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Recyclable aminophenylboronic acid modified bacterial cellulose microspheres for tetracycline removal: Kinetic, equilibrium and adsorption performance studies for hoggery sewer
2022
Zhang, Gengrong | Li, Linhan | Zhou, Guoqing | Lin, Zhiyang | Wang, Jun | Wang, Gaoxue | Ling, Fei | Liu, Tianqiang
Significant concerns have been raised regarding to the pollution of antibiotics in recent years due to the abuse of antibiotics and their high detection rate in water. Herein, a novel super adsorbent, boronic acid-modified bacterial cellulose microspheres with a size of 415 μm in diameter was prepared through a facile water-in-oil emulsion method. The adsorbent was characterized by atomic force microscopy, scanning electron microscopy, and fourier transform infrared spectroscopy analyses to confirm its properties. The microspheres were applied as packing materials for the adsorption of tetracycline (TC) from an aqueous solution and hoggery sewer via the reversible covalent interaction between cis-diol groups in TC molecules and the boronic acid ligand. TC adsorption performance had been systemically investigated under various conditions, including the pH, temperature, TC concentration, contact time, and ionic strength. Results showed that the adsorption met pseudo-second-order, Elovich kinetic model and Sips, Redlich-Peterson isothermal models. And the adsorption process was spontaneous and endothermic, with the maximum TC adsorption capacity of 614.2 mg/g. After 18 adsorption-desorption cycles, the adsorption capacity remained as high as 84.5% compared with their original adsorption capacity. Compared with other reported adsorption materials, the microspheres had high adsorption capacity, a simple preparation process, and excellent recovery performance, demonstrating great potential in application on TC removal for water purification and providing new insights into the antibiotic's adsorption behavior of bacterial cellulose-based microspheres.
Show more [+] Less [-]Low-temperature aerobic carbonization and activation of cellulosic materials for Pb2+ removal in water source
2022
Ai, Shuo | Qin, Yue | Hong, Yuxiang | Liu, Linghui | Yu, Wanguo
Targeting the removal of Pb²⁺ in wastewater, cellulosic materials were carbonized in an aerobic environment and activated via ion exchange. The maximum adsorption capacity reached 243.5 mg/g on an MCC-derived adsorbent activated with sodium acetate. The modified porous properties improved the adsorption capacity. The capacity could be completely recovered five times through elution with EDTA. Because of the negative effects of Ni, Mg, and Ca elements, the adsorption capacities of activated carbonized natural materials were lower than that of pure cellulose. N₂ adsorption measurement showed that the adsorbent had a large specific surface area as well as abundant micropores and 4-nm-sized mesopores. FTIR and surface potential results proved that carboxyl group was generated in the aerobic carbonization, and was deprotonated during ion exchange. This adsorbent consisted of C–C bonds as the building blocks and hydrophilic groups on the surface. XPS results demonstrated that the Pb 4f binding energies were reduced by 0.7–0.8 eV due to the interaction between Pb²⁺ and the activated adsorbent, indicating that the carboxylate groups bonded with Pb²⁺ through coordination interactions. Pseudo-second-order and Elovich kinetic models were well fitted with the adsorption processes on the pristine and activated carbonized adsorbents, indicative of chemisorption on heterogeneous surfaces. The Freundlich expression agreed well with the data measured, and the pristine and activated adsorbents had weak and strong affinities for Pb²⁺, respectively. The Pb²⁺ adsorption process was exothermic and spontaneous, and heat release determined the spontaneity. The adsorption capacity is attributed to the carboxylate groups and pores generated in the aerobic oxidation and ion exchange procedures.
Show more [+] Less [-]Polyethylenimine-grafted nitrogen-doping magnetic biochar for efficient Cr(VI) decontamination: Insights into synthesis and adsorption mechanisms
2022
Qu, Jianhua | Zhang, Xiubo | Bi, Fuxuan | Wang, Siqi | Zhang, Xinmiao | Tao, Yue | Wang, Yifan | Zhao, Jiang | Zhang, Ying
Herein, polyethylenimine (PEI)-grafted nitrogen (N)-doping magnetic biochar (PEIMW@MNBCBM) was synthesized, and characterization results showed that the microwave-assisted PEI grafting and ball milling-assisted N doping introduced abundant amino, pyridine N and pyrrole N structures onto biochar, which possessed high affinity to Cr(VI) in the anion form. The as-prepared PEIMW@MNBCBM displayed pH-dependence adsorption performance and high tolerance to co-existing ions with maximum uptake capacity of Cr(VI) identified as 183.02 mg/g. Furthermore, PEIMW@MNBCBM could bind Cr(VI) through electrostatic attraction, complexion, precipitation, reduction and pore filling. Especially, effective reduction of Cr(VI) was ascribed to cooperative electron transfer of partial oxygen-containing functional groups, intramolecular pyridine/pyrrole N, protonated amino and Fe²⁺ on the adsorbent, while oxygen-containing and amino functional groups from N-doping biochar and PEI synergistically complexed Cr(III) via providing lone pair electrons to form coordinate bonds. Furthermore, the stable precipitation was formed between Fe³⁺ and Cr(III). Additionally, the Cr(VI) elimination efficiency could maintain 95.83% even after four adsorption-desorption cycles, suggesting PEIMW@MNBCBM as a high-performance adsorbent for Cr(VI) contaminated water remediation.
