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Versatile Functionalization of Carbon Nanomaterials by Ferrate(VI).

ABSTRACT: As a high-valent iron compound with Fe in the highest accessible oxidation state, ferrate(VI) brings unique opportunities for a number of areas where chemical oxidation is essential. Recently, it is emerging as a novel oxidizing agent for materials chemistry, especially for the oxidation of carbon materials. However, the reported reactivity in liquid phase (H₂SO₄ medium) is confusing, which ranges from aggressive to moderate, and even incompetent. Meanwhile, the solid-state reactivity underlying the "dry" chemistry of ferrate(VI) remains poorly understood. Herein, we scrutinize the reactivity of K₂FeO₄ using fullerene C₆₀ and various nanocarbons as substrates. The results unravel a modest reactivity in liquid phase that only oxidizes the active defects on carbon surface and a powerful oxidizing ability in solid state that can open the inert C=C bonds in carbon lattice. We also discuss respective benefit and limitation of the wet and dry approaches. Our work provides a rational understanding on the oxidizing ability of ferrate(VI) and can guide its application in functionalization/transformation of carbons and also other kinds of materials.

SUBMITTER: Zhou Y

PROVIDER: S-EPMC7770691 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Ferrate(VI) Oxidation Mechanism of Substituted Anilines: A Density Functional Theory Investigation.

Project description:Ferrate(VI) (Fe(VI)) is a promising oxidant coagulant and disinfectant for the degradation of organic micropollutants. However, it is hard to elucidate the detailed oxidation mechanism through the current experimental approaches. Substituted anilines (SANs) are important chemical compounds that are widely used in many industries. This paper presents the use of density functional theory (DFT) to understand the oxidation mechanism of SANs by Fe(VI) and the effect of substituents. The calculation results revealed that the primary oxidations of SANs follow the hydrogen atom transfer (HAT) mechanism. Interestingly, the hydroxyl oxygen of HFeO4 - is more reactive than the carbonyl oxygen when reacting with SANs. The formation of the SAN radical is crucial, and all of the products are formed from it. Azobenzene is more favorable to generate the above products. In addition, the obtained results indicate that this kind of substituent has a much greater influence on the reaction rather than the position. Thus, the present study provides a valuable insight into the transformation pathways of SANs in the Fe(VI) oxidation process and the effects of the substituent on oxidation. These results will advance the understanding of Fe(VI) involved in wastewater treatment.

| S-EPMC8190916 | biostudies-literature

Oxidation of Pharmaceuticals by Ferrate(VI)-Amino Acid Systems: Enhancement by Proline.

Project description:The occurrence of micropollutants in water threatens public health and ecology. Removal of micropollutants such as pharmaceuticals by a green oxidant, ferrate(VI) (FeVIO42-, Fe(VI)) can be accomplished. However, electron-deficient pharmaceuticals, such as carbamazepine (CBZ) showed a low removal rate by Fe(VI). This work investigates the activation of Fe(VI) by adding nine amino acids (AA) of different functionalities to accelerate the removal of CBZ in water under mild alkaline conditions. Among the studied amino acids, proline, a cyclic AA, had the highest removal of CBZ. The accelerated effect of proline was ascribed by demonstrating the involvement of highly reactive intermediate Fe(V) species, generated by one-electron transfer by the reaction of Fe(VI) with proline (i.e., Fe(VI) + proline → Fe(V) + proline•). The degradation kinetics of CBZ by a Fe(VI)-proline system was interpreted by kinetic modeling of the reactions involved that estimated the rate of the reaction of Fe(V) with CBZ as (1.03 ± 0.21) × 106 M-1 s-1, which was several orders of magnitude greater than that of Fe(VI) of 2.25 M-1 s-1. Overall, natural compounds such as amino acids may be applied to increase the removal efficiency of recalcitrant micropollutants by Fe(VI).

| S-EPMC10848263 | biostudies-literature

Dissolved Organic Phosphorus Removal in Secondary Effluent by Ferrate (VI): Performance and Mechanism.

Project description:Dissolved organic phosphorus (DOP), which is recalcitrant in municipal wastewater treatment, accounts for 26-81% of dissolved total phosphorus in the effluent. More importantly, the majority of DOP could be bioavailable, potentially threatening the aquatic environment through eutrophication. This study aimed to develop a ferrate (VI)-based advanced treatment to effectively destruct and remove DOP from secondary effluent and use deoxyribonucleic acid (DNA) and adenosine-5'-triphosphate (ATP) as DOP model compounds to explore the relevant mechanisms. The results showed that ferrate (VI) treatment could efficiently destruct and remove 75% of the DOP in secondary effluent from an activated sludge-adopted municipal wastewater treatment plant, under normal operating conditions. Moreover, the coexistence of nitrate, ammonia, and alkalinity barely affected the effectiveness, while the presence of phosphate significantly inhibited DOP removal. The mechanistic study revealed that ferrate (VI)-induced particle adsorption was the dominant way to achieve DOP reduction, rather than oxidating DOP to phosphate and forming precipitation afterward. Meanwhile, DOP molecules could be effectively decomposed into smaller ones by ferrate (VI) oxidation. This study clearly demonstrated that ferrate (VI) treatment could achieve a promising DOP removal from secondary effluent for mitigating the risk of eutrophication in receiving water bodies.

| S-EPMC9956993 | biostudies-literature

Versatile electrification of two-dimensional nanomaterials in water.

