Title: Melamine-based functionalized graphene oxide and zirconium phosphate for high performance removal of mercury and lead ions from water
Heavy metal ions are highly toxic and widely spread as environmental pollutants. This work reports the development of two novel chelating adsorbents, based on the chemical modifications of graphene oxide and zirconium phosphate by functionalization with melamine-based chelating ligands for the effective and selective extraction of Hg( ii ) and Pb( ii ) from contaminated water sources. The first adsorbent melamine, thiourea-partially reduced graphene oxide (MT-PRGO) combines the heavier donor atom sulfur with the amine and triazine nitrogen's functional groups attached to the partially reduced GO nanosheets to effectively capture Hg( ii ) ions from water. The MT-PRGO adsorbent shows high efficiency for the extraction of Hg( ii ) with a capacity of 651 mg g −1 and very fast kinetics resulting in a 100% removal of Hg( ii ) from 500 ppb and 50 ppm concentrations in 15 second and 30 min, respectively. The second adsorbent, melamine zirconium phosphate (M-ZrP), is designed to combine the amine and triazine nitrogen's functional groups of melamine with the hydroxyl active sites of zirconium phosphate to effectively capture Pb( ii ) ions from water. The M-ZrP adsorbent shows exceptionally high adsorption affinity for Pb( ii ) with a capacity of 681 mg g −1 and 1000 mg g −1 using an adsorbent dose of 1 g L −1 and 2 g L −1 , respectively. The high adsorption capacity is also coupled with fast kinetics where the equilibrium time required for the 100% removal of Pb( ii ) from 1 ppm, 100 ppm and 1000 ppm concentrations is 40 seconds, 5 min and 30 min, respectively using an adsorbent dose of 1 g L −1 . In a mixture of six heavy metal ions at a concentration of 10 ppm, the removal efficiency is 100% for Pb( ii ), 99% for Hg( ii ), Cd( ii ) and Zn( ii ), 94% for Cu( ii ), and 90% for Ni( ii ) while at a higher concentration of 250 ppm the removal efficiency for Pb( ii ) is 95% compared to 23% for Hg( ii ) and less than 10% for the other ions. Because of the fast adsorption kinetics, high removal capacity, excellent regeneration, stability and reusability, the MT-PRGO and M-ZrP are proposed as top performing remediation adsorbents for the solid phase extraction of Hg( ii ) and Pb( ii ), respectively from contaminated water. more »« less
Adly, Mina Shawky; El-Dafrawy, S. M.; Ibrahim, Amr A.; El-Hakam, S. A.; El-Shall, M. Samy
(, RSC Advances)
null
(Ed.)
A highly porous adsorbent based on a metal–organic framework was successfully designed and applied as an innovative adsorbent in the solid phase for the heavy metal removal. MIL-125 was densely decorated by 2-imino-4-thiobiuret functional groups, which generated a green, rapid, and efficacious adsorbent for the uptake of Hg( ii ) and Pb( ii ) from aqueous solutions. ITB-MIL-125 showed a high adsorption affinity toward mercury( ii ) ions of 946.0 mg g −1 due to covalent bond formation with accessible sulfur-based functionality. Different factors were studied, such as the initial concentration, pH, contact time, and competitive ions, under same circumstances at the room temperature. Moreover, the experimental adsorption data were in excellent agreement with the Langmuir adsorption isotherm and pseudo-second order kinetics. At a high concentration of 100 ppm mixture of six metals, ITB-MIL-125 exhibited a high adsorption capacity, reaching more than 82% of Hg( ii ) compared to 62%, 30%, 2%, 1.9%, and 1.6% for Pb( ii ), Cu( ii ), Cd( ii ), Ni( ii ), and Zn( ii ), respectively.
Zhan, Chengbo; Sharma, Priyanka R.; He, Hongrui; Sharma, Sunil K.; McCauley-Pearl, Alexis; Wang, Ruifu; Hsiao, Benjamin S.
(, Environmental Science: Water Research & Technology)
null
(Ed.)
Rice husks are an agricultural residue of great annual production and have a high cellulose content. In this study, we have prepared highly charged carboxyl cellulose nanofibers (CNFs) from rice husks using the TEMPO-oxidation method and the extracted CNFs were evaluated as an adsorbent for the removal of lead( ii ) and lanthanum( iii ) (Pb( ii ) and La( iii )) ions from contaminated water. Three different forms of nanocellulose adsorbents were prepared: suspension, freeze-dried, and nanocomposite containing magnetic nanoparticles, where their adsorption performance was tested against the removal of the two chosen heavy metal ions. The maximum adsorption capacity of rice husk based CNFs was found to be the highest in the nanocellulose suspension, i.e. , 193.2 mg g −1 for Pb( ii ) and 100.7 mg g −1 for La( iii ). The separation of the used adsorbent in the suspension was further facilitated by the gelation of the CNFs and metal cations, where the resulting floc could be removed by gravity-driven filtration. The absorption mechanism of the investigated CNF system is mainly due to electrostatic interactions between negatively charged carboxylate groups and multivalent metal ions. It was found that 90% lanthanum content in the form of lanthanum oxychloride (determined by X-ray powder diffraction) could be obtained by incinerating the CNF/LaCl 3 gel. This study demonstrates a viable and sustainable solution to upcycle agricultural residues into remediation nanomaterials for the removal and recovery of toxic heavy metal ions from contaminated water.