Show more [+] Less [-]Biochar composite derived from cellulase hydrolysis apple branch for quinolone antibiotics enhanced removal: Precursor pyrolysis performance, functional group introduction and adsorption mechanisms
2022
Zou, Mengyuan | Tian, Weijun | Chu, Meile | Gao, Huizi | Zhang, Dantong
In this study, magnetic biochar (MAB) and humic acid (HA)-coated magnetic biochar produced from apple branches without and after cellulase hydrolysis (HMAB and CHMAB, respectively) were prepared and tested as adsorbents of enrofloxacin (ENR) and moxifloxacin (MFX) in aqueous solution. Compared with MAB and HMAB, novel adsorbent CHMAB possessed a superior mesoporous structure, greater graphitization degree and abundant functional groups. When antibiotic solutions ranged from 2 to 20 mg L⁻¹, the theoretical maximum adsorption capacities of CHMAB for ENR and MFX were 48.3 and 61.5 mg g⁻¹ at 35 °C with adsorbent dosage of 0.4 g L⁻¹, respectively, while those of MAB and HMAB were 39.6 and 54.4 mg g⁻¹, and 44.7 and 59.0 mg g⁻¹, respectively. The pseudo-second-order kinetic model and Langmuir model presented a better fitting to the spontaneous and endothermic adsorption process. The maximum adsorption capacity of ENR and MFX onto CHMAB was achieved at initial pH values of 5 and 8, respectively. Additionally, the adsorption capacity of ENR and MFX decreased with increasing concentrations of K⁺ and Ca²⁺ (0.02–0.1 mol L⁻¹). Synergism between the pore-filling effect, π-π electron-donor-acceptor interactions, regular and negative charge-assisted H-bonding, surface complexation, electrostatic interactions and hydrophobic interactions may dominate the adsorption process. This study demonstrated that a novel magnetic biochar composite prepared through pyrolysis of agricultural waste lignocellulose hydrolyzed by cellulase in combination with HA coating was a promising adsorbent for eliminating quinolone antibiotics from aqueous media.
Show more [+] Less [-]Poly-NIPAM/Fe3O4/multiwalled carbon nanotube nanocomposites for kerosene removal from water
2022
Abdullah, Thamer Adnan | Juzsakova, Tatjána | Le, Phuoc-Cuong | Kułacz, Karol | Salman, Ali D. | Rasheed, Rashed T. | Mallah, Muhammad Ali | Varga, Béla | Mansoor, Hadeel | Mako, Eva | Zsirka, Balázs | Nadda, Ashok Kumar | Nguyen, X Cuong | Nguyen, D Duc
Multiwalled carbon nanotubes (MWCNTs) were oxidized using a mixture of H₂SO₄ and HNO₃, and the oxidized MWCNTS were decorated with magnetite (Fe₃O₄). Finally, poly-N-isopropyl acrylamide-co-butyl acrylate (P-NIPAM) was added to obtain P-NIPAM/Fe/MWCNT nanocomposites. The nanosorbents were characterized by various techniques, including X-ray diffraction, transmission electron microscopy, scanning electron microscopy, thermogravimetric analysis, and Brunauer–Emmett–Teller analysis. The P-NIPAM/Fe/MWCNT nanocomposites exhibited increased surface hydrophobicity. Owing to their higher adsorption capacity, their kerosene removal efficiency was 95%; by contrast, the as-prepared, oxidized, and magnetite-decorated MWCNTs had removal efficiencies of 45%, 55%, and 68%, respectively. The P-NIPAM/Fe/MWCNT nanocomposites exhibited a sorbent capacity of 8.1 g/g for kerosene removal from water. The highest kerosene removal efficiency from water was obtained at a process time of 45 min, sorbent dose of 0.005 g, solution temperature of 40 °C, and pH 3.5. The P-NIPAM/Fe/MWCNTs showed excellent stability after four cycles of kerosene removal from water followed by regeneration. The reason may be the increase in the positive charge of the polymer at pH 3.5 and the increased adsorption affinity of the adsorbent toward the kerosene contaminant. The pseudo second-order model was found to be the most suitable model for studying the kinetics of the adsorption reaction.