Project description:The recent emergence of nanofluidics has highlighted the exceptional properties of graphene and its boron-nitride counterpart as confining nanomaterials for water and ion transport. Surprisingly, ionic transport experiments have unveiled a consequent electrification of the water/carbon surfaces, with a contrasting response for its water/boron-nitride homologue. In this paper, we report free energy calculations based on ab initio molecular dynamics simulations of hydroxide OH- ions in water near graphene and hexagonal boron nitride (h-BN) layers. Our results disclose that both surfaces get charged through hydroxide adsorption, but two strongly different mechanisms are evidenced. The hydroxide species shows weak physisorption on the graphene surface while it exhibits also strong chemisorption on the h-BN surface. Interestingly OH- is shown to keep very fast lateral dynamics and interfacial mobility within the physisorbed layer on graphene. Taking into account the large ionic surface conductivity, an analytic transport model allows to reproduce quantitatively the experimental data.

| S-EPMC6458114 | biostudies-literature

Accelerated Oxidation of Organic Contaminants by Ferrate(VI): The Overlooked Role of Reducing Additives.

Project description:This paper presents an accelerated ferrate(VI) (FeVIO42-, FeVI) oxidation of contaminants in 30 s by adding one-electron and two-electron transfer reductants (R(1) and R(2)). An addition of R(2) (e.g., NH2OH, AsIII, SeIV, PIII, and NO2-, and S2O32-) results in FeIV initially, while FeV is generated with the addition of R(1) (e.g., SO32-). R(2) additives, except S2O32-, show the enhanced oxidation of 20-40% of target contaminant, trimethoprim (TMP). Comparatively, enhanced oxidation of TMP was up to 100% with the addition of R(1) to FeVI. Interestingly, addition of S2O32- (i.e., R(2)) also achieves the enhanced oxidation to 100%. Removal efficiency of TMP depends on the molar ratio ([R(1)]:[FeVI] or [R(2)]:[FeVI]). Most of the reductants have the highest removal at molar ratio of ?0.125. A FeVI-S2O32- system also oxidizes rapidly a wide range of organic contaminants (pharmaceuticals, pesticides, artificial sweetener, and X-ray contrast media) in water and real water matrices. FeV and FeIV as the oxidative species in the FeVI-S2O32--contaminant system are elucidated by determining removal of contaminants in oxygenated and deoxygenated water, applying probing agent, and identifying oxidized products of TMP and sulfadimethoxine (SDM) by FeVI-S2O32- systems. Significantly, elimination of SO2 from sulfonamide (i.e., SDM) is observed for the first time.

| S-EPMC6300057 | biostudies-literature

Near Green Synthesis of Porous Graphene from Graphite Using an Encapsulated Ferrate(VI) Oxidant.

Project description:Graphene oxide (GO) is a conventional yet vital precursor for the synthesis of porous graphene (PG). Several strong oxidizing agents such as potassium permanganate and perchlorates are typically used for oxidization of graphite. However, they expose toxic reactants/products that harm the environment. Therefore, a greener approach is desperately needed to oxidize and exfoliate graphite. This study reports for the first time on successful oxidation of graphite by ferrate(VI) compounds via an encapsulation approach. By further reducing GO prepared from this near green route with vitamin C, PG anticipated by many highly important and expanding areas such as water treatment could be readily achieved. X-ray diffraction (XRD), Fourier transform infrared (FTIR) and UV-vis spectroscopy, and scanning electronic microscopy (SEM) along with energy-dispersive spectroscopy confirmed the high yield of GO from the oxidation of graphite. Raman spectroscopy, XRD, and TEM confirmed the formation of high-quality few-layered PG from the reduction of as-prepared GO. The above results demonstrated the practicality of using encapsulated ferrate(VI) compounds to realize green oxidation of graphite and resolve the paradox about the oxidation capability of ferrate(VI). To further illustrate its potential for the removal of emerging and crucial contaminants from water, as-prepared PG was further examined against the contaminants of methyl orange (MeO) dye and ibuprofen (IBU). Taken together, the results revealed that more than 90% removal efficiency could be achieved at a high PG dosage against MeO and IBU. This ground-breaking greener approach opens the door to risk-free, extensive graphene environmental applications.

| S-EPMC10433472 | biostudies-literature

Oxygen-evolution reaction by nickel/nickel oxide interface in the presence of ferrate(VI).

