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1.
J Environ Sci (China) ; 147: 114-130, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39003034

RESUMO

Fenton and Fenton-like processes, which could produce highly reactive species to degrade organic contaminants, have been widely used in the field of wastewater treatment. Therein, the chemistry of Fenton process including the nature of active oxidants, the complicated reactions involved, and the behind reason for its strongly pH-dependent performance, is the basis for the application of Fenton and Fenton-like processes in wastewater treatment. Nevertheless, the conflicting views still exist about the mechanism of the Fenton process. For instance, reaching a unanimous consensus on the nature of active oxidants (hydroxyl radical or tetravalent iron) in this process remains challenging. This review comprehensively examined the mechanism of the Fenton process including the debate on the nature of active oxidants, reactions involved in the Fenton process, and the behind reason for the pH-dependent degradation of contaminants in the Fenton process. Then, we summarized several strategies that promote the Fe(II)/Fe(III) cycle, reduce the competitive consumption of active oxidants by side reactions, and replace the Fenton reagent, thus improving the performance of the Fenton process. Furthermore, advances for the future were proposed including the demand for the high-accuracy identification of active oxidants and taking advantages of the characteristic of target contaminants during the degradation of contaminants by the Fenton process.


Assuntos
Peróxido de Hidrogênio , Ferro , Eliminação de Resíduos Líquidos , Ferro/química , Peróxido de Hidrogênio/química , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Águas Residuárias/química , Oxirredução , Radical Hidroxila/química
2.
J Environ Sci (China) ; 147: 370-381, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39003055

RESUMO

Two strains of Fe/Mn oxidizing bacteria tolerant to high concentrations of multiple heavy metal(loid)s and efficient decontamination for them were screened. The surface of the bio-Fe/Mn oxides produced by the oxidation of Fe(II) and Mn(II) by Pseudomonas taiwanensis (marked as P4) and Pseudomonas plecoglossicida (marked as G1) contains rich reactive oxygen functional groups, which play critical roles in the removal efficiency and immobilization of heavy metal(loid)s in co-contamination system. The isolated strains P4 and G1 can grow well in the following environments: pH 5-9, NaCl 0-4%, and temperature 20-30°C. The removal efficiencies of Fe, Pb, As, Zn, Cd, Cu, and Mn are effective after inoculation of the strains P4 and G1 in the simulated water system (the initial concentrations of heavy metal(loid) were 1 mg/L), approximately reaching 96%, 92%, 85%, 67%, 70%, 54% and 15%, respectively. The exchangeable and carbonate bound As, Cd, Pb and Cu are more inclined to convert to the Fe-Mn oxide bound fractions in P4 and G1 treated soil, thereby reducing the phytoavailability and bioaccessible of heavy metal(loid)s. This research provides alternatives method to treat water and soil containing high concentrations of multi-heavy metal(loid)s.


Assuntos
Metais Pesados , Poluentes do Solo , Poluentes Químicos da Água , Poluentes Químicos da Água/metabolismo , Poluentes Químicos da Água/análise , Poluentes do Solo/metabolismo , Oxirredução , Pseudomonas/metabolismo , Manganês , Ferro/química , Ferro/metabolismo , Solo/química , Biodegradação Ambiental , Microbiologia do Solo
3.
J Environ Sci (China) ; 147: 523-537, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39003068

RESUMO

Due to its high efficiency, Fe(II)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants. A lot of chemical Fe sludge along with various refractory pollutants was concomitantly produced, which may cause secondary environmental problems without proper disposal. We here innovatively proposed an effective method of achieving zero Fe sludge, reusing Fe resources (Fe recovery = 100%) and advancing organics removal (final TOC removal > 70%) simultaneously, based on the in situ formation of magnetic Ca-Fe layered double hydroxide (Fe3O4@CaFe-LDH) nano-material. Cations (Ca2+ and Fe3+) concentration (≥ 30 mmol/L) and their molar ratio (Ca:Fe ≥ 1.75) were crucial to the success of the method. Extrinsic nano Fe3O4 was designed to be involved in the Fe(II)-catalytic wastewater treatment process, and was modified by oxidation intermediates/products (especially those with COO- structure), which promoted the co-precipitation of Ca2+ (originated from Ca(OH)2 added after oxidation process) and by-produced Fe3+ cations on its surface to in situ generate core-shell Fe3O4@CaFe-LDH. The oxidation products were further removed during Fe3O4@CaFe-LDH material formation via intercalation and adsorption. This method was applicable to many kinds of organic wastewater, such as bisphenol A, methyl orange, humics, and biogas slurry. The prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported CaFe-LDHs. This work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(II)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.


