Analytical Methods
·
2023
·Vol. 15
·期 36
·4758-4766
·
IF 3.1
Qiang Wang,Yulin Nie,Zhibin Wu,Yuan Yang
We developed an approach of magnetic dispersive solid-phase extraction (MSPE) based on magnetic graphene nanocomposite rGO/Fe3O4 for the determination of trace Sb(III) and Sb(V) using inductively coupled plasma mass spectrometry (ICP-MS). Scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared spectroscopy (FT-IR) were used to characterize the sorbent. The adsorption behavior of Sb(III) and Sb(V) on rGO/Fe3O4 was investigated. The results showed that the adsorption capacity of Sb(V) was nearly zero at pH = 9, while Sb(III) could be well adsorbed on rGO/Fe3O4. The magnetic SPE parameters including pH, adsorbent dosage, eluent type, and volume were optimized. The detection limit of Sb(III) under ideal conditions was 6 ng L−1, and the relative standard deviation was 7.6% (c = 1 g L−1, n = 7). The technique was used to identify Sb(III) at trace levels in environmental water samples, and its validity was examined by recovery experiments and the examination of an approved reference material.
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JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Jianhui Li,Zaisheng Wang
Trimethyl borate (TMB) has been identified as electrolyte additive to suppress self-discharge for high voltage layered lithium-rich oxide cathode (LRO) for lithium ion batteries in our previous work. To expand pervious findings, its derivatives, triethyl borate (TEB) and tripropyl borate (TPB) with increased alkyl chains, have been considered as electrolyte additives to mitigate self-discharge behavior of LRO cathode for lithium ion batteries and we make a contrast to explain which one is better and why is better. It is found that fully charged (4.8 V, vs. Li/Li + ) LRO cathode suffers severe self-discharged issue upon storage in standard (STD) electrolyte (1 mol L −1 LiPF 6 -EC/EMC/DEC (3:5:2, in weight)). In contrast, this detrimental self-discharge behavior of LRO cathode at high voltage can be effectively depressed by introducing TEB or TPB into the electrolyte system. Combinations of electrochemical methods and multi spectroscopy techniques have been employed to evaluate effects of TEB and TPB on the LRO cathode surface . They reveal that the B–O and B–F bonds species in the film formed by TEB and TPB prevents electrolyte decomposition and protects LRO from structure transformation. These species in the film formed by TEB is much more than TPB, which explains the better effect for TEB.
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RSC Advances
·
2018
·Vol. 8
·期 38
·21480-21494
·
IF 2.936
Ruihong Meng,Tan Chen,Yaxin Zhang,Wenjing Lu,Yanting Liu,Tianchu Lu,Yanjun Liu,Hongtao Wang
In this work, a low-cost and available material for use as a permeable reactive barrier (PRB) to prevent vanadium in groundwater from leaking into river water was developed. Three modified biochars were prepared from available corn straw pretreated with CsCl, Zn(II), and Zr(IV) to enhance ion exchange capacity (IEC) and specific surface area, and were designated as Cs-BC, Zn-BC, and Zr-BC, respectively. These materials were characterized via IEC, N2 adsorption–desorption, Fourier-transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD) analyses. The Langmuir isotherm model could be applied for the best fit for the adsorption data of Cs-BC and Zr-BC, indicating that vanadium(V) sorption occurred in a monolayer. The vanadium(V) adsorption capacities of Cs-BC, Zn-BC, and Zr-BC were 41.07, 28.46, and 23.84 mg g−1, respectively, which were 3.22–5.55 times higher than that of commercial activated carbon (AC) (7.40 mg g−1), probably because of their higher IECs and specific surface areas after modification. In addition, no heavy metal leaching was found from the modified biochars during the adsorption processes when pH > 2. According to the FTIR and XRD patterns, the adsorption mechanism of Cs-BC and Zr-BC was ion exchange, whereas for Zn-BC, it was mainly surface precipitation and electrostatic attraction. The adsorption of vanadium(V) onto the modified biochars was independent of pH in the range of 4.0 to 8.0. Furthermore, the removal efficiency of the vanadium(V) in real contaminated groundwater from the catchment of the Chaobei River by Zn-BC reached 100% at a dose of 4 g L−1. Hence, modified biochars are promising PRB filling materials for removing vanadium(V) from contaminated groundwater.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Li Liu,Qianqian Wei,Yeqing Lan,Cheng Chen
