SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Qinqin He,Hongjun Zhao,Zedong Teng,Yin Wang,Weiling Sun,Yali Guo,Xiaonan Ji,Wei Hu,Su Shiung Lam,Min Li
Phosphorus (P) is known as a valuable resource, and recycling it from wastewater can avoid environmental pollution and resource waste. Herein, a regenerable magnetic Fe 3 O 4 and La-based metal–organic framework functional material (Fe 3 O 4 /La-MOF) was synthesized by solvent thermal method and its adsorption performances of phosphate were evaluated. The as-prepared magnetic Fe 3 O 4 /La-MOF exhibited magnetic separation efficiency of 97.9% and it could maintain the high adsorption capacity over a wide pH range from 3 to 10, as well as showed an excellent P adsorption selectivity in presence of Cl - , NO 3 – , HCO 3 – , CO 3 2– and SO 4 2- . The isotherm data were consistent with the Langmuir model, and the adsorption kinetic data conformed to the pseudo-second-order model, revealing that there was chemical adsorption between Fe 3 O 4 /La-MOF and phosphate. The electrochemical behavior of Fe 3 O 4 /La-MOF before and after phosphate adsorption showed that the band gap energy of LUMO (Lowest Unoccupied Molecular Orbital) and HOMO (Highest Occupied Molecular Orbital) of P adsorbed Fe 3 O 4 /La-MOF was lower than that of the material itself, which indicated the successful adsorption of phosphate on Fe 3 O 4 /La-MOF and the forming of a perfect hybrid structure. The characterization analysis of FT-IR and XPS illustrated that intra-sphere complex (La O P) formed between Fe 3 O 4 /La-MOF and phosphate by ligand exchange, which might be the dominant mechanism, followed by electrostatic attraction and precipitation. This study highlighted the great promise of magnetic reusable Fe 3 O 4 /La-MOF composite for application in phosphate removal and recovery.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhen Pu,Jianwei Qin,Xiaoguo Fu,Ruizhi Qiu,Bin Su,Maobing Shuai,Fang Li
Fundamental investigation of metal–CO interactions is of great importance for the development of high-performance catalysts to CO activation. Herein, a series of side-on bonded mononuclear lanthanide (Ln) oxocarbonyl complexes OLn(η2-CO) (Ln = La, Ce, Pr, and Nd) have been prepared and identified in solid argon matrices. The complexes exhibit uncommonly low C–O stretching bands near 1630 cm–1, indicating remarkable C–O bond activation in these Ln analogues. The η2-CO ligand in OLn(η2-CO) can be claimed as an anion on the basis of the experimental observations and quantum chemistry investigations, although the CO anion is commonly considered to be unstable with electron auto-detachment. The CO activation in OLn(η2-CO) is attributed to the photoinduced intramolecular charge transfer from LnO to CO rather than the generally accepted metal → CO π back-donation, which conforms to the traditional Dewar–Chatt–Duncanson motif. Energy decomposition analysis combined with natural orbitals for chemical valence calculations demonstrates that the bonding between LnO and η2-CO arises from the combination of dominant ionic forces (>76%) and normal Lewis “acid–base” interactions. The fundamental findings provide guidelines for the catalyst design of CO activation.
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TALANTA
·
2022
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IF 6.556
Wenxin Cui,Zhaoqing Cai,Qing Li,Haiyun Qu,Jiaqian Zheng,Dengguang Yu,Junfeng Chen,Zheng Wang
In this study, a laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) method for in-situ determination of yttrium and trace elements in yttrium-doped barium fluoride (BaF 2 : Y) crystals was proposed. A facile, micro-damage procedure for quantifying the segregation coefficient of doping elements was investigated, and it was found that the actual yttrium doping concentration increases from the seed end to the tail end in BaF 2 : Y crystals. In micro-area analysis, this method has higher mass sensitivity which was applied to quantify the impurity content and distribution during the growth of BaF 2 : Y crystals. Regression coefficient of calibration curve for each element ranged from 0.9918 to 0.9995. Detection limits (DLs) were 0.05, 0.03, 0.01 and 0.01 μg g −1 for Mg, Zn, Sr and Pb, respectively. The accuracy of the proposed method was verified by inductively coupled plasma mass spectrometry/atomic emission spectroscopy (ICP-MS/AES) with wet-chemical pretreatment. The objective of the presented work was to provide a less damaging and more novelty approach for crystal sample analysis.