Assuntos
Oxirredução , Eliminação de Resíduos Líquidos , Águas Residuárias , Poluentes Químicos da Água , Poluentes Químicos da Água/química , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Catálise , Ferro/química
4.
Biomaterials ; 313: 122793, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39226655

RESUMO

Numerous nanoparticles have been utilized to deliver Fe2+ for tumor ferroptosis therapy, which can be readily converted to Fe3+via Fenton reactions to generate hydroxyl radical (•OH). However, the ferroptosis therapeutic efficacy of large tumors is limited due to the slow conversion of Fe3+ to Fe2+via Fenton reactions. Herein, a strategy of intratumor Fe3+/2+ cyclic catalysis is proposed for ferroptosis therapy of large tumors, which was realized based on our newly developed hollow mesoporous iron sesquioxide nanoparticle (HMISN). Cisplatin (CDDP) and Gd-poly(acrylic acid) macrochelates (GP) were loaded into the hollow core of HMISN, whose surface was modified by laccase (LAC). Fe3+, CDDP, GP, and LAC can be gradually released from CDDP@GP@HMISN@LAC in the acidic tumor microenvironment. The intratumor O2 can be catalyzed into superoxide anion (O2•-) by LAC, and the intratumor NADPH oxidases can be activated by CDDP to generate O2•-. The O2•- can react with Fe3+ to generate Fe2+, and raise H2O2 level via the superoxide dismutase. The generated Fe2+ and H2O2 can be fast converted into Fe3+ and •OH via Fenton reactions. The cyclic catalysis of intratumor Fe3+/2+ initiated by CDDP@GP@HMISN@LAC can be used for ferroptosis therapy of large tumors.


Assuntos
Ferroptose , Ferro , Ferroptose/efeitos dos fármacos , Animais , Catálise , Humanos , Ferro/química , Linhagem Celular Tumoral , Nanopartículas/química , Porosidade , Camundongos , Cisplatino/química , Cisplatino/uso terapêutico , Neoplasias/tratamento farmacológico , Antineoplásicos/uso terapêutico , Antineoplásicos/química , Camundongos Endogâmicos BALB C , Peróxido de Hidrogênio/química , Microambiente Tumoral/efeitos dos fármacos , Camundongos Nus , Feminino
5.
J Environ Sci (China) ; 148: 198-209, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095157

RESUMO

Norfloxacin is widely used owing to its strong bactericidal effect on Gram-negative bacteria. However, the residual norfloxacin in the environment can be biomagnified via food chain and may damage the human liver and delay the bone development of minors. Present work described a reliable and sensitive smartphone colorimetric sensing system based on cobalt-doped Fe3O4 magnetic nanoparticles (Co-Fe3O4 MNPs) for the visual detection of norfloxacin. Compared with Fe3O4, Co-Fe3O4 MNPs earned more remarkably peroxidase-like activity and TMB (colorless) was rapidly oxidized to oxTMB (blue) with the presence of H2O2. Interestingly, the addition of low concentration of norfloxacin can accelerate the color reaction process of TMB, and blue deepening of the solution can be observed with the naked eye. However, after adding high concentration of norfloxacin, the activity of nanozyme was inhibited, resulting in the gradual fading of the solution. Based on this principle, a colorimetric sensor integrated with smartphone RGB mode was established. The visual sensor exhibited good linearity for norfloxacin monitoring in the range of 0.13-2.51 µmol/L and 17.5-100 µmol/L. The limit of visual detection was 0.08 µmol/L. In the actual water sample analysis, the spiked recoveries of norfloxacin were over the range of 95.7%-104.7 %. These results demonstrated that the visual sensor was a convenient and fast method for the efficient and accurate detection of norfloxacin in water, which may have broad application prospect.


