥水中氮磷的去除效果以及对晶体产物的产量、分布、形态、粒径和成分的影响。结果表明,随着气水比的增加,污泥水的出水碱度降低、pH值升高、PO43--P和氨氮的去除率均增加,当气水比为15:1、30:1、60:1时,PO43--P的平均去除率分别为73%、82%和87%,氨氮的去除率均在17%~23%之间。同时,气水比影响晶体产物的产量、粒径和分布,但对晶体形态和组成的影响较小。同一气水比条件下,反应器底部和内壁晶体的形态存在明显差异,其中底部晶体大多纤细碎小,内壁晶体则均呈硕大的楔形,但X衍射谱图分析表明,以上二者的主成分均为鸟粪石。     

Fate of disinfection by-products in groundwater during aquifer storage and recovery with reclaimed water

Knowledge on the behaviour of disinfection by-products (DBPs) during aquifer storage and recovery (ASR) is limited even though this can be an important consideration where recovered waters are used for potable purposes. A reclaimed water ASR trial in an anoxic aquifer in South Australia has provided some of the first quantitative information at field-scale on the fate and transport of trihalomethanes (THMs) and haloacetic acids (HAAs). The results revealed that THM half-lives varied from <1 to 65 days, with persistence of chloroform being highest and bromoform lowest. HAA attenuation was rapid (<1 day). Rates of THM attenuation were shown to be highly dependent on the geochemical environment as evidenced by the 2-5 fold reduction in half-lives at the ASR well which became methanogenic during the storage phase of the trial, as compared to an observation well situated 4 m away, which remained nitrate-reducing. These findings agree with previous laboratory-based studies which also show persistence declining with increased bromination of THMs and reducing redox conditions. Modelling suggests that the chlorinated injectant has sufficient residual chlorine and natural organic matter for substantial increases in THMs to occur within the aquifer, however this is masked in some of the field observations due to concurrent attenuation, particularly for the more rapidly attenuated brominated compounds. The model is based on data taken from water distribution systems and may not be representative for ASR since bromide and ammonia concentrations in the injected water and the possible role of organic carbon in the aquifer were not taken into consideration. During the storage phase DBP formation potentials were reduced as a result of the removal of precursor material despite an increase in the THM formation potential per unit weight of total organic carbon. This suggests that water quality improvements with respect to THMs and HAAs can be achieved through ASR in anoxic aquifers.     

Fate of disinfection by-products in groundwater during aquifer storage and recovery with reclaimed water

Knowledge on the behaviour of disinfection by-products (DBPs) during aquifer storage and recovery (ASR) is limited even though this can be an important consideration where recovered waters are used for potable purposes. A reclaimed water ASR trial in an anoxic aquifer in South Australia has provided some of the first quantitative information at field-scale on the fate and transport of trihalomethanes (THMs) and haloacetic acids (HAAs). The results revealed that THM half-lives varied from <1 to 65 days, with persistence of chloroform being highest and bromoform lowest. HAA attenuation was rapid (<1 day). Rates of THM attenuation were shown to be highly dependent on the geochemical environment as evidenced by the 2-5 fold reduction in half-lives at the ASR well which became methanogenic during the storage phase of the trial, as compared to an observation well situated 4 m away, which remained nitrate-reducing. These findings agree with previous laboratory-based studies which also show persistence declining with increased bromination of THMs and reducing redox conditions. Modelling suggests that the chlorinated injectant has sufficient residual chlorine and natural organic matter for substantial increases in THMs to occur within the aquifer, however this is masked in some of the field observations due to concurrent attenuation, particularly for the more rapidly attenuated brominated compounds. The model is based on data taken from water distribution systems and may not be representative for ASR since bromide and ammonia concentrations in the injected water and the possible role of organic carbon in the aquifer were not taken into consideration. During the storage phase DBP formation potentials were reduced as a result of the removal of precursor material despite an increase in the THM formation potential per unit weight of total organic carbon. This suggests that water quality improvements with respect to THMs and HAAs can be achieved through ASR in anoxic aquifers.     

