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1.
Angew Chem Int Ed Engl ; 63(19): e202319796, 2024 May 06.
Article in English | MEDLINE | ID: mdl-38451050

ABSTRACT

The low specific capacity determined by the limited electron transfer of p-type cathode materials is the main obstruction to their application towards high-performance aqueous zinc-ion batteries (ZIBs). To overcome this challenge, boosting multi-electron transfer is essential for improving the charge storage capacity. Here, as a typical heteroaromatic p-type material, we unveil the unique reversible two-electron redox properties of phenoxazine in the aqueous electrolytes for the first time. The second oxidation process is stabilized in the aqueous electrolytes, a notable contrast to its less reversibility in the non-aqueous electrolytes. A comprehensive investigation of the redox chemistry mechanism demonstrates remarkably stable redox intermediates, including a stable cation radical PNO⋅+ characterized by effective electron delocalization and a closed-shell state dication PNO2+. Meanwhile, the heightened aromaticity contributes to superior structural stability during the redox process, distinguishing it from phenazine, which features a non-equivalent hybridized sp2-N motif. Leveraging these synergistic advantages, the PNO electrodes deliver a high capacity of 215 mAh g-1 compared to other p-type materials, and impressive long cycling stability with 100 % capacity retention over 3500 cycles. This work marks a crucial step forward in advanced organic electrodes based on multi-electron transfer phenoxazine moieties for high-performance aqueous ZIBs.

2.
J Chromatogr A ; 1705: 464142, 2023 Aug 30.
Article in English | MEDLINE | ID: mdl-37329652

ABSTRACT

Surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS) is an effective method for detecting of low-mass molecules. In this study, two-dimensional boron nanosheets (2DBs) were fabricated through thermal oxidation etching and coupling liquid exfoliation technologies, and applied as a matrix and selective sorbent for detecting cis-diol compounds by SALDI-TOF MS. The outstanding nanostructure and boric acid active sites of 2DBs endow them with sensitivity for cis-diol compound detection, excellent selectivity, and low background interference for complex samples. The specific in-situ enrichment faculty of the 2DBs as a matrix was investigated by SALDI-TOF MS using glucose, arabinose, and lactose as model analytes. In the presence of 100 -fold more interfering substances, the 2DBs showed high selectivity against cis-diol compounds, and exhibited a better sensitivity and a reduced limit of detection through enrichment treatment than graphene oxide matrices. The linearity, limit of detection (LOD), reproducibility, and accuracy of the method were evaluated under optimized conditions. The results showed that the linear relationships of six saccharides remained in the range of 0.05-0.6 mM with a correlation coefficient r ≥0.98. The LODs of six saccharides were 1 nM (glucose, lactose, mannose, fructose) and 10 nM (galactose, arabinose). Sample-to-sample (n = 6) with relative standard deviations (RSDs) of 3.2% to 8.1% were observed. Recoveries (n = 5) of 87.9-104.6% were obtained at three spiked levels in the milk samples. The proposed strategy promoted the development of a matrix for use with SALDI-TOF MS detection, in which the UV absorption properties and enrichment capabilities of 2DBs were combined.


Subject(s)
Arabinose , Boron , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods , Lactose , Reproducibility of Results , Glucose , Lasers
3.
J Chromatogr A ; 1696: 463963, 2023 May 10.
Article in English | MEDLINE | ID: mdl-37054637

ABSTRACT

Endocrine-disrupting chemicals (EDCs) in environmental water samples, a rapid, sensitive, and high-throughput method should be developed. In this study, an in situ-synthesized composite material of three-dimensional mesoporous graphene (3D-MG) and zirconium-based metal-organic frameworks (MOFs), denoted as MG@UiO-66, was used as both the adsorbent and matrix in surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS) for steroid detection. Both graphene-based materials and MOFs have proven to be ineffective in detecting steroids as a matrix; however, their composites can detect steroids with higher sensitivity and lower interference. After screening different types of MOFs, a composite of UiO-66 and 3D-MG was selected as the new matrix for steroid detection. The combination of 3D-MG and UiO-66 further enhanced the ability of the material to enrich steroids, and reduced the limit of detection (LOD) of steroids. The method was evaluated for linearity, LODs, limit of quantitation (LOQs), reproducibility, and precision under optimized conditions. The results showed that the linear relationships of three steroids are kept in the range of 0-300 nM/L with a correlation coefficient r ≥ 0.97. The LODs and LOQs of the steroids were in the range of 3-15 and 10-20 nM/L, respectively. Recoveries (n = 5) of 79.3-97.2% were obtained at three spiked levels in the blank water samples. This fast and efficient method of using SALDI-TOF MS can be extended to detect the steroids in EDCs in environmental water samples.


