Adsorbent regeneration

  • 文章类型: Journal Article
    由于农药的广泛应用及其对生物体的危害,迫切需要从废水中有效地去除它们。本文描述的掺入金属的碳矿物复合材料(Ni/Mn-CMC和Ni/Fe-CMC)当然可以用于此目的。它们是通过结合机械化学和热解过程合成的,并且使用多种方法研究了它们的物理化学性质(SEM-EDS,N2吸附/解吸,XRD,表面电荷,FTIR)。在自然生态系统中通常检测到的有和没有杂质的情况下,对敌草隆和羧素的吸附能力,镉离子或亚砷酸盐,是测量的。结果表明,Ni/Fe-CMC由于其表面发达,是更有效的农药吸附剂。它能够在溶液中结合158.34mgg-1的敌草隆和133.58mgg-1的羧基,那里只有一种杀虫剂。反过来,Ni/Mn-CMC样品的这些值分别为126.49mg/g和102.08mg/g,分别。应该注意的是,复合材料在多组分溶液中保持了高吸附能力,即,同时含有农药和金属离子。然后,农药吸附的最大减少仅为8.36。Ni/Mn-CMC和Ni/Fe-CMC用乙醇成功再生,而不改变其结构和吸附能力。此外,研究材料的提取物对植物生长没有负面影响。这证实了碳-矿物复合材料反复多次使用的适用性,对生物体没有毒性作用。
    Due to the extensive application of pesticides and their hazardous effects on organisms, there is an urgent need to remove them effectively from wastewater. Metal-incorporated carbon-mineral composites (Ni/Mn-CMC and Ni/Fe-CMC) described in this paper can certainly be applied for this purpose. They were synthesized by combining mechanochemical and pyrolytic processes and their physicochemical properties were investigated using numerous methods (SEM-EDS, N2 adsorption/desorption, XRD, surface charge, FTIR). Adsorption capacity towards diuron and carboxin with and without impurities commonly detected in natural ecosystems, cadmium ions or arsenite, was measured. The obtained results indicated that Ni/Fe-CMC is more efficient adsorbent of pesticides due to its well-developed surface. It was able to bind 158.34 mg g-1 of diuron and 133.58 mg g-1 of carboxin in the solutions, where only one pesticide was present. In turn, these values for the Ni/Mn-CMC sample were 126.49 mg g-1 and 102.08 mg g-1, respectively. It should be noted that the composites maintained their high adsorption capacity in the multicomponent solutions, i.e., containing both pesticide and metal ions. Then, the maximum reduction in pesticide adsorption was only 8.36. Ni/Mn-CMC and Ni/Fe-CMC were successfully regenerated with ethanol without changing their structure and adsorption capacity. Also, the extracts from investigated materials did not have negative impact on plant growth. This confirmed suitability of carbon-mineral composites for repeated multiple use without toxic effects to organisms.
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  • 文章类型: Journal Article
    层状双氢氧化物(LDH)已被证明是有效的吸附剂,但是它们用于处理水中的全氟烷基和多氟烷基物质(PFAS)的效用尚未得到充分探索。在这项研究中,9PFAS在水滑石(HT)上的吸附,一种LDH,使用具有环境相关PFAS浓度的反应溶液进行了研究。HT对单个PFAS的吸附取决于一系列因素,包括用于预处理的温度(即,煅烧)HT,老化条件,以及溶液中阴离子的存在。在400°C附近煅烧的HT最有效地吸附PFAS,但其吸附PFAS的能力对储存条件敏感。从空气中吸附CO2和水分,这可能导致CO32-重新嵌入HT的夹层区域,观察到减少PFAS吸附,并可以解释性能随时间的损失。9PFAS之间的吸附趋势以及Cl-对这一过程的影响,NO3-,SO42-,和CO32-表明吸附是通过离子交换的组合发生的,静电吸引,和疏水相互作用,尽管每种机制的相对重要性值得进一步研究。在这项研究中,我们还首次证明HT可以在400°C下热再生,而不会影响其吸附PFOS和PFBA的能力。总的来说,我们的结果表明,HT可能是PFAS治疗的有效替代方案.