Efficient purification of the wastewater containing organoarsenic by activated peroxymonosulfate (PMS) usually faces with a great challenge because the degradation of organoarsenic is coupled with the release of its byproduct As(V). Heterogeneous catalysts with catalytic and adsorption functions show great potential in activating PMS for the degradation of organoarsenic and the removal of secondary inorganic arsenic. In this study, Co-CeMnO was designed and fabricated to realize simultaneous elimination of p -arsanilic ( p -ASA) and As(V) in Co-CeMnO (0.2 g/L)/PMS (0.25 mM) system, in which 50 µM p -ASA was almost completely degraded within 5 min and approximately 100% of the produced As(V) was removed within 30 min. The rate constant of the pseudo-first-order kinetics for the p -ASA degradation by PMS mediated with Co-CeMnO was high up to 0.65 min −1 , approximately 6.5 times higher than that in the system of CeMnO/PMS. It was revealed that SO 4 •− , • OH and 1 O 2 acted as the main oxidant species responsible for the oxidation of organics and As(III), and the surface −OH of Co-CeMnO led to the adsorption of As(V) via ion exchange. The excellent reusability and stability of Co-CeMnO was verified by five cycles with high removal efficiencies of p -ASA (>92% within 10 min) and arsenic (>98% within 90 min) and low leached metal ion concentrations (Co ions < 0.27 mg/L; Mn ions < 0.15 mg/L; Ce ions ≈ 0). Under the condition of initial pH 5, p -ASA was degraded completely and over 98% of total arsenic was adsorbed in different water matrices, indicating the practical application potential of Co-CeMnO/PMS system. Thus, the present study provided a reliable PMS activation strategy by constructing bifunctional catalysts to achieve satisfactory treatment of the wastewater containing p -ASA.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Zhicheng Xu,Jin Xiong,Yuran Li,Junxiang Guo,Bin Wang,Tingyu Zhu
For industrial flue gas purification at medium and low temperatures, it is highly necessary to promote the denitrification activity of V-based catalysts in a SO2 atmosphere. Transition metals (Ce, Co, Fe, and Mn) are used to modify V/Ti catalysts to improve SO2 resistance with ammonium bisulfate deposition on the catalysts. Sulfation on Ce with less ammonium bisulfate deposition considerably improves the SO2 resistance of V1Ce5/Ti, and stable sulfation on TiO2 promoted by Co provides additional Brønsted acid sites for V1Co5/Ti to reduce the deactivation. Serious sulfation on V1Mn5/Ti with large ammonium bisulfate deposition on V1Fe5/Ti causes deeper deactivation. The formation mechanism of ammonium bisulfate on active metal sites and TiO2 carriers has been clarified. SO2 is adsorbed on V sites and transition metal sites followed by oxidation and ammoniation or adsorbed on TiO2 carriers followed by ammoniation and oxidation. The first pathway is more dominant than the second pathway in the presence of O2 with the co-oxidation of SO2 by O2 and lattice oxygen. The initial formation temperature and stable temperature of dominant intermediates were determined by in situ DRIFTS. SO2 adsorbed on TiO2 carriers is oxidized by V sites above 170 °C to form a tridentate sulfate, while SO2 adsorbed on transition metal sites is initially oxidized by transition metal sites above 50 °C to form monodentate and bidentate sulfates, as well as competitively oxidized by V sites above 170 °C to form tridentate sulfates. The selective adsorption of SO2 on transition metal sites or TiO2 carriers and the competitive oxidation of SO2 by transition metal sites and V sites provide a synergistic effect between V sites and transition metal sites to reduce ammonium sulfate deposition and release more active sites. These findings provide theoretical guidance to design and prepare V-based catalysts with high denitrification activity in the presence of SO2.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Lian Xia,Andi Huang,Xiaojuan Niu,Zhen Wu,Yue Tang,Jianli Zhou,Yuangen Wu