Subject(s)
Graphite , Metal-Organic Frameworks , Metal-Organic Frameworks/chemistry , Zirconium , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods , Reproducibility of Results , Steroids , Water
4.
Sci Data ; 10(1): 107, 2023 02 23.
Article in English | MEDLINE | ID: mdl-36823205

ABSTRACT

The irregular shape of mineral particles directly affects the angle of repose, bulk density and flow-properties, and the interaction behaviour between the particles and a contact surface. This paper presents a dataset of spatial data and shape parameters collected from 37 gangue particles and 135 anthracite coal particles, which come from the Shangzhuang Coal Mine. The particle surface models were obtained by a Wiiboox white light raster 3D scanner and Reeyee software. To obtain the scanning surface, each particle was scanned 8 times in different axial rotation directions. The final scanning model was obtained by stacking two scanning surfaces, and the shape parameters, such as length ratio, flatness ratio, and Zingg index, were obtained. This dataset is particularly useful for researchers and engineers who want to investigate the shape of coal and gangue particles or who want to test or benchmark measurement methods concerning the three-dimensional morphology of particles.

5.
Ecotoxicol Environ Saf ; 241: 113742, 2022 Aug.
Article in English | MEDLINE | ID: mdl-35679726

ABSTRACT

The application of plastic mulch films brings convenience to agricultural production, but also causes plastic waste that can be degraded into microplastics (MPs). However, little is known about the fate of plastic waste in agricultural ecosystem under freeze-thaw alternation in middle and high latitudes, as well as in highlands around the world. Whether the release of plasticizers, i.e. phthalate esters (PAEs), under such conditions would pose a potential risk to exposed organisms due to bioaccumulation is also unknown. To fill these data gaps, the agricultural fields in Liaoning of China with typical freeze-thaw alternation was selected as the study area. The transformation of plastic film was demonstrated by simulation freeze-thaw alternating from -30 to 20 â„ƒ. Soil samples were collected to investigate the patterns of MP composition, abundance, and distribution. Concurrently, the concentrations of two PAEs including bis(2-ethylhexyl) phthalate (DEHP) and diethyl phthalate (DEP) in soils were analyzed to provide information on the correlation between MPs abundance and PAEs concentrations as well as potential risks. The results showed that freeze-thaw alternating can accelerate the formation of MPs and release of PAEs from plastic waste. The abundance of MPs was positively correlated with the concentration of PAEs. Soil PAEs ranged from 3268 ± 213-6351 ± 110 µg/kg, indicating that over 40 % of the PAEs were transferred from plastic films to soils. Such residual amounts could pose risk for exposed organisms. Hence, the current study suggested that special concerns should be given to the release plasticizers in plastic waste of agricultural soils.


Subject(s)
Phthalic Acids , Soil Pollutants , China , Dibutyl Phthalate , Ecosystem , Esters , Plasticizers/analysis , Plastics , Soil , Soil Pollutants/analysis
6.
Food Chem ; 339: 128094, 2021 Mar 01.
Article in English | MEDLINE | ID: mdl-33152882

ABSTRACT

The aim of this work is to evaluate the effect of dextrose equivalent (DE) of maltodextrins (MD) on the stability of whey protein and maltodextrin stabilized oil-in-water (o/w) emulsions. Emulsions with DE 15 maltodextrin (MD 15) exhibited better stability under light acidic (pH 6), neutral and alkaline (pH 8-9) conditions, as well as during temperature ramps (20-60 °C). After 15-days of storage, MD 15 emulsion showed increase in polydispersity and decrease in the average droplet size. The apparent viscosity of the emulsions decreased with increasing DE. The shear stresses of all emulsions fitted well with the power law model (R2 > 0.9), while MD 15 showed the most stable k and n indexes. The brightness and whiteness of emulsion decreased with increases in DE. In conclusion, emulsions with MD 15 exhibited better stability, which suggests their good potential for use in the preparation of energy drinks.


Subject(s)
Emulsions/chemistry , Polysaccharides/chemistry , Whey Proteins/chemistry , Temperature , Viscosity
7.
J Environ Sci (China) ; 25(12): 2403-9, 2013 Dec 01.
Article in English | MEDLINE | ID: mdl-24649670

ABSTRACT

Excess nitrogenous compounds are detrimental to natural water systems and to human health. To completely realize autohydrogenotrophic nitrogen removal, a novel 3-dimensional biofilm-electrode reactor was designed. Titanium was electroplated with ruthenium and used as the anode. Activated carbon fiber felt was used as the cathode. The reactor was separated into two chambers by a permeable membrane. The cathode chamber was filled with granular graphite and glass beads. The cathode and cathode chamber were inhabited with domesticated biofilm. In the absence of organic substances, a nitrogen removal efficiency of up to 91% was achieved at DO levels of 3.42 +/- 0.37 mg/L when the applied current density was only 0.02 mA/cm2. The oxidation of ammonium in biofilm-electrode reactors was also investigated. It was found that ammonium could be oxidized not only on the anode but also on particle electrodes in the cathode chamber of the biofilm-electrode reactor. Oxidation rates of ammonium and nitrogen removal efficiency were found to be affected by the electric current loading on the biofilm-electrode reactor. The kinetic model of ammonium at different electric currents was analyzed by a first-order reaction kinetics equation. The regression analysis implied that when the current density was less than 0.02 mA/cm2, ammonium removal was positively correlated to the current density. However, when the current density was more than 0.02 mA/cm2, the electric current became a limiting factor for the oxidation rate of ammonium and nitrogen removal efficiency.


Subject(s)
Ammonium Compounds/chemistry , Bioreactors , Nitrogen/isolation & purification , Water Purification/instrumentation , Electrodes , Oxidation-Reduction
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