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1.
J Environ Sci (China) ; 147: 370-381, 2025 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-39003055

RESUMEN

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.


Asunto(s)
Metales Pesados , Contaminantes del Suelo , Contaminantes Químicos del Agua , Contaminantes Químicos del Agua/metabolismo , Contaminantes Químicos del Agua/análisis , Contaminantes del Suelo/metabolismo , Oxidación-Reducción , Pseudomonas/metabolismo , Manganeso , Hierro/química , Hierro/metabolismo , Suelo/química , Biodegradación Ambiental , Microbiología del Suelo
2.
J Environ Sci (China) ; 148: 88-106, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095204

RESUMEN

In this study, a string of Cr-Mn co-modified activated coke catalysts (XCryMn1-y/AC) were prepared to investigate toluene and Hg0 removal performance. Multifarious characterizations including XRD, TEM, SEM, in situ DRIFTS, BET, XPS and H2-TPR showed that 4%Cr0.5Mn0.5/AC had excellent physicochemical properties and exhibited the best toluene and Hg0 removal efficiency at 200℃. By varying the experimental gas components and conditions, it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg0. Although O2 promoted the abatement of toluene and Hg0, the inhibitory role of H2O and SO2 offset the promoting effect of O2 to some extent. Toluene significantly inhibited Hg0 removal, resulting from that toluene was present at concentrations orders of magnitude greater than mercury's or the catalyst was more prone to adsorb toluene, while Hg0 almost exerted non-existent influence on toluene elimination. The mechanistic analysis showed that the forms of toluene and Hg0 removal included both adsorption and oxidation, where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr3+ + Mn3+/Mn4+ ↔ Cr6+ + Mn2+, which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process, and even the CrMn1.5O4 spinel structure could provide a larger catalytic interface, thus enhancing the adsorption/oxidation of toluene and Hg0. Therefore, its excellent physicochemical properties make it a cost-effective potential industrial catalyst with outstanding synergistic toluene and Hg0 removal performance and preeminent resistance to H2O and SO2.


Asunto(s)
Contaminantes Atmosféricos , Mercurio , Óxidos , Tolueno , Tolueno/química , Óxidos/química , Contaminantes Atmosféricos/química , Mercurio/química , Coque , Catálisis , Cromo/química , Adsorción , Manganeso/química , Compuestos de Manganeso/química , Modelos Químicos
3.
J Environ Sci (China) ; 149: 616-627, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181672

RESUMEN

HONO is a critical precursor of •OH, but its sources are controversial due to its complex formation mechanism. This study conducted comprehensive observations in Zhengzhou from April 26 to May 11, 2022. Low NOx concentrations were observed during the Covid epidemic period (EP) (10.4 ± 3.0 ppb), compared to the pre-epidemic period (PEP) (12.5 ± 3.8 ppb). The mean HONO concentration during EP (0.53 ± 0.34 ppb) was 0.09 ppb lower than that during PEP (0.62 ± 0.53 ppb). The decrease in HONO concentration during EP came mainly at night due to the reduction in the direct emission (Pemi) (0.03 ppb/hr), the homogeneous reaction between •OH and NO (POH+NO) (0.02 ppb/hr), and the heterogeneous conversion of NO2 on the ground (0.01 ppb/hr). Notably, there was no significant change in daytime HONO concentration. The daytime HONO budget indicated that the primary HONO sources during PEP were the nitrate photolysis (Pnitrate), followed by the POH+NO, Pemi, the photo-enhanced reaction of NO2 on the ground (Pground+hv) and aerosol surface (Paerosol+hv). The primary HONO sources were Pnitrate, POH+NO, Pemi, and Paerosol+hv during EP, respectively. The missing source has a high correlation with solar radiation, there might be other photo-related HONO sources or the contributions of photosensitized reactions were underestimated. In the extremely underestimated cases, HONO production rates from the Pnitrate, Pground+hv, and Paerosol+hv increased by 0.17, 0.10, and 0.10 ppb/hr during PEP, 0.23, 0.13, and 0.16 ppb/hr during EP, and Pnitrate was still the primary source during both PEP and EP.