Assuntos
Cobalto , Colorimetria , Norfloxacino , Smartphone , Poluentes Químicos da Água , Norfloxacino/análise , Colorimetria/métodos , Cobalto/análise , Cobalto/química , Poluentes Químicos da Água/análise , Antibacterianos/análise , Peroxidase , Limite de Detecção
6.
J Environ Sci (China) ; 148: 274-282, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095164

RESUMO

Developing cost-effective and high-performance catalyst systems for dry reforming of methane (DRM) is crucial for producing hydrogen (H2) sustainably. Herein, we investigate using iron (Fe) as a promoter and major alumina support in Ni-based catalysts to improve their DRM performance. The addition of iron as a promotor was found to add reducible iron species along with reducible NiO species, enhance the basicity and induce the deposition of oxidizable carbon. By incorporating 1 wt.% Fe into a 5Ni/10ZrAl catalyst, a higher CO2 interaction and formation of reducible "NiO-species having strong interaction with support" was observed, which led to an ∼80% H2 yield in 420 min of Time on Stream (TOS). Further increasing the Fe content to 2wt% led to the formation of additional reducible iron oxide species and a noticeable rise in H2 yield up to 84%. Despite the severe weight loss on Fe-promoted catalysts, high H2 yield was maintained due to the proper balance between the rate of CH4 decomposition and the rate of carbon deposit diffusion. Finally, incorporating 3 wt.% Fe into the 5Ni/10ZrAl catalyst resulted in the highest CO2 interaction, wide presence of reducible NiO-species, minimum graphitic deposit and an 87% H2 yield. Our findings suggest that iron-promoted zirconia-alumina-supported Ni catalysts can be a cheap and excellent catalytic system for H2 production via DRM.


Assuntos
Óxido de Alumínio , Hidrogênio , Ferro , Metano , Níquel , Zircônio , Metano/química , Zircônio/química , Catálise , Ferro/química , Hidrogênio/química , Óxido de Alumínio/química , Níquel/química
7.
Spectrochim Acta A Mol Biomol Spectrosc ; 324: 124948, 2025 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-39146630

RESUMO

Herein, a nanocomposite of Cu,Ce-containing phosphotungstates (Cu,Ce-PTs) with outstanding laccase-like activity was fabricated via a one-pot microwave-assisted hydrothermal method. Notably, it was discovered that both Fe3+ and Cr6+ could significantly enhance the electron transfer rates of Ce3+ and Ce4+, along with generous Cu2+ with high catalytic activity, thereby promoting the laccase-like activity of Cu,Ce-PTs. The proposed system can be used for the detection of Fe3+ and Cr6+ in a range of 0.667-333.33 µg/mL and 0.033-33.33 µg/mL with a low detection limit of 0.135 µg/mL and 0.0288 µg/mL, respectively. The proposed assay exhibits excellent reusability and selectivity and can be used in traditional Chinese medicine samples analysis.


Assuntos
Cério , Cromo , Colorimetria , Cobre , Ferro , Lacase , Cobre/análise , Cobre/química , Cromo/análise , Colorimetria/métodos , Lacase/metabolismo , Lacase/química , Ferro/análise , Ferro/química , Cério/química , Limite de Detecção , Ácido Fosfotúngstico/química , Nanocompostos/química , Catálise
8.
Spectrochim Acta A Mol Biomol Spectrosc ; 324: 124970, 2025 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-39153349

RESUMO

Due to their exceptional optical properties and adjustable functional characteristics, hydrogen-bonded organic frameworks (HOFs) demonstrate significant potential in applications such as sensing, information encryption. However, studies on the synthesis of HOFs designed to construct multifunctional platforms are scant. In this work, we report the synthesis of a new fluorescent HOF by assembling melem and isophthalic acid (IPA), designated as HOF-IPA. HOF-IPA exhibited good selectivity and sensitivity towards Fe3+, making it suitable as a fluorescent sensor for Fe3+ detection. The sensor achieved satisfactory recoveries ranging from 97.79 % to106.42 % for Fe3+ sensing, with a low relative standard deviation (RSD) of less than 3.33 %, indicating significant application potential for HOF-IPA. Due to the ability of F- to mask the electrostatic action on the surface of Fe3+ and inhibit the photoelectron transfer (PET) of HOF-IPA, the HOF-IPA - Fe3+ system can be utilized as a fluorescent "off-on" sensor for F- detection. Additionally, owing to the colorless, transparent property of HOF-IPA in aqueous solution under sunlight and its blue fluorescence property under UV light (color) or microplate reader (fluorescence intensity), HOF-IPA based ink can be used for various types of information encryption, and all yielding favorable outcomes.