    Layered double hydroxides (LDH) have been shown to be effective adsorbents, but their utility for the treatment of per- and polyfluoroalkyl substances (PFAS) in water has not been fully explored. In this study, the adsorption of 9 PFAS on hydrotalcite (HT), a type of LDH, was investigated using reaction solutions with environmentally relevant PFAS concentrations. The adsorption of individual PFAS by HT depended upon a range of factors, including the temperature used to pre-treat (i.e., calcine) the HT, aging conditions, and the presence of anions in the solution. HT calcined near 400 °C most effectively adsorbed PFAS, but its ability to adsorb PFAS was sensitive to storage conditions. The adsorption of CO2 and moisture from air, which likely resulted in the re-intercalation of CO32- into the interlayer regions of HT, was observed to reduce PFAS adsorption and may explain performance loss over time. The adsorption trend among 9 PFAS and the influence on this process by Cl-, NO3-, SO42-, and CO32- indicated that adsorption occurred via a combination of ion exchange, electrostatic attraction, and hydrophobic interactions, although the relative importance of each mechanism deserves further investigation. During this study, we also demonstrated for the first time that HT can be thermally regenerated at 400 °C without affecting its ability to adsorb PFOS and PFBA. Overall, our results suggest that HT may serve as an effective alternative for PFAS treatment.
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  • 文章类型: Journal Article
    通过羧甲基壳聚糖(CMC)和聚酰胺胺(PAMAM)交联合成了一种新型的生物质基磁性纳米粒子(Fe3O4-P-CMC/PAMAM),然后通过掺入磁性氧化铁纳米颗粒进行磷酸化。表征结果验证了吸附剂的成功官能化和结构完整性,表面积约为。43m2/g。批量吸附实验表明,在pH5.5和298.15K下,吸附剂对U(VI)的最大吸附容量为1513.47mg·g-1,Fe3O4-P-CMC/G1.5-2系列中亲和力最高。吸附动力学符合伪二级模型(R2=0.99,qe,exp=463.81mg·g-1,k2=2.15×10-2g·mg-1·min-1),表示化学驱动的过程。热力学分析表明,吸附是吸热的和自发的(ΔH°=14.71kJ·mol-1,ΔG°=-50.63kJ·mol-1,298。15K),随着在较高温度下吸附容量的增加。在存在竞争性阳离子的情况下,吸附剂对U(VI)具有显着的选择性,Fe3O4-P-CMC/G1.5-2显示出较高的选择性系数。进行的解吸和重复使用试验表明,使用1MHCl可以有效地再生吸附剂,五个循环后保持其吸附能力。XPS分析强调了膦酸酯和氨基在与铀酰离子络合中的作用,并验证了在380.1eV和390.1eV处存在属于U4f7/2和U4f5/2的双峰U4f峰。这项研究的结果强调了开发的吸附剂作为处理铀污染废水的有效和选择性材料的前景。
    A novel biomass-based magnetic nanoparticle (Fe3O4-P-CMC/PAMAM) was synthesized by crosslinking carboxymethyl chitosan (CMC) and poly(amidoamine) (PAMAM), followed by phosphorylation with the incorporation of magnetic ferric oxide nanoparticles. The characterization results verified the successful functionalization and structural integrity of the adsorbents with a surface area of ca. 43 m2/g. Batch adsorption experiments revealed that the adsorbent exhibited a maximum adsorption capacity of 1513.47 mg·g-1 for U(VI) at pH 5.5 and 298.15 K, with Fe3O4-P-CMC/G1.5-2 showing the highest affinity among the series. The adsorption kinetics adhered to a pseudo-second-order model (R2 = 0.99, qe,exp = 463.81 mg·g-1, k2 = 2.15×10-2 g·mg-1·min-1), indicating a chemically driven process. Thermodynamic analysis suggested that the adsorption was endothermic and spontaneous (ΔH° = 14.71 kJ·mol-1, ΔG° = -50.63 kJ·mol-1, 298. 15 K), with increasing adsorption capacity at higher temperatures. The adsorbent demonstrated significant selectivity for U(VI) in the presence of competing cations, with Fe3O4-P-CMC/G1.5-2 showing a high selectivity coefficient. The performed desorption and reusability tests indicated that the adsorbent could be effectively regenerated using 1M HCl, maintaining its adsorption capacity after five cycles. XPS analysis highlighted the role of phosphonate and amino groups in the complexation with uranyl ions, and validated the existence of bimodal U4f peaks at 380.1 eV and 390.1 eV belonging to U 4f7/2 and U 4f5/2. The results of this study underscore the promise of the developed adsorbent as an effective and selective material for the treatment of uranium-contaminated wastewater.