Li, Duning; Lee, Cheng-Shiuan; Zhang, Yi; Das, Rasel; Akter, Fahmida; Venkatesan, Arjun K.; Hsiao, Benjamin S.
(, Journal of Materials Chemistry A)
Although most manufacturers stopped using long-chain per- and polyfluoroalkyl substances (PFASs), including perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS), short-chain PFASs are still widely employed. Short-chain PFASs are less known in terms of toxicity and have different adsorption behavior from long-chain PFASs. Previous studies have shown electrostatic interaction with the adsorbent to be the dominant mechanism for the removal of short-chain PFASs. In this study, we designed a high charge density cationic quaternized nanocellulose (QNC) to enhance the removal of both short- and long-chain PFASs from contaminated water. Systematic batch adsorption tests were conducted using the QNC adsorbent to compare its efficiency against PFASs with varying chain lengths and functional groups. From the kinetic study, PFBA (perfluorobutanoic acid), PFBS (perfluorobutanesulfonic acid) and PFOS showed rapid adsorption rates, which reached near equilibrium values (>95% of removal) between 1 min to 15 min, while PFOA required a relatively longer equilibration time of 2 h (it obtained 90% of removal within 15 min). According to the isotherm results, the maximum adsorption capacity ( Q m ) of the QNC adsorbent exhibited the following trend: PFOS ( Q m = 559 mg g −1 or 1.12 mmol g −1 ) > PFOA ( Q m = 405 mg g −1 or 0.98 mmol g −1 ) > PFBS ( Q m = 319 mg g −1 or 1.06 mmol g −1 ) > PFBA ( Q m = 121 mg g −1 or 0.57 mmol g −1 ). This adsorption order generally matches the hydrophobicity trend among four PFASs associated with both PFAS chain length and functional group. In competitive studies, pre-adsorbed short-chain PFASs were quickly desorbed by long-chain PFASs, suggesting that the hydrophobicity of the molecule played an important role in the adsorption process on to QNC. Finally, the developed QNC adsorbent was tested to treat PFAS-contaminated groundwater, which showed excellent removal efficiency (>95%) for long-chain PFASs (C7–C9) even at a low adsorbent dose of 32 mg L −1 . However, short-chain PFASs ( i.e. , PFBA and perfluoropentanoic acid (PFPeA)) were poorly removed by the QNC adsorbent (0% and 10% removal, respectively) due to competing constituents in the groundwater matrix. This was further confirmed by controlled experiments that revealed a drop in the performance of QNC to remove short-chain PFASs at elevated ionic strength (NaCl), but not for long-chain PFASs, likely due to charge neutralization of the anionic functional group of PFASs by inorganic cations. Overall, the QNC adsorbent featured improved PFAS adsorption capacity at almost two-fold of PFAS removal by granular activated carbons, especially for short-chain PFASs. We believe, QNC can complement the use of common treatment methods such as activated carbon or ionic exchange resin to remove a wide range of PFAS pollutants, heading towards the complete remediation of PFAS contamination.
Ansari, Ali; Silva_Jacovone, Raynara Maria; Nadres, Enrico Tapire; Đỗ, Minh; Rodrigues, Debora Frigi
(, Environmental Science: Water Research & Technology)
Toxic oxyanions of Cr(VI) can be potentially removed by adsorbents with positively charged surfaces. In this study, we synthesized a stable and insoluble amine-rich polymer composite (CS–PEI–GLA) by crosslinking polyethyleneimine (PEI), a soluble amine-rich synthetic polymer, and chitosan (CS) with glutaraldehyde (GLA). The positively charged amine groups were the main adsorption sites. The batch investigation demonstrated that the adsorbent was able to remove ≥90% of chromium at pH ranging from 2 to 8. Due to deprotonation of the amine groups, chromium removal decreased at higher pH values. The adsorption was fast and reached equilibrium after 45 min. The maximum adsorption capacity was 500 mg g−1 according to the Langmuir isotherm and did not decrease in the presence of monovalent anions. In the column study, the adsorption capacity was the highest when the flow rate was the lowest (5 mL min−1), influent concentration was medium (225 mg L−1), and the bed height was the shortest (3.5 cm). NaOH was the best recovery reagent with recovery of 67% in batch and 31% in the column. The CS–PEI–GLA composite was able to remove 97.1 ± 0.1% chromium in batch and treat 750 mL of electroplating wastewater with a 3.5 cm packed-bed column.
Xu, J.; Luu, L.; Tang, Y.