9.
Spectrochim Acta A Mol Biomol Spectrosc ; 324: 124993, 2025 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-39159512

RESUMO

BODIPY-based chemosensors are widely used owing to merits like good selectivity, high fluorescence quantum yield, and excellent optical stability. As such, a pH-switchable hydrophilic fluorescent probe, BODIPY-PY-(SO3Na)2, was developed for detection of Fe3+ ion in aqueous solutions. BODIPY-PY-(SO3Na)2 revealed strong fluorescence intensity and was responsive to pH value in the range of 6.59-1.96. Additionally, BODIPY-PY-(SO3Na)2 showed good selectivity and sensitivity towards Fe3+. A good linear relationship for Fe3+ detection was obtained from 0.0 µM to 50.0 µM with low detecting limit of 6.34 nM at pH 6.59 and 2.36 nM at pH 4.32, respectively. The response to pH and detection of Fe3+ induced obvious multicolor changes. BODIPY-PY-(SO3Na)2 can also be utilized to quantitatively detect Fe3+ in real water sample. Different mechanisms of Fe3+ detection at investigated pH values were unraveled through relativistic density functional theory (DFT) calculations in BODIPY-PY-(SO3Na)2 and experiments of coexisting cations, anions and molecules. These results enabled us to gain a deeper understanding of the interactions between BODIPY-PY-(SO3Na)2 and Fe3+ and provide valuable fundamental information for design of efficient multicolor chemosensors for Fe3+ as well.

10.
J Environ Sci (China) ; 150: 78-90, 2025 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-39306442

RESUMO

The migration and transformation of hexavalent chromium (Cr(VI)) in the environment are regulated by pyrite (FeS2). However, variations in pyrite crystal facets influence the adsorption behavior and electron transfer between pyrite and Cr(VI), thereby impacting the Cr(VI) reduction performance. Herein, two naturally common facets of pyrite were synthesized hydrothermally to investigate the facet-dependent mechanisms of Cr(VI) reduction. The experimental results revealed that the {111} facet exhibited approximately 1.30-1.50 times higher efficiency in Cr(VI) reduction compared to the {100} facet. Surface analyses and electrochemical results indicated that {111} facet displayed a higher iron-sulfur oxidation level, which was affected by its superior electrochemical properties during the reaction with Cr(VI). Density functional theory (DFT) calculations demonstrated that the narrower band gap and lower work function on {111} facet were more favorable for the electron transfer between Fe(II) and Cr(VI). Furthermore, different adsorption configurations were observed on {100} and {111} surfaces due to the unique arrangements of Fe and S atoms. Specifically, O atoms in Cr2O72- directly bound with the S sites on {100} but the Fe sites on {111}. According to the density of states (DOS), the Fe site had better reactivity than the S site in the reaction, which appeared to be related to the fracture of S-S bonds. Additionally, the adsorption configuration of Cr2O72- on {111} surface showed a stronger adsorption energy and a more stable coordination mode, favoring subsequent Cr(VI) reduction process. These findings provide an in-depth analysis of facet-dependent mechanisms underlying Cr(VI) reduction behavior, offering new insights into studying environmental interactions between heavy metals and natural minerals.


Assuntos
Cromo , Ferro , Oxirredução , Sulfetos , Cromo/química , Ferro/química , Sulfetos/química , Modelos Químicos , Adsorção
11.
J Colloid Interface Sci ; 677(Pt A): 25-34, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39079213

RESUMO

HYPOTHESIS: Through the rational design of nanomaterial composites, broadband light harvesting and good thermal insulation can be achieved simultaneously to improve the efficiency of water evaporation. EXPERIMENT: Solar evaporation experiments were carried out on liquid marbles (LMs) coated with Fe3O4 nanoparticles, carbon nanotubes (CNTs) and hybrid nanomaterials (Fe3O4/CNTs) with different mass ratios of 2:1, 1:1 and 1:2. FINDING: The results showed that the mixture of Fe3O4/CNTs enhances the light harvesting ability and solar interfacial evaporation performance. Fe3O4/CNT-LM at the mass ratio of 2:1 case provides the highest evaporation rate of 11.03 µg/s, which is about 1.22 and 1.34 times higher than that of Fe3O4 and CNT, respectively. This high performance is mainly due to the synergistic effect between Fe3O4 nanoparticles and CNTs, as the hybrid nanostructure significantly improves the both photothermal conversion and heat localization capability. Numerical simulation further supports that the composite can concentrate the electromagnetic field and heat at the phase-change interface. This leads to a rapid evaporation of the boundary region. This study provides a novel approach to a three-dimensional interface by assembling nanomaterials on the drop surface to enhance evaporation, which may have far-reaching implications for seawater desalination.