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Horticulturae
·
2022
·Vol. 8
·期 11
·1029
·
IF 2.923
Qing-Fang Xu,Liang Fan,Kai-Xiang Lu,Dong-Mei Zhao,Ming-Xia Zhang,Jian Cai
Both free and glycosidically bound forms of volatile compounds in Vidal grapes from the Shangri-La high-altitude region during the on-vine non-destructive dehydration process were investigated by headspace solid-phase micro-extraction (HS-SPME) combined with gas chromatography–mass spectrometry (GC-MS), following which the data were processed by multivariate statistical analysis. Fatty-acid-derived volatiles (FADs), amino-acid-derived volatiles (AADs), and isoprene-derived volatiles (IPDs), which occurred mainly in bound forms, were the three major volatiles in dehydrated Vidal grapes. Water-loss concentration, biosynthesis, and biodegradation all occurred during dehydration, eventually modifying some volatiles significantly, especially some powerful odorants such as hexanal,trans-2-hexenal, 2-phenethyl acetate, β-myrcene, linalool, geraniol,cis-rose oxide, and β-damascenone. 1-Octen-3-ol was relatively stable during the non-destructive on-vine dehydration process and its content in grape juice was mainly determined by the concentration effect. 2,4-Di-tert-butylphenol, 2-phenethyl acetate, 2-methyl-1-propanol, and hexanol were screened as some of the most important metabolic markers to discriminate grapes at different dehydration degrees. Our study also highlights the fundamental importance of the expression of volatile content in the metabolomic study of grape berries.Keywords:late harvest;over-ripening;dessert wine;metabolomics;clustered heatmap;OPLS-DA
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Lingchao Kong,Jun Zhang,Yi Wang,Qinlin Yan,Jiayu Xu,Xi Quan,Charles B. Andrews,Zuotai Zhang,Chunmiao Zheng
Hazardous oxyanions in water bodies are potentially toxic to aquatic life, and the coexistence of multiple anions aggravates the toxicity. Herein, bowknot-like Zr/La bimetallic organic frameworks (Zr/La-BTC) were developed with superior hazardous oxyanion adsorption capacities, i.e., approximately 102 mg/g for arsenate and 159 mg/g for phosphate, respectively. The molar ratio of Zr to La in Zr/La-BTC plays a significant role in the structure and the adsorption efficiencies. Notably, the experiment-derived adsorption capacities of various Zr/La-BTC samples were consistent with their adsorption energies calculated by density-function theory (DFT). Further mechanism analysis revealed that coordination of Zr/La atoms with the target anion groups occurred during adsorption. The positive shift of binding energies in La 3d and Zr 3d XPS spectra and Bader charge analysis unveiled that back-donation interactions dominated the adsorption process . The reliable adsorption selectivity and reusability of 0.1Zr/La-BTC were verified with anion competition experiments and four adsorption-desorption cycles. Overall, this study provides significant insight into the design of high-performance bimetallic organic frameworks for the enhanced removal of hazardous oxyanions from water.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yi Liu,Dengjie Zhong,Yunlan Xu,Haixing Chang,Lin Dong,Zhuofan Han,Jun Li,Nianbing Zhong
The limited metal sites of monometallic MOFs and the high influence of pH limit their adsorption capacity. To solve these problems, La/Al bimetallic MOFs/chitosan composite was prepared by hydrothermal synthesis and impregnation methods and then characterized by XRD, FTIR, SEM, BET and XPS techniques. The doping of La has no obvious effect on the structure of Al-MOFs, but chitosan has greatly changed the structure of La/Al bimetallic MOFs. The phosphate adsorption of the composite was affected by La/Al molar ratio, chitosan/bimetallic MOFs mass ratio, temperature, phosphate initial concentration, adsorbent dosage, pH, and coexisting ions. The optimum molar ratio of La/Al and mass ratio of chitosan/bimetallic MOFs are 0.5:1 and 5.0%, respectively. The addition of La and chitosan can provide additional adsorption active sites, inhibit metal leaching, and enhance the phosphate adsorption performance, stability, and acid-alkali resistance of the composite. Its maximum adsorption capacity was 264.48 mg·g −1 . Its phosphate removal efficiency is above 90% at pH= 3.0–9.0. The actual phosphorus-containing wastewater with 7.064 mg·L −1 PO 4 3- and initial pH 7.4 can be treated to meet Chinese first-class effluent quality standard. La, Al, amino groups, and hydroxyl groups play an important role in the adsorption process of phosphate. When pH < pH pzc (4.99), phosphate is adsorbed by electrostatic gravitation between it and protonated positively charged amino and hydroxyl groups on La and Al, while when pH > pH pzc , phosphate is removed by ligand exchange between it and hydroxyl groups on La and Al. A stable, low-cost, and efficient bimetallic MOFs-based phosphate adsorbent was designed and prepared in this paper, and the results can provide reference for researchers in environmental chemical engineering .