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  • 文章类型: Journal Article
    吸附过程可有效去除水中的全氟烷基和多氟烷基物质(PFAS),但是管理耗尽的吸附剂提出了显着的环境和经济挑战。常规处置方法,比如焚烧,可能会将PFAS重新引入环境。因此,先进的再生技术是必要的,以防止在处置和提高可持续性和成本效益浸出。这篇综述严格地评估了载有PFAS的吸附剂的热和化学再生方法,阐明其运作机制,水质参数的影响,以及它们固有的优势和局限性。热再生实现显著的解吸效率,达到99%的活性炭。然而,它需要大量的能量输入和风险损害吸附剂的结构完整性,导致相当大的质量损失(10-20%)。相比之下,化学再生呈现出不同再生剂的不同效率景观,包括水,酸性/碱性,盐,溶剂,和多组分解决方案。与溶剂型溶液(12.50%)相比,多组分溶液具有更高的效率(>90%),which,反过来,跑赢盐(2.34%),酸性/碱性(1.17%),和水(0.40%)再生剂。这种分层的有效性强调了化学再生的细微差别,受再生剂成分等因素的显著影响,PFAS的分子结构,以及有机共污染物的存在。探索热和化学再生方法的条件功效强调了基于特定类型的PFAS和材料特性进行战略选择的必要性。通过强调特定再生方案的局限性和潜力,并倡导未来的研究方向,例如探索过硫酸盐活化治疗,这篇综述旨在促进更有效的再生过程的发展。最终目标是通过PFAS补救工作的无害环境解决方案来确保水质和公共卫生保护。
    The adsorption process efficiently removes per- and polyfluoroalkyl substances (PFAS) from water, but managing exhausted adsorbents presents notable environmental and economic challenges. Conventional disposal methods, such as incineration, may reintroduce PFAS into the environment. Therefore, advanced regeneration techniques are imperative to prevent leaching during disposal and enhance sustainability and cost-effectiveness. This review critically evaluates thermal and chemical regeneration approaches for PFAS-laden adsorbents, elucidating their operational mechanisms, the influence of water quality parameters, and their inherent advantages and limitations. Thermal regeneration achieves notable desorption efficiencies, reaching up to 99% for activated carbon. However, it requires significant energy input and risks compromising the adsorbent\'s structural integrity, resulting in considerable mass loss (10-20%). In contrast, chemical regeneration presents a diverse efficiency landscape across different regenerants, including water, acidic/basic, salt, solvent, and multi-component solutions. Multi-component solutions demonstrate superior efficiency (>90%) compared to solvent-based solutions (12.50%), which, in turn, outperform salt (2.34%), acidic/basic (1.17%), and water (0.40%) regenerants. This hierarchical effectiveness underscores the nuanced nature of chemical regeneration, significantly influenced by factors such as regenerant composition, the molecular structure of PFAS, and the presence of organic co-contaminants. Exploring the conditional efficacy of thermal and chemical regeneration methods underscores the imperative of strategic selection based on specific types of PFAS and material properties. By emphasizing the limitations and potential of particular regeneration schemes and advocating for future research directions, such as exploring persulfate activation treatments, this review aims to catalyze the development of more effective regeneration processes. The ultimate goal is to ensure water quality and public health protection through environmentally sound solutions for PFAS remediation efforts.