12.
J Colloid Interface Sci ; 677(Pt A): 264-272, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39094487

RESUMO

The electrocatalytic nitrogen reduction reaction (NRR) is a crucial process in addressing energy shortages and environmental concerns by synthesizing the NH3. However, the difficulty of N2 activation and fewer NRR active sites limit the application of NRR. Therefore, the NRR performance can be improved by rapid electron transport paths to participate in multi-electron reactions and N2 activation. Doping with transition metal element is a viable strategy to provide electrons and electronic channels in the NRR. This study focuses on the synthesis of Fe2(MoO4)3 (FeMo) and x%La-doped FeMo (x = 3, 5, 7, and 10) using the hydrothermal method. La-doping creates electron transport channels Fe2+-O2--Fe3+ and oxygen vacancies, achieving an equal molar ratio of Fe2+/Fe3+. This strategy enables the super-exchange in Fe2+-O2--Fe3+, and then enhances electron transport speed for a rapid hydrogenation reaction. Therefore, the synergistic effect of Fe2+/Fe3+ cycling and oxygen vacancies improves the NRR performance. Notably, 5%La-FeMo demonstrates the superior NRR performance (NH3 yield rate: 29.6 µg h-1 mgcat-1, Faradaic efficiency: 5.8%) at -0.8 V (vs. RHE). This work analyzes the influence of the catalyst electronic environment on the NRR performance based on the effect on different valence states of ions on electron transport.

13.
J Colloid Interface Sci ; 677(Pt A): 369-377, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39096705

RESUMO

In the domain of electrocatalytic NO3- reduction (NO3-RR) for the treatment of low-concentration nitrate-containing domestic or industrial wastewater, the conversion of NO3- into NH4+ holds significant promise for resource recovery. Nevertheless, the central challenge in this field revolves around the development of catalysts exhibiting both high catalytic activity and selectivity. To tackle this challenge, we design a two-step hydrothermal combine with carbonization process to fabricate a cobalt-doped Fe-based MOF (MIL-101) catalyst at 800 °C temperatures. The aim was to fully leverage cobalt's demonstrated high selectivity in NO3- electroreduction and enhance activity by promoting electron transfer through the d-band of Fe. The results indicate that the synthesized catalyst inherits multiple active sites from its precursor, with the co-doping process optimized through the topological properties of the MOF. Elemental analysis and oxidation state testing were employed to scrutinize the fundamental characteristics of this catalyst type and comprehend how these features may influence its efficiency. Electrochemical analysis revealed that, even under conditions of low NO3- concentration, the Cox@MIL-Fe catalyst achieved an impressive nitrate conversion rate of 98 % at -0.9 V vs. RHE. NH4+ selectivity was notably high at 87 %, and the by-product NO2- levels remained at a minimal threshold. The Faradaic efficiency for NH4+ reached 74 %, with ammonia yield approaching 0.08 mmol h-1 cm-2. This study furnishes indispensable research data for the design of Fe-based electrocatalysts for nitrate reduction, offering profound insights into the modulation of catalysts to play a pivotal role in the electroreduction of nitrate ions.

14.
J Colloid Interface Sci ; 677(Pt A): 771-780, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39121661

RESUMO

Oxygen reduction reaction (ORR) serves as the foundation for various electrochemical energy storage devices. Fe/NC catalysts are expected to replace commercial Pt/C as oxygen electrode catalysts based on the structural tunability at the atomic level, abundant iron ore reserves and excellent activity. Nevertheless, the lack of durability and low active site density impede its advancement. In this work, a durable catalyst, CuFe/NC, for ORR was prepared by modulating the interfacial composition and electronic structure. The introduction of Cu nanoclusters partially eliminates the Fenton effect from Fe and optimizes the electron structure of FeNx, thereby effectively enhancing the long-term durability and activity. The prepared CuFe/NC exhibits a half-wave potential (E1/2) of 0.90 V and superior stability with a decrease in E1/2 of only 20 mV after 10,000 cycles. The assembled alkaline Zinc-Air batteries (ZABs) with CuFe/NC exhibit an open-circuit potential of 1.458 V. At a current density of 5 mA cm-2, the batteries are capable of operation for 600 h with a stable polarization. This CuFe/NC may promote the practical application of novel and renewable electrochemical energy storage devices.

