低温一步法活性炭基脱硫剂的制备与评价

以木屑为原料,在低温条件下一步法制得活性炭基吸附剂,考察了吸附剂制备条件和液-固、气-固吸附条件对吸附剂脱硫性能的影响。结果表明,吸附剂的最佳制备条件为,浸渍液与木屑质量比为1：1,浸渍液中硝酸质量分率为30%、吸附剂表面NiO负载量为5%,常温下浸渍24 h,400℃焙烧3 h。该吸附剂在0.2 g吸附剂/10 mL模拟油、温度为40℃及时间为5 h的液-固吸附脱硫的条件下,脱硫率为28.36%,吸附四次后饱和吸附硫容量可达2.34 mgS/g;在气-固吸附温度为250℃、空速为6.3 h^-1的条件下,饱和吸附硫容量为2.37 mgS/g;高温气-固吸附脱硫对吸附剂的影响表明,与脱硫前相比,吸附剂在比表面积、总孔体积、微孔体积均有明显提高,这说明气-固吸附脱硫过程同时实现了活性炭的扩孔活化。甲苯溶剂再生实验表明,经五次再生后吸附剂的再生性能均可达90%以上。     

Removal of methylene blue with hemicellulose/clay hybrid hydrogels

In this study, we chose corn stover hemicellulose for the preparation of hydrogels with admirable adsorption properties under mild alkaline conditions. Clay nanosheets were introduced to this system and hemicellulose/clay hybrid hydrogels were prepared. Morphological, mechanical properties and the methylene blue adsorption behaviors of the prepared hydrogels were studied. Results suggested that the addition of clay not only improved the mechanical strength of hemicellulose-based hydrogels, but also increased the adsorption capacity on methylene blue. Moreover, the adsorptions were confirmed to follow pseudo-second order equation for both gels with and without clay. The maximum adsorption capacities on methylene blue for hemicellulose-based hydrogels with or without clay reached 148.8 and 95.6 mg/g, respectively. These results implied that hemicellulose-based hydrogels could be used as promising adsorbents for the removal of methylene blue from waste water.     

Characterization and adsorption properties of diatomaceous earth modified by hydrofluoric acid etching

This work was a study of the chemical modification of diatomaceous earth (DE) using hydrofluoric acid (HF) solution. Under the experimental conditions investigated, it was found that HF under controlled conditions significantly etched inward into the interior of the existing pore structure in the clay mineral due to its high content of silica, leaving a framework possessing a larger BET surface area (ca. 10 m2 g(-1)) in comparison with that (ca. 4 m2 g(-1)) of its precursor (i.e., DE). Further, the results indicated that the HF concentration is a more determining factor in creating more open pores than other process parameters (temperature, holding time, and solid/liquid ratio). This observation was also in close agreement with the examinations by the silicon analysis, scanning electron microscopy, X-ray diffraction, and Fourier transform infrared spectroscopy. The adsorption kinetics and the adsorption isotherm of methylene blue onto the resulting clay adsorbent can be well described by a pseudo-second-order reaction model and the Freundlich model, respectively.     

掺杂铜的介孔SiO2微球的制备以及对亚甲基蓝的吸附

通过水热法在室温下合成了不同铜含量的介孔SiO2微球(Cu-MSM)。目的在于研究吸附剂量、MB的初始浓度以及吸附时间对Cu-MSM从溶液中移除亚甲基蓝(MB)吸附性能的影响。结果表明,当增加Cu-MSM的量时,MB的去除率会大大提高;掺杂铜的介孔SiO2微球可以通过吸附去除水溶液中的亚甲蓝。最后,简要探讨了亚甲基蓝的吸附机理。     

Methylene blue removal from aqueous solution by magnetic clinoptilolite/chitosan/EDTA nanocomposite