The detrimental growth of water pollutants such as heavy metals has become a life-threatening problem in the modern era. Challenges remain in the development of rapid and accurate methods for detecting pentavalent arsenic [As(V)] in environmental water. The octahedral Mn 3 O 4 nanoparticles (NPs) did not display excellent laccase-mimicking catalytic activity, whereas the adsorbed As(V) on the surface significantly enhanced the catalytic activity. Meanwhile, the quinone imine generated from the substrates 2,4-dichlorophenol (2,4-DP) and 4-aminoantipyrine (4-AAP) catalyzed by octahedral Mn 3 O 4 NPs further quenched the carbon dots fluorescence. Thus, it is possible to establish a fast and accurate dual-mode sensor for detecting As(V). The developed dual-mode method of As(V) detection has good sensitivity and selectivity. The limit of detection for As(V) in colorimetric mode is 6.96 μg·L −1 , whereas in the fluorescent mode, it is as low as 2.56 μg·L −1 . Moreover, the detection data obtained by the dual-mode method can be validated by each other, thereby ensuring the dependability of the sensing system. The constructed dual-mode method with merits of sensitivity, speed and accuracy can offer a powerful tool for As(V) detection in environmental water. Furthermore, the application of laccase-mimicking activity in dual-mode detection provides new strategies for other environmental hazard detection.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Na Yang,Xu Guo,Jing Yu,Yu Zhang,Qi Liu,Jiahui Zhu,Hongsen Zhang,Jun Wang
The integration of external field-enhanced effects such as the photothermal effect has emerged as a promising strategy for improving the adsorption efficiency of adsorbents toward Cs + and Sr 2+ due to its energy saving and high efficiency. Herein, a multifunctional photothermal adsorbent is rationally designed and synthesized via a simple one-step hydrothermal method and electrostatic assembly by combining V, W co-doped MoS 2 , P-MXene, and biomass-derived carbon aerogel (VWMoS 2 /P-MXene/C). Doping of V and W induces the phase transition of MoS 2 to the more active 1T phase, providing more accessible active adsorption sites. Moreover, the 3D porous structure of the biomass-derived carbon aerogel offers sufficient water transport channels, accelerating the diffusion kinetics of Cs + and Sr 2+ . The excellent photothermal conversion capability of the VWMoS 2 /P-MXene/C composite drives water evaporation, which promotes the increase of local concentrations of Cs + and Sr 2+ in the water medium. This synergistic mechanism combining phase engineering and photothermal enhancement collectively contributes to the excellent performance in Cs + and Sr 2+ capture. The VWMoS 2 /P-MXene/C demonstrates adsorption capacities of 158.3 mg/g for Cs + and 110.1 mg/g for Sr 2+ within 1 h, respectively, under photothermal enhancement. Simultaneously, the adsorbent exhibits excellent ion selectivity and reusability. The possible adsorption mechanisms mainly involve surface complexation and electrostatic interactions. Moreover, VWMoS 2 /P-MXene/C demonstrates a long-term solar-driven desalination capability with an evaporation rate of 1.98 kg·m −2 ·h −1 in natural seawater. Notably, the VWMoS 2 /P-MXene/C also shows promising application potential for dye removal and oil adsorption. This work provides a universal strategy for designing multifunctional integrated adsorbents and promotes their practical applications in radioactive wastewater treatment and seawater desalination
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Catalysts
·
2021
·Vol. 11
·期 3
·394
·
IF 4.146
Baohe Wang,Honggang Dong,Liang Lu,Hongxia Liu,Zhaobang Zhang,Jing Zhu
A series of KxH1.1-xCu0.2Cs1(NH4)1.5PVMo11O40(KxCuCsNH4PVA) catalysts with differentxvalues were synthesized to catalyze the selective oxidation of methacrolein (MAL) to methacrylic acid (MAA). The effects of potassium (K) ions on both the structure and catalytic activity were studied in detail. The optimum K0.6CuCsNH4PVA exhibited a large surface area, more acid sites, and abundant active species (V4+/VO2+) in the secondary structure of the Keggin structure, consequently offering good catalytic performance. Furthermore, K ions increased the MAA selectivity at the expense of carbon monoxide and carbon dioxide (together defined as COX). Additionally, several process parameters for MAL oxidation were evaluated in the processing experiments. The effects of aldehyde impurities (formaldehyde and propanal) on the catalytic performance were investigated. Possible detrimental effects (catalyst poisoning and structural damage) of aldehyde impurities were excluded. A light decrease in MAL conversion could be attributed to the competitive adsorption of aldehyde impurities and MAL on the catalyst. Hopefully, this work contributes to the design of stable and feasible catalysts for the industrial production of MAA.Keywords:potassium;methacrolein;formaldehyde;propanal;selective oxidation;methacrylic acid;catalytic performance