Asunto(s)
Contaminantes Atmosféricos , COVID-19 , COVID-19/epidemiología , China/epidemiología , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , SARS-CoV-2 , Pandemias , Ciudades , Humanos
4.
J Environ Sci (China) ; 150: 692-703, 2025 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-39306440

RESUMEN

Nitrogen oxides (NOx) are crucial in tropospheric photochemical ozone (O3) production and oxidation capacity. Currently, the widely used NOx measurement technique is chemiluminescence (CL) (CL-NOx), which tends to overestimate NO2 due to atmospheric oxidation products of NOx (i.e., NOz). We developed and characterized a NOx measurement system using the cavity attenuated phase shift (CAPS) technique (CAPS-NOx), which is free from interferences with nitrogen-containing species. The NOx measured by the CAPS-NOx and CL-NOx analyzers were compared. Results show that both analyzers showed consistent measurement results for NO, but the NO2 measured by the CAPS-NOx analyzer (NO2_CAPS) was mostly lower than that measured by the CL-NOx analyzer (NO2_CL), which led to the deviations in O3 formation sensitivity regime and Ox (= O3 + NO2) sources (i.e., regional background and photochemically produced Ox) determined by the ozone production efficiencies (OPE) calculated from NO2_CL and NO2_CAPS. Overall, OPE_CL exceeded OPE_CAPS by 18.9%, which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL, as compared to calculations using OPE_CAPS. During the observation period, days dominated by regional background Ox accounted for 46% and 62% when determined using NO2_CL and NO2_CAPS, respectively. These findings suggest that the use of the CL-NOx analyzer tends to underestimate both the VOCs-limited regime and the regional background Ox dominated days. The newly built CAPS-NOx analyzer here can promote the accurate measurement of NO2, which is meaningful for diagnosing O3 formation regimes and Ox sources.


Asunto(s)
Contaminantes Atmosféricos , Monitoreo del Ambiente , Óxidos de Nitrógeno , Ozono , Óxidos de Nitrógeno/análisis , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Monitoreo del Ambiente/instrumentación , Ozono/análisis , Atmósfera/química
5.
Small Methods ; : e2400264, 2024 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-39248649

RESUMEN

Cation deficiency tuning is a central issue in thin-film epitaxy of functional metal oxides, as it is typically more difficult than anion deficiency tuning, as anions can be readily supplied from gas sources. Here, highly effective internal deficiency compensation of Ru cations is demonstrated for Ca2RuO4 epitaxial films based on diffusive transfer of metal cations in the A2BO4 Ruddlesden-Popper lattice from solid-phase cation sources. Through detailed structural characterization of Ca2RuO4/LaAlO3 (001) thin films grown with external cation sources by solid-phase epitaxy, the occurrence of intercalation-like, interstitial diffusion of La cations (from the substrates) in the A2BO4 structure is revealed, and that of Ru cations is also suggested. Relying on the interstitial-type diffusion, an optimized Ru deficiency compensation method, which does not induce the formation of Can +1RunO3 n +1 Ruddlesden-Popper impurity phases with higher n, is proposed for Ca2RuO4 epitaxial films. In the Ca2RuO4/LaAlO3 (001) thin films grown with Ru deficiency compensation, record-high resistivity values (102-10-1 Ω cm) and a large (more than 200 K) increase in the temperature range of the nonlinear transport properties are demonstrated by transport measurements, demonstrating the possible advantages of this method in the control of the current-induced quantum phase transition of Ca2RuO4.