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  • 文章类型: Journal Article
    全氟烷基和多氟烷基物质(PFAS)是普遍存在于环境中的人造有机化合物。由于它们的持久性和生物蓄积性,由于PFAS的法规越来越严格,将它们从环境中移除是必要的。我们的初步研究确定了全二氧化硅沸石β作为具有高选择性的替代吸附剂,亲和力,以及去除全氟辛酸(PFOA)和全氟辛烷磺酸(PFOS)的能力。这里,我们研究了PFAS链长对新材料的亲和力和容量的影响,全二氧化硅沸石β,表明*BEA沸石是去除具有8个碳的PFAS的理想吸附剂。溶液pH和向水基质中添加阳离子或天然有机物质对沸石去除PFOA/PFOS的影响最小。接下来,对负载全氟辛烷磺酸的沸石的再生进行了评估;除了热,沸石的溶剂驱动再生也是可能的,使用精心挑选的非有害溶剂的组合。最后,连续吸附实验表明,沸石可用于更大规模的应用。
    Per- and polyfluoroalkyl substances (PFAS) are man-made organic compounds ubiquitously present in the environment. Due to their persistency and bioaccumulative nature, and because of increasingly stringent regulations of PFAS, their removal from the environment is necessary. Our initial study identified all-silica zeolite β as an alternative adsorbent with a high selectivity, affinity, and capacity for perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) removal. Here, we study the influence of the PFAS chain length on the affinity and capacity of a novel material, all-silica zeolite β, showing that the *BEA zeolite is an ideal sorbent for the removal of PFAS with 8 carbons. The solution pH and the addition of cations or natural organic substances to the water matrix have minimal influence on PFOA/PFOS removal with the zeolite. Next, regeneration of a PFOS-loaded zeolite was assessed; besides thermal, solvent-driven regeneration of the zeolite is also possible, using well-selected combinations of non-noxious solvents. Lastly, continuous adsorption experiments show that zeolite can be used for larger-scale applications.
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  • 文章类型: Journal Article
    研究了热解的镰刀菌壳作为吸附剂从水溶液中去除亚甲基蓝染料分子的潜力。研究发现,在600°C的热解温度下产生的吸附剂,吸附剂质量为0.5g,颗粒直径为0.297-0.149mm,和pH值12.0,显示出最高的染料分子去除效率为82.41%。通过扫描电子显微镜观察材料的孔隙率,有利于吸附,傅里叶变换红外光谱和X射线衍射分析证实了结晶相中碳酸钙的存在。发现伪二阶模型是数据的最佳拟合,表明吸附机理包括两个步骤:外部扩散和通过固体孔的扩散。Redlich-Peterson等温线模型更好地表示了平衡数据,发现亚甲基蓝吸附是自发的,有利的,和吸热。过氧化氢与紫外线氧化被发现是最有效的再生方法,使用600mmol实现63%的再生百分比。L-1的氧化剂。结果表明,热解的镰刀菌壳可以作为生态上可行的吸附剂替代品,减少当地环境中产生的废物量,同时从水中去除污染物。在第一次吸附-氧化循环中,材料的吸附容量几乎保持不变,表明其重复使用的潜力。
    The potential of pyrolyzed Mytella falcata shells as an adsorbent for removing methylene blue dye molecules from aqueous solutions was investigated. The study found that the adsorbent produced at 600 °C of pyrolysis temperature, with an adsorbent mass of 0.5 g, particle diameter of 0.297-0.149 mm, and pH 12.0, demonstrated the highest dye molecule removal efficiency of 82.41%. The material\'s porosity was observed through scanning electron microscopy, which is favorable for adsorption, while Fourier-transform infrared spectroscopy and X-Ray diffraction analysis analyses confirmed the presence of calcium carbonate in the crystalline phases. The pseudo-second order model was found to be the best fit for the data, suggesting that the adsorption mechanism involves two steps: external diffusion and diffusion via the solid pores. The Redlich-Peterson isotherm model better represented the equilibrium data, and the methylene blue adsorption was found to be spontaneous, favorable, and endothermic. The hydrogen peroxide with UV oxidation was found to be the most efficient method of regeneration, with a regeneration percentage of 63% achieved using 600 mmol.L-1 of oxidizing agents. The results suggest that pyrolyzed Mytella falcata shells could serve as an ecologically viable adsorbent alternative, reducing the amount of waste produced in the local environment and at the same time removing pollutants from the water. The material\'s adsorption capacity remained almost constant in the first adsorption-oxidation cycles, indicating its potential for repeated use.