(, Desalination and water treatment)
Modern industrial waste waters often contain high concentrations of phosphate, and many methods have been explored to aid in its removal. This study investigates the use of magnetic nanoparticles as an adsorbent for phosphate removal. Aluminum-doped magnetic nanoparticles were synthesized using a co-precipitation method. Structure and composition analysis of the prepared magnetic nanoparticles indicated an inverse spinal structure with a composition of FeAl0.75Fe1.25O4. These nanoparticles were tested for their phosphate removal properties, including adsorption capacity, selectivity, and kinetic models. They showed great affinity to phosphate with a maximum adsorption capacity of 102 mg/g. Additionally, the adsorption was selective, and the presence of other common anions and organic matters did not interfere with the phosphate adsorption efficacy. The kinetic analysis of phosphate adsorption suggested a pseudo-second-order adsorption behavior, and the adsorption isotherm studies indicated a Langmuir type adsorption. The phosphate removal capabilities of the nanoparticles were also tested in poultry rinsing water, tap water, and municipal wastewaters, all with high phosphate removal efficiency. The overall results from these experiments showed promising results for the phosphate removal efficacy of these nanoparticles.
Bakry, Ayyob M., Awad, Fathi S., Bobb, Julian A., Ibrahim, Amr A., and El-Shall, M. Samy. Melamine-based functionalized graphene oxide and zirconium phosphate for high performance removal of mercury and lead ions from water. Retrieved from https://par.nsf.gov/biblio/10275602. RSC Advances 10.62 Web. doi:10.1039/d0ra07546a.
Bakry, Ayyob M., Awad, Fathi S., Bobb, Julian A., Ibrahim, Amr A., & El-Shall, M. Samy. Melamine-based functionalized graphene oxide and zirconium phosphate for high performance removal of mercury and lead ions from water. RSC Advances, 10 (62). Retrieved from https://par.nsf.gov/biblio/10275602. https://doi.org/10.1039/d0ra07546a
Bakry, Ayyob M., Awad, Fathi S., Bobb, Julian A., Ibrahim, Amr A., and El-Shall, M. Samy.
"Melamine-based functionalized graphene oxide and zirconium phosphate for high performance removal of mercury and lead ions from water". RSC Advances 10 (62). Country unknown/Code not available. https://doi.org/10.1039/d0ra07546a.https://par.nsf.gov/biblio/10275602.
@article{osti_10275602,
place = {Country unknown/Code not available},
title = {Melamine-based functionalized graphene oxide and zirconium phosphate for high performance removal of mercury and lead ions from water},
url = {https://par.nsf.gov/biblio/10275602},
DOI = {10.1039/d0ra07546a},
abstractNote = {Heavy metal ions are highly toxic and widely spread as environmental pollutants. This work reports the development of two novel chelating adsorbents, based on the chemical modifications of graphene oxide and zirconium phosphate by functionalization with melamine-based chelating ligands for the effective and selective extraction of Hg( ii ) and Pb( ii ) from contaminated water sources. The first adsorbent melamine, thiourea-partially reduced graphene oxide (MT-PRGO) combines the heavier donor atom sulfur with the amine and triazine nitrogen's functional groups attached to the partially reduced GO nanosheets to effectively capture Hg( ii ) ions from water. The MT-PRGO adsorbent shows high efficiency for the extraction of Hg( ii ) with a capacity of 651 mg g −1 and very fast kinetics resulting in a 100% removal of Hg( ii ) from 500 ppb and 50 ppm concentrations in 15 second and 30 min, respectively. The second adsorbent, melamine zirconium phosphate (M-ZrP), is designed to combine the amine and triazine nitrogen's functional groups of melamine with the hydroxyl active sites of zirconium phosphate to effectively capture Pb( ii ) ions from water. The M-ZrP adsorbent shows exceptionally high adsorption affinity for Pb( ii ) with a capacity of 681 mg g −1 and 1000 mg g −1 using an adsorbent dose of 1 g L −1 and 2 g L −1 , respectively. The high adsorption capacity is also coupled with fast kinetics where the equilibrium time required for the 100% removal of Pb( ii ) from 1 ppm, 100 ppm and 1000 ppm concentrations is 40 seconds, 5 min and 30 min, respectively using an adsorbent dose of 1 g L −1 . In a mixture of six heavy metal ions at a concentration of 10 ppm, the removal efficiency is 100% for Pb( ii ), 99% for Hg( ii ), Cd( ii ) and Zn( ii ), 94% for Cu( ii ), and 90% for Ni( ii ) while at a higher concentration of 250 ppm the removal efficiency for Pb( ii ) is 95% compared to 23% for Hg( ii ) and less than 10% for the other ions. Because of the fast adsorption kinetics, high removal capacity, excellent regeneration, stability and reusability, the MT-PRGO and M-ZrP are proposed as top performing remediation adsorbents for the solid phase extraction of Hg( ii ) and Pb( ii ), respectively from contaminated water.},
journal = {RSC Advances},
volume = {10},
number = {62},
author = {Bakry, Ayyob M. and Awad, Fathi S. and Bobb, Julian A. and Ibrahim, Amr A. and El-Shall, M. Samy},
editor = {null}
}
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