15.
J Colloid Interface Sci ; 677(Pt A): 800-811, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39121664

RESUMO

Zinc-air batteries, as one of the emerging areas of interest in the quest for sustainable energy solutions, are hampered by the intrinsically sluggish kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), and still suffer from the issues of low energy density. Herein, we report a MOF-on-MOF-derived electrocatalyst, FeCo@NC-II, designed to efficiently catalyze both ORR (Ehalf = 0.907 V) and OER (Ej=10 = 1.551 V) within alkaline environments, surpassing esteemed noble metal benchmarks (Pt/C and RuO2). Systematically characterizations and density functional theory (DFT) calculations reveal that the synergistic effect of iron and cobalt bimetallic and the optimized distribution of nitrogen configuration improved the charge distribution of the catalysts, which in turn optimized the adsorption / desorption of oxygenated intermediates accelerating the reaction kinetics. While the unique leaf-like core-shell morphology and excellent pore structure of the FeCo@NC-II catalyst caused the improvement of mass transfer efficiency, electrical conductivity and stability. The core and shell of the precursor constructed through the MOF-on-MOF strategy achieved the effect of 1 + 1 > 2 in mutual cooperation. Further application to zinc-air batteries (ZABs) yielded remarkable power density (212.4 mW/cm2), long cycle (more than 150 h) stability and superior energy density (∼1060 Wh/kg Zn). This work provides a methodology and an idea for the design, synthesis and optimization of advanced bifunctional electrocatalysts.

16.
Heliyon ; 10(19): e38244, 2024 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-39386859

RESUMO

Mechanical alloying allows obtaining nonequilibrium structures in various systems, often possessing unique properties, including magnetic ones. Considering the unusual structural features of the magnetostrictive Fe-Ga alloy, this approach may be promising for this system. In this work, extensive experimental studies were carried out aimed at studying the features of mechanical alloying of Fe-Ga. The object of the study was the system Fe-20 wt% Ga in which disordered solid solution α-Fe(Ga) is formed. It was shown that high-intensity milling is an effective tool for mechanical alloying of solid-liquid binary system Fe-Ga, but a serious problem is a low powder recovery, less than 50 %. To solve this problem, various process control agents were tested. Their influence on powder recovery, process kinetics, particle size, carbon contamination, and magnetic properties was studied using a large set of techniques such as XRD, SEM, EDS, VSM, LIBS, and others. It has been shown that, based on a combination of factors, the optimal process control agent for this system is ethanol in an amount of 1 wt.

17.
Water Res ; 267: 122548, 2024 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-39357156

RESUMO

Structural Fe in phyllosilicates represents a crucial and potentially renewable reservoir of electron equivalents for contaminants reduction in aquatic and soil systems. However, it remains unclear how in-situ modification of Fe redox states within Fe-bearing phyllosilicates, induced by electron shuttles such as naturally occurring organics, influences the fate of contaminants. Herein, this study investigated the processes and mechanism of Cr(VI) reduction on two typical Fe(II/III)-bearing phyllosilicates, biotite and chlorite, in the presence of cysteine (Cys) at circumneutral pH. The experimental results demonstrated that Cys markedly enhanced the rate and extent of Cr(VI) reduction by biotite/chlorite, likely because of the formation of Cr(V)-organic complexes and consequent electron transfer from Cys to Cr(V). The concomitant production of non-structural Fe(II) (including aqueous Fe(II), surface bound Fe(II), and Cys-Fe(II) complex) cascaded transferring electrons from Cys to surface Fe(III), which further contributed to Cr(VI) reduction. Notably, structural Fe(II) in phyllosilicates also facilitated Cr(VI) reduction by mediating electron transfer from Cys to structural Fe(III) and then to edge-sorbed Cr(VI). 57Fe Mössbauer analysis revealed that cis-coordinated Fe(II) in biotite and chlorite exhibits higher reductivity compared to trans-coordinated Fe(II). The Cr end-products were insoluble Cr(III)-organic complex and sub-nanometer Cr2O3/Cr(OH)3, associated with residual minerals as micro-aggregates. These findings highlight the significance of in-situ produced Fe(II) from Fe(II/III)-bearing phyllosilicates in the cycling of redox-sensitive contaminants in the environment.