Show more [+] Less [-]Potential of nanocomposites of zero valent copper and magnetite with Eleocharis dulcis biochar for packed column and batch scale removal of Congo red dye
2022
Imran, Muhammad | Andrews, Martina | Murtaza, Behzad | Ansar, Sabah | Shah, Noor Samad | Haq Khan, Zia Ul | Ali, Shahid | Boczkaj, Grzegorz | Hafeez, Farhan | Ali, Shafaqat | Rizwan, Muhammad
The current study is the first attempt to prepare nanocomposites of Eleocharis dulcis biochar (EDB) with nano zero-valent Copper (nZVCu/EDB) and magnetite nanoparticles (MNPs/EDB) for batch and column scale sequestration of Congo Red dye (CR) from synthetic and natural water. The adsorbents were characterized with advanced analytical techniques. The impact of EDB, MNPs/EDB and nZVCu/EDB dosage (1–4 g/L), pH (4–10), initial concentration of CR (20–500 mg/L), interaction time (180 min) and material type to remove CR from water was examined at ambient temperature. The CR removal followed sequence of nZVCu/EDB > MNPs/EDB > EDB (84.9–98% > 77–95% > 69.5–93%) at dosage 2 g/L when CR concentration was increased from 20 to 500 mg/L. The MNPs/EDB and nZVCu/EDB showed 10.9% and 20.1% higher CR removal than EDB. The adsorption capacity of nZVCu/EDB, MNPs/EDB and EDB was 212, 193 and 174 mg/g, respectively. Freundlich model proved more suitable for sorption experiments while pseudo 2nd order kinetic model well explained the adsorption kinetics. Fixed bed column scale results revealed excellent retention of CR (99%) even at 500 mg/L till 2 h when packed column was filled with 3.0 g nZVCu/EDB, MNPs/EDB and EDB. These results revealed that nanocomposites with biochar can be applied efficiently for the decontamination of CR contaminated water.
Show more [+] Less [-]Fabrication of activated carbon supported modified with bimetallic-platin ruthenium nano sorbent for removal of azo dye from aqueous media using enhanced ultrasonic wave
2022
Herein, activated carbon supported modified with bimetallic-platin ruthenium nano sorbent (PtRu@AC) was synthesized by a thermal decomposition process and used in the removal of methylene blue (MB) from aqueous solutions. The synthesized nano sorbents were characterized by X-ray Diffraction (XRD), Transmission Electron Microscopy (TEM), and X-ray Photoelectron Spectroscopy (XPS) spectroscopic techniques. The data obtained from characterization studies showed that PtRu@AC nano sorbent was highly crystalline and in a form of PtRu alloy with a monodispersed composition. The results indicated that the maximum adsorption capacity (qemax) for the removal of MB with PtRu@AC under optimum conditions was detected to be 1.788 mmol/g (569.4 mg/g). The experimental kinetic results of the study revealed that the adsorption of methylene blue was found to be more compatible with the false second-order model compared to some tested models. Calculations for thermodynamic functions including enthalpy change (ΔHo), entropy change (ΔSo), and Gibbs free energy change (ΔGo) values were performed to get an idea about the adsorption mechanism. As a result, the synthesized PtRu@AC nano adsorbent was detected as a highly effective adsorbent material in the removal of MB from aquatic mediums.
Show more [+] Less [-]Simultaneous capturing of mixed contaminants from wastewater using novel one-pot chitosan functionalized with EDTA and graphene oxide adsorbent
2022
Verma, Monu | Ashwani Kumar, | Lee, Ingyu | Kumar, Vinod | Park, Ju-Hyun | Kim, Hyunook
The emergence of inorganic and organic contaminants has raised great concerns owing to their adverse impact on human health and ecological security. Herein, first time one-pot process was applied for chitosan (CS) functionalization using graphene oxide (GO) and ethylenediaminetetraacetic acid (EDTA) for simultaneous capturing of toxic inorganic (lead (Pb²⁺) and cadmium (Cd²⁺)) and organic (ciprofloxacin (CIP) and sildenafil (SDF)) contaminants from wastewater. In this approach, we believe that CS would work as a backbone, GO would capture both inorganic and organic contaminants via electrostatic interactions, while EDTA would make complexation with heavy metals. Various parameters including pH, reaction time, concentration, reusability etc. were evaluated to achieve the best experimental result in monocomponent system. The prepared adsorbent displayed an excellent monolayer adsorption capacity of 351.20 and 264.10 mg g⁻¹ for Pb²⁺ and Cd²⁺, respectively, while a heterogeneous sorption capacity of 75.40 and 40.90 mg g⁻¹ for CIP and SDF, respectively. The kinetics data fitted well to Pseudo-second order (PSO) kinetics model for both types of contaminants and gave faster interaction towards metal ions (higher k₂) than organic contaminants. Experimental results showed excellent adsorption efficiencies at environmental levels in the capturing of both inorganic and organic contaminants at the same time from polluted water. The capturing mechanism of both types of contaminants was explained by elemental mapping, EDS, and FT−IR spectra. Overall, easy synthesis, excellent capturing capacity, and reusability imply that the prepared adsorbent has a sufficient potential for the treatment of co-existing toxic contaminants in water.