Project description:In this study, we investigate the effect of K2FeO4, as a new and soluble Fe salt at alkaline conditions, on oxygen-evolution reaction (OER) of Ni oxide. Both oxidation and reduction peaks for Ni in the presence and absence of Fe are linearly changed by (scan rate)1/2. Immediately after the interaction of [FeO4]2- with the surface of the electrode, a significant increase in OER is observed. This could be indicative of the fact that either the [FeO4]2- on the surface of Ni oxide is directly involved in OER, or, it is important to activate Ni oxide toward OER. Due to the change in the Ni(II)/(III) peak, it is hypothesized that Fe impurity in KOH or electrochemical cell has different effects at the potential range. At low potential, [FeO4]2- is reduced on the surface of the electrode, and thus, is significantly adsorbed on the electrode. Finally, oxygen-evolution measurements of K2FeO4 and Ni2O3 are investigated under chemical conditions. K2FeO4 is not stable in the presence of Ni(II) oxide, and OER is observed in a KOH solution (pH ≈ 13).

| S-EPMC7260238 | biostudies-literature

Interaction studies of carbon nanomaterials and plasma activated carbon nanomaterials solution with telomere binding protein.

Project description:Most cancer cells have telomerase activity because they can express the human telomerase reverse transcriptase (hTERT) gene. Therefore, the inhibition of the hTERT expression can play an important role in controlling cancer cell proliferation. Our current study aims to inhibit hTERT expression. For this, we synthesized graphene oxide (GO) and a functionalized multiwall carbon nanotube (f-MWCNT), latter treated them with cold atmospheric pressure plasma for further analysis of the hTERT expression. The inhibition of hTERT expression by GO, f-MWCNT, plasma activated GO solution (PGOS), and plasma activated f-MWCNT solution (PCNTS), was studied using two lung cancer cell lines, A549 and H460. The hTERT experimental results revealed that GO and PGOS sufficiently decreased the hTERT concentration, while f-MWCNT and PCNTS were unable to inhibit the hTERT concentration. Therefore, to understand the inhibition mechanism of hTERT, we studied the binding properties of GO and PGOS with telomere binding protein (AtTRB2). The interaction studies were carried out using circular dichroism, fluorescence, 1H-15N NMR spectroscopy, and size-exclusion chromatography (SEC) binding assay. We also used docking simulation to have an better understanding of the interactions between GO nanosheets and AtTRB2 protein. Our results may provide new insights that can benefit in biomedical treatments.

| S-EPMC5454022 | biostudies-literature

Ferrate(VI) pre-treatment and subsequent chlorination of blue-green algae: Quantification of disinfection byproducts.

Project description:Algal organic matter (AOM) from seasonal algal blooms may be an important precursor of disinfection byproducts (DBPs) in drinking water. This paper presents the effect of ferrate(VI) treatment on two blue-green algae, Chlorella sp. and Pseudanabaena limnetica, in eutrophic water. The results demonstrated that Fe(VI) removed the algal cells by causing cell death, apoptosis, and lost integrity, and decreased AOM (in terms of total organic carbon) in water via oxidation and coagulation. Chlorination of the Fe(VI) pre-oxidized algal water samples generated halogenated DBPs (including trihalomethanes, haloacetic acids, haloketones, chloral hydrate, haloacetonitriles, and trichloronitromethane), but the concentrations of DBPs were lower than those formed in the chlorinated samples without pre-treatment by Fe(VI). Higher Fe(VI) dose, longer oxidation time, and alkaline pH were beneficial in controlling DBPs. In bromide-containing algal solutions, negligible amount of bromo-DBPs were generated in the Fe(VI) pre-oxidation, and halogenated DBPs were mainly formed in the subsequent chlorination.

| S-EPMC7711035 | biostudies-literature

Stabilized Lignin Nanoparticles for Versatile Hybrid and Functional Nanomaterials.

Project description:Spherical lignin nanoparticles are emerging biobased nanomaterials, but instability and dissolution in organic solvents and aqueous alkali restrict their applicability. Here, we report the synthesis of hydroxymethylated lignin nanoparticles and their hydrothermal curing to stabilize the particles by internal cross-linking reactions. These colloidally stable particles contain a high biobased content of 97% with a tunable particle size distribution and structural stability in aqueous media (pH 3 to 12) and organic solvents such as acetone, ethanol, dimethylformamide, and tetrahydrofuran. We demonstrate that the free phenolic hydroxyl groups that are preserved in the cured particles function as efficient reducing sites for silver ions, giving rise to hybrid lignin-silver nanoparticles that can be used for quick and facile sensing of hydrogen peroxide. The stabilized lignin particles can also be directly modified using base-catalyzed reactions such as the ring-opening of cationic epoxides that render the particles with pH-dependent agglomeration and redispersion properties. Combining scalable synthesis, solvent stability, and reusability, this new class of lignin nanoparticles shows potential for its use in circular biobased nanomaterials.

| S-EPMC9667459 | biostudies-literature

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