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ANALYTICAL LETTERS
·
2021
·
IF 2.329
Zhaoxue Zhang,Yi Lu,Haipu Li,Nan Zhang,Junfei Cao,Bo Qiu,Zhaoguang Yang
The simultaneous separation and determination of inorganic trivalent antimony Sb(III) and pentavalent antimony Sb(V) in plant, soil, and sediment samples was carried out by high performance liquid chromatography – inductively coupled plasma – mass spectrometry (HPLC-ICP-MS). The chromatographic conditions (composition and concentration of competing ion, pH value and flow rate of mobile phase) and the operating parameters for inductively coupled plasma – mass spectrometry were optimized by single factor experiments. The separation of the Sb species was achieved within 6 min using the optimized chromatographic conditions. The detection limits of the method were 0.016 μg/L and 0.021 μg/L for Sb(III) and Sb(V), respectively. The retention times of Sb(V) and Sb(III) were 2.7 min and 4.5 min, respectively. The relative standard deviations for replicate measurements (n = 6) of low (5 μg/L), medium (20 μg/L), and high (40 μg/L) concentrations of Sb(III) and Sb(V) were less than 4%. The results of spiking and recovery experiments for the extracting solutions of soil, sediments, and plants showed that the spiked recoveries of the two species ranged from 92% to 103%. This method has been used to determine the antimony species in extracts of environmental samples.
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CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
Jin-Xia Yang,Xin Zhang,Ye-Yan Qin,Yuan-Gen Yao
A 2D network of {[Zn(Hbcpt)(H2O)3]·7H2O} (1) was hydrothermally synthesized and structurally characterized. By employing different N-donor ligands into the system of 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole (H3bcpt) and Zn(II) cations, six novel entangled coordination polymers, namely, {[Zn2(bcpt)(μ2-OH)(H2O)]·(py)·4H2O} (2), {[Zn2(Hbcpt)2(bpa)2]·2H2O} (3), {[Zn(Hbcpt)(bpp)]·[Zn(Hbcpt)(bpp)]·2.5H2O} (4), {[Zn5(bcpt)2(biimpy)2(μ2-OH)4]·5H2O} (5), {[Zn2(bcpt)(bib)(μ2-OH)]·H2O} (6), and {[Zn2(bcpt)(bix)4(μ2-OH)]·3H2O} (7) (H3bcpt = 3,5-bis(4′-carboxyl-phenyl)-1,2,4-triazole, bpa = 1,2-bis(4-pyridyl)ethane, bpp = 1,3-bi(4-pyridyl)propane, biimpy = 2,6-bis(imidazole-1-yl)pyridine, bib = 1,4-bis(N-imidazolyl)butane, bix = 1,4-bis(imidazol-1-ylmethyl)-benzene, py = pyridine), were obtained. Single-crystal X-ray diffraction analysis reveals that, with the different N-donor ligands, the resulting compounds present entangled structures with different topologies. Compound 1 shows a 2D (4, 4) network, and the adjacent sheets are extended into a 3D supramolecular framework via hydrogen-bonding interactions. Interesting, by introducing a series of ditopic N-donor ligands into the reaction system, compounds 2–7 with entangled structures were harvested. Compound 2 exhibits a 3D self-penetrating network with an 8-connected bcu topology. Compound 3 features an 8-fold dia network showing an unusual [4 + 4] mode of interpenetration. Compound 4 is comprised of two parts of undulated 2D 44-sql networks, and the adjacent undulated layers are parallel interpenetrated to each other to give a 2D → 3D polycatenated framework. Compound 5 presents an unusual 3D self-penetrating network with a novel 4,6,6-connected trinodal network with the point symbol of (32·4·52·6)(32·4·56·66}{32·56·66·7}. Compound 6 shows a 2-fold interpenetrating 3D architecture with 6-connected sxd topology. Compound 7 displays an unprecedented self-penetration derived from abnormal [3 + 2] 5-fold interpenetrating dia subnets. Structural diversity of these compounds suggests that different N-donor ligands can induce the organic ligand to present different conformations and coordination modes, and the influence on the final structures. Furthermore, the luminescent properties of compounds 1–7 have been investigated in the solid state.