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  • 文章类型: Journal Article
    工业废水是自然生态系统中过量钼(Mo)的主要来源。在废水排放到环境中之前,必须从废水中去除Mo。钼酸盐离子(VI)是天然储层和工业废水中最常见的Mo形式。在这项工作中,使用氧化铝评估从水性介质中吸附去除Mo(VI)。评价了溶液的pH和温度等因素的影响。三个吸附等温线,即,朗缪尔,Freundlich和Temkin,用于描述实验结果。发现伪一级动力学模型较好地拟合了吸附过程的动力学数据,在25°C和pH4下,最大Mo(VI)吸附容量为31mg/g。热力学参数表明,Mo(VI)在Al2O3上的吸附过程是放热的和自发的。结果表明,Mo的吸附强烈取决于pH。在pH值低于7时观察到最有效的吸附。吸附剂再生实验表明,在很宽的pH值范围内,Mo(VI)可以有效地从氧化铝表面解吸到磷酸盐溶液中。Mo(VI)在磷酸盐溶液中解吸后,发现氧化铝适合重复该程序至少五次。
    Industrial wastewater is the main source of an excessive amount of molybdenum (Mo) in natural ecosystems. It is necessary to remove Mo from wastewater before it is discharged into the environment. Molybdate ion(VI) is the most common form of Mo in natural reservoirs and industrial wastewater. In this work, the sorption removal of Mo(VI) from an aqueous medium was evaluated using aluminum oxide. The influence of such factors as the pH of the solution and the temperature was evaluated. Three adsorption isotherms, namely, Langmuir, Freundlich and Temkin, were used to describe the experimental results. It was found that the pseudo-first order kinetic model better fits the kinetic data of the adsorption process, and the maximum Mo(VI) adsorption capacity was 31 mg/g at 25 °C and pH 4. The thermodynamic parameters indicated that the process of Mo(VI) adsorption on Al2O3 was exothermic and spontaneous. It was shown that the adsorption of Mo strongly depends on pH. The most effective adsorption was observed at pH values below 7. Experiments on adsorbent regeneration showed that Mo(VI) can be effectively desorbed from the aluminum oxide surface into a phosphate solution in a wide range of pH values. After the desorption of Mo(VI) in a phosphate solution, alumina was found to be suitable for repeating the procedure at least five times.
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  • 文章类型: Journal Article
    水净化过程的强制性脱碳需要活性炭的替代再生方法。基于改变解离平衡的再生,即吸附的主要影响因素,通常需要添加酸/碱,但也可能由温度摆动触发。虽然吸附和解离都是温度相关的现象,关于痕量有机化合物(TrOCs)和大温度间隔,它们的结合很少受到关注,特别是高于ΔT≥50°C。因此,我们研究了16个TrOCs在一个颗粒活性炭上的吸附平衡,温度范围从20到95〇C。大多数化合物(12/16)表现出放热的表观吸附焓,而16个中的3个表现出吸热的表观焓。范围为-46至50kJmol-1(中位数为-17kJmol-1)。讨论了吸热吸附的可能起源。引入了改变pKa从而改变TrOCs解离的基本原理,并与现有原理进行了权衡,即改变溶质溶解度,改变吸附热容量,和吸附物的饱和效应。这种知识可以允许设计解锁解离开关的变温吸附过程。因此,提高的过程效率可以为低碳排放提供基础,循环净水过程。
    Imperative decarbonization of water purification processes entails alternative regeneration methods for activated carbon. Regeneration based on changing dissociation equilibria, i.e. a major influencing factor on adsorption, usually requires the addition of acids/bases, but may also be triggered by temperature swing. Although adsorption and dissociation are both temperature-dependent phenomena, their conjunction has received little attention regarding trace organic compounds (TrOCs) and large temperature intervals, in particular above ΔT ≥ 50 ∘C. Therefore, we studied the adsorption equilibria of 16 TrOCs onto one granular activated carbon at temperatures ranging from 20 to 95 ∘C. The majority of compounds (12/16) exhibited an exothermic apparent adsorption enthalpy, while 3 out of 16 exhibited an endothermic apparent enthalpy. The range spanned from - 46 to + 50 kJ mol-1 (median at - 17 kJ mol-1). The possible origins of endothermic adsorption were discussed. A rationale of shifting pKa and thus changing dissociation of TrOCs was introduced and traded off against existing rationales, i.e. changing solute solubility, changing adsorption heat capacity, and saturation effects of the adsorbates. This knowledge may allow designing temperature swing adsorption processes that unlock the dissociation switch. The augmented process efficiency can thus provide the foundation for low-carbon emission, circular water purification processes.