In this study, clinoptilolite as a natural zeolite which was magnetized using precipitation of maghemite nanoparticles was coated by chitosan and then modified by thylenediamine tetra-acetic acid to add functional groups and its performance in the removal of toxic methylene blue from aqueous solution was investigated. Synthesized magnetic nanocomposite was characterized by VSM, XRD, SEM, and FTIR analyses. The saturation magnetization of the final nanocomposite was obtained as 22.2 emu/g. In addition, the factors affecting adsorption process and its optimization were investigated using response surface methodology and central composite design. Data obtained by different isotherm, adsorption kinetic and thermodynamic models were also studied. The results showed good agreement of these data with the Freundlich isotherm model (R ² = 0.99), and it was found that adsorption follows the second-order kinetics model (R ² = 1). Negative values of ΔG and positive values of ΔH obtained from this adsorption thermodynamic study revealed that the methylene blue adsorption process is exothermic and spontaneous. The optimum conditions to ensure maximum adsorption efficiency were determined, and included pH = 5.54, adsorbent amount of 0.03 g, temperature of 31.18 °C, and initial solution concentration of 16.21 mg/l which resulted in a removal efficiency of 99.44%. The results indicated that this nanocomposite can be used as a proper adsorbent for adsorbing methylene blue and other dye contaminants.     

Removal of dyes from water by conducting polymeric adsorbent

Chemically synthesized conducting polyaniline (PANI) was investigated as adsorbent for its possible application in the removal of organic dyes, such as methylene blue (MB) and procion red (PR) from their aqueous solution. PANI adsorbent behaves as a charged surface upon post‐synthesis treatment of the polymer with acid and base. The adsorbent thus treated shows a high selectivity for the removal of dyes in the adsorption process. The Langmuir adsorption isotherm was used to represent the experimental adsorption data. The cationic dye, MB can be preferentially removed by the base‐treated PANI while the anionic dye, PR is predominately removed by the acid‐treated one. These observations were further evidenced from the measurements of molar conductance and pH of the dye solutions employed for adsorption. The finding can be explained considering the electrostatic nature of adsorption coupled with the morphology of the PANI surface thus treated. Copyright © 2004 John Wiley & Sons, Ltd.     

Polypyrrole-coated cotton textile as adsorbent of methylene blue dye

Pollution caused by organic dyes is of serious environmental and health concern to the population. Dyes are widely used in textile coloring applications. In the present work, cotton textile was coated with a conducting polymer, polypyrrole (PPy), in situ during the oxidative polymerization of pyrrole. The resulting materials were utilized as easily separated and recyclable adsorbent for the removal of methylene blue (MB) as a model of cationic dyes in alkaline solutions. It showed also some affinity to remove Acid Green 25 as an anionic dye in acidic medium. The adsorption was assessed by monitoring the decrease in dye concentration by UV–Visible absorption spectroscopy. The influence of various parameters such as initial dye concentration, contact time, pH, temperature, and adsorbent dose on the adsorption process was studied. The pseudo-second-order kinetic model and Freundlich isotherm model were found to describe the adsorption process. The thermodynamic study revealed that the adsorption of MB by PPy was feasible, spontaneous, and exothermic process. Investigation of the substrate regeneration revealed that PPy deposited on cotton textile can be reused for dye adsorption several times with good efficiency and it allows for the recovery of MB for recycling purposes.     

The Use of High Surface Area Mesoporous-Activated Carbon from Longan Seed Biomass for Increasing Capacity and Kinetics of Methylene Blue Adsorption from Aqueous Solution

Microporous- and mesoporous-activated carbons were produced from longan seed biomass through physical activation with CO₂ under the same activation conditions of time and temperature. The specially prepared mesoporous carbon showed the maximum porous properties with the specific surface area of 1773 m²/g and mesopore volume of 0.474 cm³/g which accounts for 44.1% of the total pore volume. These activated carbons were utilized as porous adsorbents for the removal of methylene blue (MB) from an aqueous solution and their effectiveness was evaluated for both the adsorption kinetics and capacity. The adsorption kinetic data of MB were analyzed by the pseudo-first-order model, the pseudo-second-order model, and the pore-diffusion model equations. It was found that the adsorption kinetic behavior for all carbons tested was best described by the pseudo-second-order model. The effective pore diffusivity (D_e) derived from the pore-diffusion model had the values of 4.657 × 10⁻⁷–6.014 × 10⁻⁷ cm²/s and 4.668 × 10⁻⁷–19.920 × 10⁻⁷ cm²/s for the microporous- and mesoporous-activated carbons, respectively. Three well-known adsorption models, namely the Langmuir, Freundlich and Redlich–Peterson equations were tested with the experimental MB adsorption isotherms, and the results showed that the Redlich–Peterson model provided the overall best fitting of the isotherm data. In addition, the maximum capacity for MB adsorption of 1000 mg/g was achieved with the mesoporous carbon having the largest surface area and pore volume. The initial pH of MB solution had virtually no effect on the adsorption capacity and removal efficiency of the methylene blue dye. Increasing temperature over the range from 35 to 55 °C increased the adsorption of methylene blue, presumably caused by the increase in the diffusion rate of methylene blue to the adsorption sites that could promote the interaction frequency between the adsorbent surface and the adsorbate molecules. Overall, the high surface area mesoporous carbon was superior to the microporous carbon in view of the adsorption kinetics and capacity, when both carbons were used for the removal of MB from an aqueous solution.     