6.
Artículo en Inglés | MEDLINE | ID: mdl-39261285

RESUMEN

The magnetocaloric effect (MCE) is currently intensively investigated in various rare earths (RE)-containing magnetic solids, not only for developing appropriate magnetocaloric materials (MCMs) for cryogenic magnetic cooling but also for deepening our understanding into the inherent physical properties of these materials. Here, we provide a systematic experimental investigation into a series of new RE2CuTiO6 (RE = Dy, Ho, Er) double-perovskite (DP) oxides regarding the structural and magnetic properties, especially for their cryogenic MCE and magnetic-phase transition (MPT). All of these RE2CuTiO6 oxides crystallize in a B-site-ordered hexagonal DP-type structure with the symmetry of the crystallographic space group P6̅m2. These DP oxides exhibit magnetic ordering, with MPT temperatures of approximately 2.7, 2.2, and 2.7 K for Dy2CuTiO6, Ho2CuTiO6, and Er2CuTiO6, respectively. The magnetocaloric performances of the RE2CuTiO6 DP oxides were characterized by the peak values of magnetic entropy change, the temperature-averaged magnetic entropy change (5K-lift), and relative cooling powers. These magnetocaloric parameters were deduced to be 18.7/17.9 J/kgK and 298.2 J/kg for Dy2CuTiO6, 12.5/12.2 J/kgK and 273.9 J/kg for Ho2CuTiO6, and 13.8/12.9 J/kgK and 188.4 J/kg for Er2CuTiO6 under a magnetic field change of 0-5 T. These values are comparable to those of most reported RE-containing magnetocaloric materials, indicating that these RE2CuTiO6 DP oxides are promising candidates for cryogenic magnetic cooling applications.

7.
Chemosphere ; 364: 143280, 2024 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-39243899

RESUMEN

This paper addresses the influence of bubbling flow and service life of the Ti|Ti-Ru-Ir-oxides anode during the electrosynthesis of HClO in a laboratory-scale filter-press-type electrolyzer. The electrolyzer was assembled in a flow plant in recirculation mode. Polarization curves in rotating disk electrode (RDE) revealed the coexistence of the oxygen evolution reaction (OER) during HClO electrosynthesis in diluted chloride solutions (containing 35 mM NaCl at pH 3). CFD simulations of the two-phase (O2-H2O) flow were obtained by solving simultaneously the Navier-Stokes and charge conservation equations using a finite element method code. The O2-H2O simulations show the efficient gas release in the electrolyzer provoked by the continuous phase (H2O) inertia and the well-engineered cell design. The moderated O2 dispersion caused a quasi-homogeneous current distribution along the anode. However, the current efficiency during HClO electrosynthesis gave values of ∼32% provoked by the OER on the anode. The HClO accumulations (from 3.02 to 6.64 mM) showed excellent agreement with CFD simulations. The accelerated life tests revealed that the Ti | Ti-Ru-Ir-oxides anode has a lifetime of at least 26 years during the HClO electrosynthesis in diluted chloride solutions.

8.
J Colloid Interface Sci ; 678(Pt B): 763-771, 2024 Sep 07.
Artículo en Inglés | MEDLINE | ID: mdl-39265346

RESUMEN

The integration of ternary metal oxides into carbon materials is anticipated to significantly boost the electrochemical performance of supercapacitor electrodes. This article synthesized carbon nanotubes (CNT)/(NiMn)Co2O4 composite materials using a straightforward hydrothermal method and subsequently prepared composite thin films of CNT/P-(NiMn)Co2O4@NGQD by phosphating and incorporating nitrogen-doped graphene quantum dots (NGQD). These films served as the functional electrode material for supercapacitors, enhancing their performance capabilities. The specific capacity of CNT/P-(NiMn)Co2O4@NGQD was measured at 2172.0 F g-1 at a current density of 1 A g-1, maintaining a capacitance of 1954.0 F g-1 at 10 A g-1, thus demonstrating excellent rate performance. Electrochemical impedance spectroscopy (EIS) further revealed enhancements in electrolyte flow dynamics and capacitance behavior post-NGQD introduction. The energy density of the composite material reached 94.4 Wh kg-1 at power density of 800 W kg-1, demonstrating superior electrochemical performance. The enhancement in these electrochemical properties is attributed to the high specific surface area and active sites of CNT/P-(NiMn)Co2O4@NGQD films, along with the synergistic effects of NGQD and metal ions facilitating rapid electrons and charge transfer. This work provides new insights into developing high-performance supercapacitors.

9.
Artículo en Inglés | MEDLINE | ID: mdl-39221977

RESUMEN

Magnetic materials featuring triangular arrangements of spins are frequently investigated as platforms hosting magnetic frustration. Hexagonal perovskites with ordered vacancies serve as excellent candidates for two-dimensional triangular magnetism due to the considerable separation of the magnetic planes. In this work, the effects of chemical pressure on the ferromagnetic ground state of Ba2La2NiW2O12 by substitution of Ba2+ with Sr2+ to produce Sr2La2NiW2O12 are investigated. The two materials are characterized using synchrotron-based XRD, XANES and EXAFS in addition to magnetometry in order to correlate their crystal structures and magnetic properties. Both materials form in space group R3, yet as a result of the enhanced bending of key bond angles due to the effects of chemical pressure, the TC value of the magnetic Ni2+ sublattice is reduced from ∼6 K in Ba2La2NiW2O12 to 4 K in Sr2La2NiW2O12.