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JOURNAL OF LUMINESCENCE
·
2021
·
IF 3.599
Renping Cao,Yanshu Zhao,Zuofu Hu,Wenhua Shao,Fen Xiao,Guotai Zheng,Pan Liu,Ting Chen
In this work, we successfully synthesize La(Mg 1-x Nb x )O 3 :Mn 4+ ( x = 0.296 and 0.384) deep-red emitting phosphors by using high-temperature solid state method in air and investigate their crystal structures, morphologies, and luminescence properties. A broad excitation spectral band of La(Mg 1-x Nb x )O 3 :Mn 4+ phosphors monitored at 705 nm can be observed in the region from 220 nm to 580 nm. La(Mg 1-x Nb x )O 3 :Mn 4+ phosphors show a deep-red emission in the range of 640–760 nm with a peak at ~705 nm due to 2 E → 4 A 2 transition of Mn 4+ ions and the corresponding chromaticity coordinates are (0.7316, 0.22684). The concentration dependent emission spectra indicate that their optimal Mn 4+ doping concentration is ~0.6 mol%. Their lifetime values decrease with increasing the Mn 4+ doping concentration from 0.2 mol% to 1.0 mol%. The experimental results are helpful for the research on luminescence property of Mn 4+ ions.
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ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Kai Sun,Xing Cheng,Jialin Yu,Luojian Chen,Jiajun Wei,Wenjun Chen,Jun Wang,Shunyao Li,Qingzhu Liu,Youbin Si
Estrogens, which are extensive in the eco-environments, are a category of high-toxic emerging contaminants that induce metabolic disorders and even carcinogenic risks in wildlife and humans. Here we investigate whether fungus-secreted laccase can be used as a green catalyst to eliminate a representative estrogen, 17 β -estradiol (E2). A white-rot fungus Trametes hirsuta La-7 with high laccase-productivity, was isolated from pig manure-contaminated soil. Extracellular laccase activity expressed by strain La-7 was 65.4 U·mL −1 for a 3 d inoculation under the optimal fermentation parameters. The concentrated-crude laccase from Trametes hirsuta La-7 (CC- Th Lac) was capable of effectively metabolizing E2 at pH 4–6, and the apparent pseudo first-order reaction rate constant and half-life values were respectively 0.027–0.055 min −1 and 25.86–12.67 min ( R 2 > 0.98). The mass measurement of high-resolution mass spectrometry in combination with 13 C-isotope labeling identified that the main by-products of E2 metabolism were dimers, trimers , and tetramers, which are consistent with radical-driven C–C and/or C–O–C covalent coupling pathway, involving the initial enzymatic production of phenoxy radical intermediates and then the successive oxidative-oligomerization of radical intermediates. The formation of oligomers dramatically reduced the estrogenic activity of E2. Additionally, CC- Th Lac also exhibited high-efficiency metabolism capability toward E2 in the natural water and pig manure, with more than 94.4% and 91.0% of E2 having been metabolized, respectively. These findings provide a broad prospect for the clean biotechnological applications of Trametes hirsuta La-7 in estrogen-contaminated ecosystems.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Hongtao Zou,Feng Guo,Minghong Luo,Qilu Yao,Zhang-Hui Lu
Ultrafine NiFe nanoparticles (NPs) decorated by La(OH) 3 have been successfully prepared via a facile one-step co-reduction method without the help of surfactant or support. It was found that after being decorated with La(OH) 3 , the NiFe–La(OH) 3 NPs have a smaller particle size and lower crystallinity . The resultant NiFe–La(OH) 3 nanocatalyst exhibits an excellent catalytic activity , 100% H 2 selectivity, and satisfied recyclability for hydrogen evolution from hydrous hydrazine (N 2 H 4 ·H 2 O) at 343 K under alkaline conditions, giving a high turnover frequency (TOF) value of 100.6 h −1 , which is more than 35 times higher than pure NiFe NPs (2.8 h −1 ). The kinetics study shows that with respect to the concentration of catalyst and N 2 H 4 , the N 2 H 4 dehydrogenation reaction follows fist-order kinetics and zero-order kinetics, respectively. Furthermore, NiFe–La(OH) 3 also exhibits an outstanding performance and excellent recycle stability during high dehydrogenation of hydrazine borane (N 2 H 4 BH 3 ). The excellent performances for the dehydrogenation of N 2 H 4 and N 2 H 4 BH 3 could be attributed to the strong interaction between La(OH) 3 and NiFe NPs, as well as ultrafine and low crystalline NiFe NPs due to the addition of La(OH) 3 .