Adsorption of basic dyes from aqueous solution onto pumice powder

The adsorption of methylene blue and crystal violet on pumice powder samples of varying compositions was investigated using a batch adsorption technique. The effects of various experimental parameters, such as adsorbent dosage, initial dye concentration, and contact time, were also investigated. The extent of dye removal increased with decreased initial concentration of the dye and also increased with increased contact time and amount of adsorbent used. Adsorption data were modeled using the Freundlich adsorption isotherm. The adsorption kinetic of methylene blue and crystal violet could be described by the pseudo-second-order reaction model.     

Adsorption of reactive dyes on titania-silica mesoporous materials

This paper presents a study on the adsorption of two basic dyes, methylene blue (MB) and rhodamine B (RhB), from aqueous solution onto mesoporous silica-titania materials. The effect of dye structure, adsorbent particle size, TiO(2) presence, and temperature on adsorption was investigated. Adsorption data obtained at different solution temperatures (25, 35, and 45 degrees C) revealed an irreversible adsorption that decreased with the increment of T. The presence of TiO(2) augmented the adsorption capacity (q(e)). This would be due to possible degradation of the dye molecule in contact with the TiO(2) particles in the adsorbent interior. The adsorption enthalpy was relatively high, indicating that interaction between the sorbent and the adsorbate molecules was not only physical but chemical. Both Langmuir and Freundlich isotherm equations were applied to the experimental data. The obtained parameters and correlation coefficients showed that the adsorption of the two reactive dyes (MB and RhB) on the adsorbent systems at the three work temperatures was best predicted by the Langmuir isotherm, but not in all cases. The kinetic adsorption data were processed by the application of two simplified kinetic models, first and second order, to investigate the adsorption mechanism. It was found that the adsorption kinetics of methylene blue and rhodamine B onto the mesoporous silica-titania materials surface under different operating conditions was best described by the first-order model.     

Adsorption of Ethoxylated Alkyl Phenols on Silica Gel from Aqueous Micellar Solutions

Adsorption of ethoxylated nonylphenols (Neonols) from their micellar solutions on coarse-pore KSK silica gel was studied under static conditions. The energy of adsorption interaction between micelles and silica gel surface was determined using the Hill–de Boer isotherm. For the initial parts of the isotherms (from 1 to 6 CMC₁), it was equal to –15.8kT. The study of coadsorption of Neonols with dye methylene blue showed that the micellar adsorption layer is fragmentary and that the amount of the adsorbed surfactant is dependent on the conditions of the adsorption layer formation.     

改性埃洛石材料的制备及其对亚甲基蓝吸附行为的研究

使用硅烷偶联剂KH550改性埃洛石纳米管获得改性材料HNTs-APTS,并对其吸附亚甲基蓝的行为进行研究。利用傅立叶变换红外光谱仪(FTIR)、X-衍射仪(XRD)对改性前后的埃洛石进行表征。考察了吸附时间和温度对吸附过程的影响,并采用Lagrange准二级动力学方程、Langmuir等温线方程及Freundlich等温线方程对实验数据进行拟合。结果表明,KH550成功负载到埃洛石表面;改性后材料的吸附能力大大提高。改性埃洛石对亚甲基蓝的吸附约在60 min达平衡,最大吸附容量为21.66 mg/g。其吸附过程符合准二级动力学方程,热力学较好地符合Langmuir等温线方程,且吸附过程为自发吸热,升高温度有利于吸附的进行。改性材料可重复再生6次,具有良好的再生性能,可在工业处理亚甲基蓝废水中使用。     