10.
Small ; : e2405168, 2024 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-39235421

RESUMEN

Vanadium (V)-based oxides have garnered significant attention as cathode materials for aqueous zinc-ion batteries (AZIBs) due to their multiple valences and high theoretical capacity. However, their sluggish kinetics and low conductivity remain major obstacles to practical applications. In this study, Mo-doped V2O3 with oxygen vacancies (OVs, Mo-V2O3-x@NC) is prepared from a Mo-doped V-metal organic framework. Ex situ characterizations reveal that the cathode undergoes an irreversible phase transformation from Mo-V2O3-x to Mo-V2O5-x·nH2O and serves as an active material exhibiting excellent Zn2+ storage in subsequent charge-discharge cycles. Mo-doped helps to further improve cycling stability and increases with increasing content. More importantly, the synergistic effect of Mo-doped and OVs not only effectively reduces the Zn2+ migration energy barrier, but also enhances reaction kinetics, and electrochemical performance. Consequently, the cathode demonstrates ultrafast electrochemical kinetics, showing a superior rate performance (190.9 mAh g-1 at 20 A g-1) and excellent long-term cycling stability (147.9 mAh g-1 at 20 A g-1 after 10000 cycles). Furthermore, the assembled pouch cell exhibits excellent cycling stability (313.6 mAh g-1 at 1 A g-1 after 1000 cycles), indicating promising application prospects. This work presents an effective strategy for designing and fabricating metal and OVs co-doped cathodes for high-performance AZIBs.

11.
Small ; : e2406068, 2024 Sep 02.
Artículo en Inglés | MEDLINE | ID: mdl-39223867

RESUMEN

Electrochemical upcycling of end-of-life polyethylene terephthalate (PET) using renewable electricity offers a route to generate valuable chemicals while processing plastic wastes. However, it remains a huge challenge to design an electrocatalyst with reliable structure-property relationships for PET valorization. Herein, spinel Co3O4 with rich oxygen vacancies for improved activity toward formic acid (FA) production from PET hydrolysate is reported. Experimental investigations combined with theoretical calculations reveal that incorporation of VO into Co3O4 not only promotes the generation of reactive hydroxyl species (OH*) species at adjacent tetrahedral Co2+ (Co2+ Td), but also induces an electronic structure transition from octahedral Co3+ (Co3+ Oh) to octahedral Co2+ (Co2+ Oh), which typically functions as highly-active catalytic sites for ethylene glycol (EG) chemisorption. Moreover, the enlarged Co-O covalency induced by VO facilitates the electron transfer from EG* to OH* via Co2+ Oh-O-Co2+ Td interaction and the following C─C bond cleavage via direct oxidation with a glyoxal intermediate pathway. As a result, the VO-Co3O4 catalyst exhibits a high half-cell activity for EG oxidation, with a Faradaic efficiency (91%) and productivity (1.02 mmol cm-2 h-1) of FA. Lastly, it is demonstrated that hundred gram-scale formate crystals can be produced from the real-world PET bottles via two-electrode electroreforming, with a yield of 82%.

12.
Natl Sci Rev ; 11(10): nwad296, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-39301067

RESUMEN

Spin texture in k-space is a consequence of spin splitting due to strong spin-orbit coupling and inversion symmetry breaking. It underlies fertile spin transport phenomena and is of crucial importance for spintronics. Here, we observe the spin texture in k-space of nominally centrosymmetric SrIrO3 grown on NdGaO3 (110) substrates, using non-linear magnetotransport measurements. We demonstrate that the spin texture is not only induced by the interface, which inherently breaks the inversion symmetry in strong spin-orbit coupled SrIrO3 films, but also originates from the film bulk. Structural analysis reveals that thicker SrIrO3 films exhibit a strain gradient, which could be considered as a continuous change in the lattice constant across different layers and breaks the inversion symmetry throughout the entire SrIrO3 films, giving rise to the spin texture in k-space. First-principles calculations reveal that the strain gradient creates large spin-splitting bands, inducing the spin texture with anisotropy, which is consistent with our experimental observations. Our results offer an efficient method for inducing the spin textures in k-space.