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  • 文章类型: Journal Article
    随着人们对改善室内空气质量的兴趣增加,开发有效且经济地去除挥发性有机化合物(VOC)的长效吸附剂已变得至关重要。在这项研究中,将含TiO2的活性炭作为光催化吸附剂引入可再生VOC过滤器中。采用溶胶-凝胶法制备了带有TiO2颗粒的活性炭过滤器,然后是喷涂方法。使用Tedlar袋采样技术分析了含TiO2活性炭的VOC吸附和光催化活性,以甲苯和乙醛为样品的VOC气体。在紫外线C(UV-C)照射下22小时,TiO2的光催化活性使VOC过滤器再生了99%。此外,在UV-A和发光二极管下,含TiO2的活性炭过滤器再生60%和58%,分别,22小时后。该结果确立了其作为可再生室内VOC过滤器的实际适用性。
    As interest in improving indoor air quality has increased, the development of long-lasting adsorbents that effectively and economically remove volatile organic compounds (VOCs) has become critical. In this study, TiO2-bearing activated carbon is introduced as a photocatalytic adsorbent in a renewable VOC filter. The activated carbon filter bearing TiO2 particles is prepared using the sol-gel method, followed by a spraying method. VOC adsorption and photocatalytic activity of the TiO2-bearing activated carbon are analyzed using a Tedlar bag sampling technique, using toluene and acetaldehyde as sample of VOC gas. Under ultraviolet-C (UV-C) irradiation for 22 h, the photocatalytic activity of TiO2 regenerates the VOC filters by 99 %. In addition, under UV-A and light-emitting diode, the TiO2-bearing activated carbon filters are regenerated by 60 % and 58 %, respectively, after 22 h. This result establishes its practical applicability as a renewable indoor VOC filter.
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  • 文章类型: Journal Article
    通过掺入二氧化硅(Cs-Si)开发了基于壳聚糖(Cs)的复合材料,以及二氧化硅和羟基磷灰石(Cs-Si-Hap),比较测试,以从水中隔离六价(Cr(VI))离子。XRD和FT-IR数据证实了Cs-Si和Cs-Si-Hap复合材料的形成。形态学图像表现出均匀的Cs-Si表面,用SiO2纳米颗粒装饰,虽然Cs-Si-Hap表面不均匀,具有微观结构,具有SiO2和Hap纳米颗粒。热分析数据显示开发的复合材料具有出色的热稳定性。pH值的显著影响,吸附剂剂量,接触时间,温度,观察到共存阴离子对Cr(VI)在复合材料上的吸附。在pH3时,观察到Cs和发达复合材料的最大Cr(VI)吸收。Cr(VI)在Cs-Si-Hap上的吸附平衡时间为10min,相对优于Cs和Cs-Si。吸附数据拟合到拟二级动力学和Langmuir等温线模型,Cs的最大单层吸附容量(qm)分别为55.5、64.4和212.8mg/g,Cs-Si,和Cs-Si-Hap.再生研究表明,复合材料可以连续使用三个循环而不会失去其吸附潜力。
    Chitosan (Cs)-based composites were developed by incorporating silica (Cs-Si), and both silica and hydroxyapatite (Cs-Si-Hap), comparatively tested to sequester hexavalent (Cr(VI)) ions from water. XRD and FT-IR data affirmed the formation of Cs-Si and Cs-Si-Hap composite. Morphological images exhibits homogeneous Cs-Si surface, decorated with SiO2 nanoparticles, while the Cs-Si-Hap surface was non-homogeneous with microstructures, having SiO2 and Hap nanoparticles. Thermal analysis data revealed excellent thermal stability of the developed composites. Significant influence of pH, adsorbent dose, contact time, temperature, and coexisting anions on Cr(VI) adsorption onto composites was observed. Maximum Cr(VI) uptakes on Cs and developed composites were observed at pH 3. The equilibration time for Cr(VI) adsorption on Cs-Si-Hap was 10 min, comparatively better than Cs and Cs-Si. The adsorption data was fitted to pseudo-second-order kinetic and Langmuir isotherm models with respective maximum monolayer adsorption capacities (qm) of 55.5, 64.4, and 212.8 mg/g for Cs, Cs-Si, and Cs-Si-Hap. Regeneration studies showed that composites could be used for three consecutive cycles without losing their adsorption potential.
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