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JOURNAL OF RARE EARTHS
·
2020
·
IF 3.104
Shuo Wang,Zhenke Chen,Ying Zhao,Chenlu Sun,Jianye Li
In this work, the unique starlike La-doped ZnO–SiO 2 photocatalysts were constructed by an evaporation and calcination method and characterized in detail. UV–vis reflectance and DFT calculation confirm that the doping with La allows to obtain a decrease of band gap of ZnO/SiO 2 , which enhances visible light absorbance and oxidizing ability. The photoluminescence intensity reduces greatly, indicating more effective separation of the photogenerated carriers of La-doped ZnO-SiO 2 . Photocatalytic activities of La-doped ZnO-SiO 2 with different doping ratios under simulated visible light irradiation were evaluated with malachite green (MG) as a model pollutant. Under optimized conditions including solution pH of 8, 15 mg/L of MG solution and 15 mg of catalyst dosage, 0.2% La-ZnO-SiO 2 exhibits the best catalytic activity in photodegradations of MG in water. The removal and mineralization efficiency of MG can reach 96.1% and 70.9% in 140 min, respectively. The as-prepared catalysts present superior stability and recyclability after four times reuse. Moreover, selective quenching experiments indicate that hydroxyl radical (·OH), hole (h + ) and superoxide radical (·O 2 - ) are the main reactive species responsible for MG degradation. Possible mechanism for photocatalytic elimination of MG over La-doped ZnO/SiO 2 photocatalyst is finally proposed.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Jinhui Liu,Jiasen Cui,Xing Wei,Weitao Li,Chunran Liu,Xuewen Li,Mingli Chen,Yu Fan,Jianhua Wang
It is the first time to investigate local distribution patterns of mercury (Hg) in mice organs after Hg and Se exposure with detection of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Two batch of adult mice were employed to be exposed to inorganic mercury (iHg) and methylmercury (MeHg) with or without Se at the dose of 55 μmol kg −1 . Tissue sections of brain, kidney, liver, and spleen from one batch mice were prepared to get local imaging of Hg by LA-ICP-MS. Tissues from another batch mice were used to quantify Hg and Se in tissues with ICP-MS after acid digestion . The results indicated that, for mice exposed to iHg, Hg mainly distributed in kidney, a little in liver, and hardly in brain and spleen; for mice exposed to MeHg, lower amount of Hg was found in kidney, liver and spleen, and almost no Hg was found in brain. It was interesting that for Hg and Se co-administration groups, higher level of Hg was observed in kidney, liver, spleen and even in brain than single Hg administration groups. In addition, Se level in organ tissues increased obviously not only in Se exposure group but also in MeHg exposure group, while the phenomenon was not observed in iHg exposure group. HepG2 cells were employed to investigate Se and Hg interactions in single cell level, similar bioaccumulation behavior of Hg was found between cells and mice organs. Higher level of Hg was observed in cells cultured with Se and Hg medium than cells cultured with single Hg medium. The results are expected to provide new insight to investigate Hg and Se interactions in animal bodies and in-vitro cells.
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RSC Advances
·
2021
·Vol. 11
·期 41
·25258-25265
·
IF 3.361
Long Liu,Sheng Chang,Yan Wang,Hexiang Zhao,Shuteng Wang,Chengfeng Zheng,Yingying Ding,Shixue Ren,Jiguo Zhang,Yuan-Ru Guo
An Fe3O4/carboxymethyl cellulose (Fe3O4/CMC) magnetic biosorbent was prepared using the ion-imprinting technology, where La(III) was used as the template ion. The morphology and structure of Fe3O4/CMC were characterized by SEM, FTIR and XRD. It is found that nano Fe3O4 with inverse spinel structure can distribute in CMC and endow the composite with good magnetic properties. The adsorption performance such as adsorption capacity, influence of pH and initial concentration were fully explored. The prepared Fe3O4/CMC is revealed to have good adsorption properties with Qmax of 61.5 mg g−1, in line with the pseudo-second-order kinetic model. When handling the multi-ion coexistence solution of Cu(II), Ni(II) and Cd(II), Fe3O4/CMC shows high selective adsorption for La(III). Meanwhile, cycling experiments find that the adsorption capacity is only slightly reduced (less than 5%) after 5-time reuse. Good adsorption properties, high selectivity and easy recovery give the newly-synthesized Fe3O4/CMC biosorbent broad application potential in the treatment of La(III)-containing wastewater.
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