Adsorptive reduction of water hardness by a highly porous and regenerative geopolymer fabricated from coal fly ash waste with low-temperature calcination

Environmental Science and Pollution Research - In this research paper, potassium-activated geopolymer cubes (GeoC) fabricated from waste coal fly ash with low-temperature calcination were...     

沸石/水合氧化锆吸附水中的磷

以粉煤灰为原料,采用传统水热方法制备的沸石除磷性能有限,且存在废碱液排放的问题。对此,本文首次提出了在传统水热方法基础上用氯氧化锆中和合成沸石过程中产生的废碱液,得到沸石/水合氧化锆复合吸附剂（简称锆沸石）的改进方法。锆沸石的比表面积为1.931×105 m2·kg-1,是沸石的近7倍。锆沸石的XRD衍射峰数量和位置与沸石相同,证明锆沸石中的水合氧化锆为无定形。锆沸石对磷的Langmuir最大吸附量为22.62 mg·g-1。吸附动力学实验结果表明,锆沸石对磷的吸附速率呈先快后慢的趋势。锆沸石对磷的吸附随pH上升而减少。水中常见的阴离子Cl-、NO3-不会对其除磷效果产生明显影响,而HCO32-会通过提高溶液pH值明显降低吸附量。因此,以粉煤灰为原料,采用改进的合成方法制备锆沸石可获得除磷效果大幅提高的新型吸附剂。     

Using polymer solutions to enhance recovery of mobile coal tar and creosote DNAPLs

Direct pumping and enhanced recovery of coal tar and creosote dense, non-aqueous phase liquids (DNAPLs) from the subsurface have had mixed results because these DNAPLs are viscous fluids that can potentially alter aquifer wettability. To improve the inefficiencies associated with waterflooding, the research presented here considered the use of a polymer solution that can be added to the injected flood solution to increase the viscosity and decrease the velocity of the flooding solution. Results from one-dimensional, vertically oriented laboratory column experiments that evaluate the recovery of coal-derived DNAPL with both water and polymer flooding solutions are presented. The final DNAPL saturation remaining in the column was assessed in water and oil-wet systems for three viscous DNAPLs. Adding polymer to increase the aqueous solution viscosity did not have a significant impact in water-wet systems. A final DNAPL saturation of approximately 19% was achieved for both water and polymer floods. In contrast, the addition of polymer significantly improved recovery in oil-wet systems. The final saturation was over 40% in oil-wet systems after waterflooding, but approximately 19% with a polymer flushing solution. Although the final saturation produced with polymer flooding was similar between the oil- and water-wet systems, differences in the relative permeability and distribution of DNAPL in the porous matrix caused the DNAPL recovery to be much slower in the oil-wet system.     

Presence and fate of coliphages and enteric viruses in three wastewater treatment plants effluents and activated sludge from Tunisia

Purpose

The role of water in the transmission of infectious diseases is well defined; it may act as a reservoir of different types of pathogens. Enteric viruses can survive and persist for a long time in water, maintaining infectivity in many instances. This suggests the need to include virus detection in the evaluation of the microbiological quality of waters.

Methods

In this study, enteric viruses (enteroviruses and hepatitis A virus (HAV)) were investigated by RT-PCR and coliphages (known as indicators of viral contamination) were enumerated with the double-layer technique agar in effluents and sewage sludge from three Tunisian wastewater treatment plants.

Results and discussion

The molecular detection of enteric viruses revealed 7.7% of positive activated sludge samples for enteroviruses. None of the samples was positive for HAV. Molecular virus detection threshold was estimated to be 10³?PFU/100?ml. All samples contained high concentrations of coliphages except those of dry sludge. Reductions in the concentrations of bacteriophages attained by the wastewater treatment plants are of the order of magnitude as reductions described elsewhere. Peak concentrations in raw wastewater were associated with winter rains and suspended materials rate in analysed samples. Our data which is the first in North Africa showed that similar trends of coliphages distribution to other studies in other countries.

Conclusion

No clear correlation between studied enteric viruses and coliphages concentration was proved. Coliphages abundance in collected samples should raise concerns about human enteric viruses transmission as these residues are reused in agricultural fields.