Removal of methylene blue dye from aqueous solution by semi‐interpenetrating polymer network hybrid hydrogel: Optimization through Taguchi method

In this study, sodium humate/poly(acrylamide‐co‐methacrylic acid)/kaolin semi‐interpenetrating polymer network hybrid hydrogel was synthesized as an effective adsorbent for the removal of methylene blue. The morphological and structural properties, and swelling behavior in distilled water and various environments of hybrid hydrogel were investigated with different analyses and tests. The equilibrium swelling percent of hybrid hydrogel reached to 37,000% in 240 min. The parameters (agitation time, concentration, dose, temperature, and pH) affecting adsorption process for methylene blue were optimized using Taguchi method. The data obtained in optimum conditions were well fitted to Langmuir adsorption isotherm and maximum adsorption capacity was determined as 833. 33 mg/g. In the light of the results, the utilization of hybrid hydrogel with high swelling capacity is foreseen as a favored adsorbent in several separation processes. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57, 1070–1078     

Review on recent advances of carbon based adsorbent for methylene blue removal from waste water

The growth in textile and printing industries proven detrimental to the aquatic environment as the industrial waste containing dye seeped into the ecosystem. A high concentration of dye in water possess negative impacts on water ecosystem and harmful to human health. Removal of methylene blue (MB) dye from industrial waste via adsorption pathway has been widely investigated that promised high efficiency of MB removal. This review will summarize researches published from 2008 to 2019 on the removal of MB using carbon adsorbent with focus will be given on the synthesis and modification of carbon-based materials, and the structural properties influencing the performance of MB adsorption. Summary on the type of material used for the synthesis of carbon materials (activated carbon and biochar) will be included from utilization of the naturally occurring carbon sources such as polymers, biomasses and biowastes, and also sucrose and hydrocarbon gases. Modification of carbon materials such as chemical activation and physical activation; surface grafting to form functionalized surfaces; deposition with metal and magnetic nanoparticles via impregnation; and manufacturing of carbon composites will be discussed on the effects to promote MB adsorption and desorption. Another type of carbon adsorbents such as porous carbon; graphitic carbons including graphite, graphene, graphene oxide, and carbon nitride (g-C₃N₄); and finally nanocarbon in the form of nanotube, nanorod and nanofiber; will be included in the review with details on the synthesis method and the correlation between structural properties and adsorption activity. The regeneration process to increase the life cycle of carbon adsorbent will also be discussed based on two regeneration pathway i.e. a thermal degradation and desorption on MB. Finally the thermodynamics, kinetics, and the adsorption models of MB on carbon adsorbent will be discussed in this review.     

Preparation of activated carbon from sawdust by zinc chloride activation

A series of activated carbons were prepared from sawdust by zinc chloride activation in different operation conditions. The effects of operation parameters such as impregnation ratio, activation temperature and time on the adsorption properties of activated carbons were measured and analyzed in order to optimize these operation conditions. The experimental results show that under the experimental circumstances studied, both the yield and the adsorption for iodine and methylene blue of activated carbon can reach a relatively higher value in the chemical activation process with the impregnation ratio of 100% ZnCl₂/sawdust in the activation temperature of 500 °C carbonized for 60–90 minutes which are the optimum activation conditions in making wood activated carbon. The most important operation parameter in chemical activation with zinc chloride was found to be the impregnation ratio.     

Conversion of Waste Tyres into Carbon Black and their Utilization as Adsorbent

Pyrolysis has the potential of transforming used tyres into useful recyclable products. Pyrolytic carbon black is one of the most important products of tyre pyrolysis. Waste tyres were pyrolysed at 450 °C in a batch reactor under atmospheric pressure. The recovered pyrolytic carbon black residues were studied to investigate their characteristics for use as a possible adsorbent. EDX elemental analysis and surface area determinations were used to investigate the distinctive features of pyrolytic carbon black. Due to various inorganic additives of the original tyre that contaminated the carbon black obtained, it was treated with acid for demineralization. The demineralized carbon black was activated at 900 °C in a furnace. It was observed that acid treatment and activation increased the surface areas and decreased the concentration of contaminants. Furthermore, adsorption characteristics of methylene blue on acid‐treated and activated carbon black (prepared via acid treatment) were compared with those of commercial activated carbon in liquid phase adsorption. It was found that adsorption capacity of methylene blue on acid‐treated activated carbon black was greater.     