Show more [+] Less [-]Essence of hydroxyapatite in defluoridation of drinking water: A review
2022
Rathnayake, Anushka | Hettithanthri, Oshadi | Sandanayake, Sandun | Mahatantila, Kushani | Rajapaksha, Anushka Upamali | Vithanage, Meththika
Hydroxyapatite (HAP) is an easily synthesizable, low-cost mineral that has been recognized as a potential material for fluoride removal. Some of the synthesis methods of HAP are quite straightforward and cost-effective, while some require sophisticated synthesis techniques under advanced laboratory conditions. This review assesses the physicochemical characteristics of HAP and HAP-based composites produced via various techniques, their recent development in defluoridation and most importantly, the fluoride removal performances. For the first time, fluoride removal performances of HAP and HAP composites are compared based on partition coefficient (KD) instead of maximum adsorption capacity (Qₘₐₓ), which is significantly influenced by initial loading concentrations. Novel HAP tailored composites exhibit comparatively high KD values indicating the excellent capability of fluoride removal along with specific surface areas above 120 m²/g. HAP doped with aluminium complexes, HAP doped ceramic beads, HAP-pectin nanocomposite and HAP-stilbite nanocomposite, HAP decorated nanotubes, nanowires and nanosheets demonstrated high Qₘₐₓ and KD. The secret of HAP is not the excellent fluoride removal performances but best removal at neutral and near-neutral pH, which most of the defluoridation materials are incapable of, making them ideal adsorbents for drinking water treatment. Multiple mechanisms including physical surface adsorption, ion-exchange, and electrostatic interactions are the main mechanisms involved in defluoridation. Further research work must be focused on upscaling HAP-based composites for defluoridation on a commercial scale.
Show more [+] Less [-]Enhanced removal of per- and polyfluoroalkyl substances in complex matrices by polyDADMAC-coated regenerable granular activated carbon
2022
Ramos, Pia | Singh Kalra, Shashank | Johnson, Nicholas W. | Khor, Chia Miang | Borthakur, Annesh | Cranmer, Brian | Dooley, Gregory | Mohanty, Sanjay K. | Jassby, David | Blotevogel, Jens | Mahendra, Shaily
Granular activated carbon (GAC) has been used to remove per- and polyfluoroalkyl substances (PFASs) from industrial or AFFF-impacted waters, but its effectiveness can be low because adsorption of short-chained PFASs is ineffective and its sites are exhausted rapidly by co-contaminants. To increase adsorption of anionic PFASs on GAC by electrostatic attractions, we modified GAC's surface with the cationic polymer poly diallyldimethylammonium chloride (polyDADMAC) and tested its capacity in complex water matrices containing dissolved salts and humic acid. Amending with concentrations of polyDADMAC as low as 0.00025% enhanced GAC's adsorption capacity for PFASs, even in the presence of competing ions. This suggests that electrostatic interactions with polyDADMAC's quaternary ammonium functional groups helped bind organic and inorganic ions as well as the headgroup of short-chain PFASs, allowing more overall PFAS removal by GAC. Evaluating the effect of polymer dose is important because excessive addition can block pores and reduce overall PFAS removal rather than increase it. To decrease the waste associated with this adsorption strategy by making the adsorbent viable for more than one saturation cycle, a regeneration method is proposed which uses low-power ultrasound to enhance the desorption of PFASs from the polyDADMAC-GAC with minimum disruption to the adsorbent's structure. Re-modification with the polymer after sonication resulted in a negligible decrease in the sorbent's capacity over four saturation rounds. These results support consideration of polyDADMAC-modified GAC as an effective regenerable adsorbent for ex-situ concentration step of both short and long-chain PFASs from real waters with high concentrations of competing ions and low PFAS loads.
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