13.
Environ Pollut ; : 124984, 2024 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-39303934

RESUMEN

The self-cementation characteristics of arsenic (As)-contaminated soil were comprehensively investigated in this study. Different non-thermal plasma-irradiated binary (hydro)oxides of polyvalent ferromanganese (poly-Fe-Mn) were synthesized and exploratorily dispersed to soil samples to activate solidification and stabilization during the self-cemented process. The maximum compressive strength of 56.35 MPa and the lowest leaching toxicity of 0.004 mg/L were obtained in the proof test under optimal conditions (i.e., the mass ratio of the poly-Fe-Mn to the soil sample of 0.05; the mass ratio of the composite alkali activator (NaOH + CaO) to the soil sample of 0.25; the mass ratio of CaO to NaOH of 1.5; the mass ratio of the DI water to the binder of 0.515). The composite alkaline activator primarily contributed to the strength formation of the self-cemented matrix while the poly-Fe-Mn significantly influenced the reduction of the As-leaching toxicities. The poly-Fe-Mn maintained diffusion-controlled polycondensation and strengthened the nucleation process during self-cementation. The amount of water and the dosage of poly-Fe-Mn caused an interactive influence on the self-cemented solidification of contaminated soils. The solidified samples with poly-Fe-Mn exhibited better thermal decomposition than their counterparts, reflecting the enhancement of poly-Fe-Mn to the matrix. Some minerals including C-S-H, kaolinite, gehlenite, diopside sodian, augite, and albite were matched in the samples, directly demonstrating the geopolymerization-steered self-cementation of the As soil. The employment of poly-Fe-Mn not only reinforced the immobilization of As pollutants in the matrix but also induced the self-cementation of soils by intensifying the composite alkaline-activated geopolymerization kinetics.

14.
Angew Chem Int Ed Engl ; : e202415997, 2024 Sep 21.
Artículo en Inglés | MEDLINE | ID: mdl-39305188

RESUMEN

The pressing demand for large-scale energy storage solutions has propelled the development of advanced battery technologies, among which zinc-ion batteries (ZIBs) are prominent due to their resource abundance, high capacity, and safety in aqueous environments. However, the use of manganese oxide cathodes in ZIBs is challenged by their poor electrical conductivity and structural stability, stemming from the intrinsic properties of MnO2 and the destabilizing effects of ion intercalation. To overcome these limitations, our research delves into atomic-level engineering, emphasizing quantum spin exchange interactions (QSEI). These essential for modifying electronic characteristics, can significantly influence material efficiency and functionality. We demonstrate through density functional theory (DFT) calculations that enhanced QSEI in manganese oxides broadens the O p band, narrows the bandgap, and improves both proton adsorption and electron transport. Empirical evidence is provided through the synthesis of Ru-MnO2 nanosheets, which display a marked increase in energy storage capacity, achieving 314.4 mAh g-1 at 0.2 A g-1 and maintaining high capacity after 2000 cycles. Our findings underscore the potential of QSEI to enhance the performance of TMO cathodes in ZIBs, pointing to new avenues for advancing battery technology.

15.
J Colloid Interface Sci ; 678(Pt C): 608-618, 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39305628

RESUMEN

Unstable cathode/electrolyte interphase and severe interfacial side reaction have long been identified as the main cause for the failure of layered oxide cathode during fast charging and long-term cycling for rechargeable sodium-ion batteries. Here, we report a superionic conductor (Na3V2(PO4)3, NVP) bonding surface strategy for O3-type layered NaNi1/3Fe1/3Mn1/3O2 (NFM) cathode to suppress electrolyte corrosion and near-surface structure deconstruction, especially at high operating potential. The strong bonding affinity at the NVP/NFM contact interface stabilizes the crystal structure by inhibiting surface parasitic reactions and transition metal dissolution, thus significantly improving the phase change reversibility at high desodiation state and prolonging the lifespan of NFM cathode. Due to the high-electron-conductivity of NFM, the redox activity of NVP is also enhanced to provide additional capacity. Therefore, benefiting from the fast ion transport kinetics and electrochemical Na+-storage activity of NVP, the composite NFM@NVP electrode displays a high initial coulombic efficiency of 95.5 % at 0.1 C and excellent rate capability (100 mAh g-1 at 20 C) within high cutoff voltage of 4.2 V. The optimized cathode also delivers preeminent cyclic stability with ∼80 % capacity retention after 500 cycles at 2 C. This work sheds light on a facile and universal strategy on improving interphase stability to develop fast-charging and sustainable batteries.