KOH活化木屑生物炭制备活性炭及其表征

以木屑热裂解的生物质炭为原料,氢氧化钾为活化剂,采用化学活化法制备活性炭,探讨了碱炭比、活化温度和活化时间对活性炭吸附亚甲基蓝吸附值的影响。 利用N2吸附实验、XRD和FTIR等实验技术,对原料与制备活性炭的结构与性能进行了表征。 结果表明,在碱炭质量比为1.5、活化温度750 ℃、活化时间2 h的条件下,所制备的活性炭对亚甲基蓝吸附值为255 mg/g,BET总比表面积为1514 m2/g,中孔比表面积为110 m2/g,吸附总孔容为0.821 cm3/g,中孔孔容为0.117 cm3/g,吸附平均孔径为2.170 nm。     

Liquid-phase adsorption: Characterization and use of activated carbon prepared from diosgenin production residue

The adsorption behavior of activated carbon (AC) prepared from the residue of diosgenin by-product was characterized. The adsorption capacities of AC such as iodine, phenol and methylene blue (MB) are 933.28, 145.38 and 165 mg/g, respectively. The results of MP analysis and BJH method show AC has developed micropore and mesopore volumes, which are 0.1621 and 0.2623 cm³/g respectively, with the mean pore diameter of 1.49 nm. Comparison of the liquid phase adsorption capacities of AC to the standard activated carbon (SAC) and the commercial activated carbon (CAC) for wastewater treatment showed AC was superior to SAC and CAC. Experiments on phenol and MB adsorption and COD and chroma removal from diosgenin wastewater were carried out under different conditions of contact time, temperature, concentration, adsorbent dose and pH. The removal of COD and chroma of 10-multiple wastewater is 92.46 mg/g and 88 %, respectively. Adsorption parameters for the Langmuir and Freundlich isotherm models were determined. At lower temperatures, the data for phenol and COD fitted Freundlich model better than Langmuir model and vise versa for MB and chroma. Adsorption followed second-order kinetics. The study proves that AC prepared from the residue of diosgenin by-product can be used as adsorbent for the treatment of diosogenin wastewater as a cost-effective approach of resource recycle of Discorea zingiberensis C.H. Wright.     

Adsorption characteristics of activated carbons obtained from corncobs

Dried, crushed, corncobs were carbonized at 500°C and steam activated (in one- or two-step schemes), or activated with H₃PO₄. The products were characterized by N₂ adsorption at 77 K, using the BET, _s and DR methods. Adsorption capacity was demonstrated by the iodine and phenol numbers, and the isotherms of methylene blue and Pb²⁺ ions, from aqueous solutions. A distribution of porosity in the carbons was estimated within the various ranges (ultra-, super-, meso- and macropores). Simple carbonization yields a poor adsorbing carbon; only its uptake for iodine was high and proposed to be due to an addition reaction on residual unsaturation of the parent lignocellulosic structures. Enhanced porosity was best associated with chemical activation and/or steam pyrolysis at 700°C. These activated carbons proved highly porous and rich in mesopores, and showed high adsorption capacity for methylene blue and Pb²⁺ ions. Phenol uptake was found to depend on surface chemical nature of the carbon rather than its porous properties. Corncobs were postulated to be feasible as feedstock to produce good adsorbing carbons, under the one-step activation schemes outlined here.     

Adsorptive Removal of Methylene Blue from Aqueous Solution using a Ni-Metal Organic Framework Material

A specific metal organic framework (MOF) material was synthesized based on Ni(Ac)₂ · 4H₂O and 1-H-benzimidazole-5-carboxylic acid through hydrothermal method. It was a promising candidate as adsorbent due to its large surface areas, porous structure, ordering and controllable properties. In this paper, it was characterized by XRD, SEM, FTIR, TGA and N₂ adsorption isotherm. Meanwhile MOF was treated as adsorbent for absorption of methylene blue. Using this material to remove methylene blue, which is low cost, simple and high efficiency. It shows great potential in removing other dyes and the adsorption rate could reach 85.08%.