18.
J Colloid Interface Sci ; 679(Pt A): 109-118, 2024 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-39357221

RESUMO

Nickel-based catalysts are suitable for water splitting to generate hydrogen. However, the low conductivity and weak stability have always been urgent issues to be addressed in nickel-based catalysts. Fe-doped nickel oxide/nickel phosphide (Fe-NiO/Ni2P) was prepared as a bifunctional electrocatalyst by doping metal and constructing heterogeneous interface. The introduction of Fe contributed to the reinforced interfacial coupling effect of NiO/Ni2P to promote charge transfer and accelerate reaction kinetics. The heterojunction regulated the interfacial charge density between NiO and Ni2P to improve the electronic environment of Ni2+ and enhance conductivity. The O-Fe-P bond at the heterogeneous interface induced the directional transfer of electrons and ensured the structure stability. The synergistic effect of Fe doping and heterogeneous interface increased the adsorption energy of *O and coordinated the adsorption energy of *H, advancing the catalytic performance. Fe-NiO/Ni2P exhibited the overpotential of 242 mV and 141 mV at 10 mA cm-2 for oxygen and hydrogen evolution, respectively.

19.
J Colloid Interface Sci ; 679(Pt A): 132-140, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39357223

RESUMO

Mixed iron-based phosphate Na4Fe3(PO4)2P2O7/C (NFPP) has gradually emerged as a promising cathode material for sodium-ion batteries (SIBs) owing to its affordability and convenient preparation. However, poor electrical conductivity and inadequate sodium-ion diffusion limit the exertion of its electrochemical properties. Herein, a structural modulation strategy based on Cd doping is applied to NFPP to address the above limitations. In situ X-ray diffraction analysis reveals that Cd-doped NFPP (NFCPP) undergoes an incomplete solid-solution reaction driven by Fe2+/Fe3+ redox. Cd doping effectively stabilises the crystal structure, resulting in a minimal 1 % change in unit cell volume during cycling. Density of state calculations indicate that Cd doping reduces the band gap, increases the local electron density and significantly improves electron conductivity. Benefitting from the enhanced electrochemical kinetics and intercalation pseudocapacitance, the optimised Na4Fe2.91Cd0.09(PO4)2P2O7/C (NFCPP@3%) exhibits exceptional rate performance (capacity of 62 mAh/g at 20 C) and ultra-long cycling life (82.7 % after 6000 cycles at 20 C). A full SIB prepared using NFCPP@3% and hard carbon, display a 91 % capacity retention rate at a current density of 130 mA g-1 over 200 cycles. This work demonstrates that doping can effectively enhance electrochemical performance and offers insights into future development of SIBs.

20.
ACS Appl Mater Interfaces ; 16(39): 52814-52823, 2024 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-39358894

RESUMO

Microbiologically influenced corrosion (MIC) poses considerable challenges in various industries, prompting the exploration of advanced materials to mitigate microbial threats. This study successfully synthesized nanoscale vermiculite (VMT) from natural seawater and utilized it as a foundation to integrate magnetic nanoparticles (Fe3O4) and chlorhexidine acetate (CA) for inhibiting MIC. A comprehensive investigation encompassing the synthesis, characterization, and application of these VMT/Fe3O4/CA composites was conducted to evaluate their antimicrobial effectiveness against Escherichia coli, Staphylococcus aureus, and sulfate-reducing bacteria (SRB), demonstrating an efficacy exceeding 99.5%. Moreover, the composite material demonstrated the capability to align with a magnetic field, enabling precise drug targeting and release, thereby facilitating biofilm removal. This research makes a significant contribution to the advancement of intelligent, efficient, and eco-friendly corrosion protection solutions.


Assuntos
Biofilmes , Escherichia coli , Staphylococcus aureus , Biofilmes/efeitos dos fármacos , Staphylococcus aureus/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Antibacterianos/farmacologia , Antibacterianos/química , Clorexidina/farmacologia , Clorexidina/química , Corrosão , Nanopartículas de Magnetita/química , Testes de Sensibilidade Microbiana
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