16.
Micron ; 187: 103718, 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39305702

RESUMEN

Two-dimensional (2D) magnets, especially strongly correlated 2D transition-metal perovskite oxides, have attracted significant attention due to their intriguing electromagnetic properties for potential applications in spintronic devices. Potentially electron magnetic circular dichroism (EMCD) under zone axis conditions can provide three-dimensional components of magnetic moments in 2D materials, but the collection efficiency and the signal-to-noise ratio for out-of-plane (OOP) components is limited due to the limited collection angle. Here we conducted a comprehensive computational simulation to optimize the experimental setting of EMCD for detecting the OOP components of magnetic moments in three beam conditions (3BCs) on 2D perovskite oxides La1-xSrxMnO3 (LSMO) in a TEM. The key parameters are sample thickness, accelerating voltage, Sr doping concentration, collection semi-angle and position, and sample orientation including systematic reflections excited and tilt angle. Our simulation results demonstrate that the relative dynamical diffraction coefficients of Mn OOP EMCD of LaMnO3 with a thickness ranging from 1 unit cell (uc) to 4 uc can be optimized in a 3BC with (110) systematic reflections excited and a relatively large collection semi-angle of 19 mrad at the relatively low accelerating voltage of 80 kV. In most cases, the relative dynamic diffraction coefficients for La1-xSrxMnO3 with the thickness ranging from 1 uc to 4 uc decrease with the increase of the Sr doping concentrations. The optimal tilt angle from a zone axis to a 3BC is 18° for the cases of the LSMO thickness of 2 uc, 3 uc and 4 uc, and 22° for the monolayer LSMO. Our work provides the theoretical simulation foundation for optimized EMCD experiments for measuring OOP components of magnetic moments in 2D transition-metal perovskite oxides.

17.
J Hazard Mater ; 480: 135864, 2024 Sep 17.
Artículo en Inglés | MEDLINE | ID: mdl-39298968

RESUMEN

The distribution characteristics of Cr(VI) species in contaminated soil is crucial for soil remediation; however, there is currently a lack of methods for analysing anionic Cr(VI) species in soil. This study has developed a novel sequential extraction method for speciation of Cr(VI) and Cr(III). Besides extraction experiments, simulated chromium species were prepared to verify the presence of proposed chromium species. The results show that Cr(VI) species in soil can be categorized into water-soluble Cr(VI), electrostatically adsorbed Cr(VI), Cr(VI) specifically adsorbed by minerals containing exchangeable Ca2+, Cr(VI) specifically adsorbed by hydrous metal oxides, calcium chromate Cr(VI) and stable complexed adsorption Cr(VI). These Cr(VI) species can be selectively extracted by specific solutions through ion exchange or weak acid dissolution. The most stable Cr(VI) species is Cr(VI) complexed by hydrous iron oxides through bidentate ligand binding; only by dissolution of hydrous iron oxides can this Cr(VI) species be leached. The distribution of Cr(VI) species is closely linked to particular soil compositions including exchangeable Ca2+ and hydrous iron oxides which determinate the Cr(VI) adsorption in soil. Cr(III) species comprise Fe-Cr coprecipitate hydroxides Cr(III), Fe-Mn oxide-bound Cr(III), organic matter-bound Cr(III) and residual Cr(III). Their distribution depends on the types of reductants present in the soil.