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Advanced Energy Materials
·
2020
·Vol. 10
·期 25
·2000892
·
IF 25.245
Yongchao Tang,Xuejin Li,Haiming Lv,Dong Xie,Wenlong Wang,Chunyi Zhi,Hongfei Li
In aqueous alkaline Zn batteries (AZBs), the Co 3+ /Co 4+ redox pair offers a higher voltage plateau than its Co 2+ /Co 3+ counterpart. However, related studies are scarce, due to two challenges: the Co 3+ /Co 4+ redox pair is more difficult to activate than Co 2+ /Co 3+ ; once activated, the Co 3+ /Co 4+ redox pair is unstable, owing to the rapid reduction of surplus Co 3+ to Co 2+ . Herein, CoSe 2− x is employed as a cathode material in AZBs. Electrochemical analysis recognizes the principal contributions of the Co 3+ /Co 4+ redox pair to the capacity and voltage plateau. Mechanistic studies reveal that CoSe 2− x initially undergoes a phase transformation to derived Co x O y Se z , which has not been observed in other Zn//cobalt oxide batteries. The Se doping effect is conducive to sustaining abundant and stable Co 3+ species in Co x O y Se z . As a result, the battery achieves a 10 000-cycle ultralong lifespan with 0.02% cycle −1 capacity decay, a 1.9-V voltage plateau, and an immense areal specific capacity compared to its low-valence oxide counterparts. When used in a quasi-solid-state electrolyte, as-assembled AZB delivers 4200 cycles and excellent tailorability, a promising result for wearable applications. The presented effective strategy for obtaining long-cyclability cathodes via a phase transformation-induced heteroatom doping effect may promote high-valence metal species mediation toward highly stable electrodes.
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Food & Function
·
2025
·
IF 5.4
Xuan Chen,Xinmiao Wang,Qian Wang,Dong Cai,Jinghan Yu,Beiwei Zhu,Dayong Zhou,Fawen Yin
The heat treatment method was used to synthesize starch inclusion complexes from starch and short-chain alkyl gallates (a typical representative of phenololipids), such as butyl gallate, propyl gallate, ethyl gallate and methyl gallate. In an everted rat gut sac model, HPLC-UV analysis revealed that the released alkyl gallates from inclusion complexes were degraded to produce gallic acid. Gallic acids (0.009455–0.014160 nmol min−1) and alkyl gallates (0.2695–0.9441 nmol min−1) were both able to pass through intestinal membranes. After transmembrane transfer, alkyl gallates could also be hydrolyzed to produce gallic acid (1.947 × 10−5–2.290 × 10−5 min−1). It was evident that such an inclusion complex demonstrated superior dual sustained-release characteristics for phenolic compounds. Meanwhile, starch inclusion complexes can also slow down starch digestion by raising resistant starch (from 12.2% to 27.2–46.0%) and lowering rapidly digestible starch (from 51.2% to 22.2–51.2%), according to a glucose oxidase–peroxidase analysis. The delayed digestion behavior of starch in inclusion complexes is very beneficial for blood glucose control. Thus, our work effectively established a theoretical foundation for modifying the dual sustained-release behavior of phenolic compounds and the retardation of starch digestion by adjusting the carbon-chain length in starch inclusion complexes.
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