18.
J Hazard Mater ; 479: 135748, 2024 Nov 05.
Artículo en Inglés | MEDLINE | ID: mdl-39243540

RESUMEN

A novel nitrate-dependent manganese (Mn) redox strain was isolated and identified as Dechloromonas sp.YZ8 in this study. The growth conditions of strain YZ8 were optimized by kinetic experiments. The nitrate (NO3--N) removal efficiency was 100.0 % at 16 h at C/N of 2.0, pH of 7.0, and Mn(II) or Mn(IV) addition of 10.0 or 500.0 mg L-1, along with an excellent Mn redox capacity. Transmission electron microscopy supported the Mn redox process inside and outside the cells of strain YZ8. When strain YZ8 was exposed to different concentrations of copper ion (Cu(II)), it turned out that moderate amounts of Cu(II) increased microbial activity and metabolic activities. Moreover, it was discovered that the appropriate amount of Cu(II) promoted the conversion of Mn(IV) and Mn(II) to Mn(III) and improved electron transfer capacity in the Mn redox system, especially the Mn redox process dominated by Mn(IV) reduction. Then, δ-MnO2 and bio-manganese oxides (BMO) produced during the reaction process have strong adsorption of Cu(II). The surface valence changes of δ-MnO2 before and after the reaction and the production of BMO, Mn(III)-rich intermediate black manganese ore (Mn3O4), and Mn secondary minerals together confirmed the Mn redox pathway. The study provided new insights into the promotion mechanism and immobilization effects of redox-coupled denitrification of Mn in groundwater under Cu(II) stress.


Asunto(s)
Cobre , Desnitrificación , Manganeso , Nitratos , Oxidación-Reducción , Cobre/química , Desnitrificación/efectos de los fármacos , Nitratos/metabolismo , Nitratos/química , Manganeso/química , Manganeso/metabolismo , Contaminantes Químicos del Agua/metabolismo , Contaminantes Químicos del Agua/toxicidad , Contaminantes Químicos del Agua/química , Rhodocyclaceae/metabolismo , Biodegradación Ambiental
19.
Small Methods ; : e2400481, 2024 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-39252662

RESUMEN

Orthorhombic perovskite GdFeO3 nanostructures are promising materials with multiferroic properties. In this study, a new low-temperature plasma-assisted approach is developed via dual anodic dissolution of solid metallic precursors for the preparation of perovskite GdFeO3 nanoparticles (NPs) that can be collected both as colloids as well as deposited as a thin film on a substrate. Two solid metallic foils of Gd and Fe are used as precursors, adding to the simplicity and sustainability of the method. The formation of the orthorhombic perovskite GdFeO3 phase is supported by high-resolution transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and Raman measurements, while a uniform elemental distribution of Gd, Fe, and O is confirmed by energy dispersive X-ray spectroscopy, proving the successful preparation of ternary compound NPs. The magnetic properties of the NPs show zero remnant magnetization typical of antiferromagnetic materials, and saturation at high fields that can be caused by spin interaction between Gd and Fe magnetic sublattices. The formation mechanism of ternary compound NPs in this novel plasma-assisted method is also discussed. This method is also modified to demonstrate the direct one-step deposition of thin films, opening up opportunities for their future applications in the fabrication of magnetic memory devices and gas sensors.

20.
Nanomaterials (Basel) ; 14(17)2024 Aug 23.
Artículo en Inglés | MEDLINE | ID: mdl-39269040

RESUMEN

The pseudocapacitive effect can improve the electrochemical lithium storage capacity at high-rate current density. However, the cycle stability is still unsatisfactory. To overcome this issue, a multivalent oxide with a carbon coating represents a plausible technique. In this work, a CuO-Cu2O@C composite has been constructed by a one-step bilayer salt-baking process and utilized as anode material for lithium-ion batteries. At a current density of 2.0 A g-1, the as-prepared composite delivered a stable discharge capacity of 431.8 mA h g-1 even after 600 cycles. The synergistic effects of the multivalence, the pseudocapacitive contribution from copper, and the carbon coating contribute to the enhanced electrochemical lithium storage performance. Specifically, the existence of cuprous suboxide improves the electrochemical conductivity, the pseudocapacitive effect enhances the lithium storage capacity, and the presence of carbon ensures cycle stability. The testing results show that CuO-Cu2O@C composite has broad application prospects in portable energy storage devices. The present work provides an instructive precedent for the preparation of transition metal oxides with controllable electronic states and excellent electrochemical performance.

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