DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 3
·989-996
·
IF 4.099
Ling Yang,Tian Zhao,Ishtvan Boldog,Christoph Janiak,Xiao-Yu Yang,Qiang Li,Yan-Jia Zhou,Yong Xia,Deng-Wang Lai,Yue-Jun Liu
The concentration of benzoic acid was found to exercise efficient control over the formation of either MIL-101(Cr) or MIL-88B(Cr) under otherwise similar hydrothermal synthetic conditions. Nanocrystals of MIL-101(Cr) with ∼100 nm average size and excellent SBET = 3467 m2 g−1 are obtained at lower concentrations of benzoic acid, while at higher concentrations the microparticulated MIL-88B(Cr) product is formed. Hereby a new efficient synthetic method towards the elusive MIL-88B(Cr), yet reported only once without synthetic details, is proposed. The obtained MIL-88B(Cr) has an interesting and potentially valuable property of retaining its high-volume form (Vcell ∼ 2000 Å3) after thermal activation. The degassing of MIL-88B(Cr) in a vacuum at 250 °C yields a porous material with a SBET area of 1136 m2 g−1, which is around the theoretical maximum. The transition to the denser ‘closed’ form (Vcell ∼ 1500 Å3) occurs only at 350 °C, when all of the benzoate/benzoic acid, hindering the process, is removed.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chengfang Zhang,Zhenyu Song,Chao Li,Qinglong Liu,Jingchun Tang
In the actual polluted environment, the composite pollution system was usually composed of heavy metals and organic pollutants, especially Cr(VI) and chlorophenols often co-existed in industrial wastewater. In this study, a composite material consisting of multilayer graphene carbon shells coated with nZVI (gBC@nZVI) with various excellent properties was applied to deal with the composite system of Cr(VI) and 2,4-dichlorophenol (2,4-DCP) coexisting in the wastewater, and the intrinsic mechanism for the simultaneous removal of heavy metals and organic pollutants was systematically investigated. The results showed that in the composite pollution system (Cr(VI) = 20 mg/L, 2,4-DCP = 15 mg/L), complete removal of Cr(VI) could be achieved in 60 min, while 2,4-DCP achieved 95.2 % removal, with the contribution of oxidative degradation being 76.4 %. It was found that during the efficient adsorption and reduction of Cr(VI) by gBC@nZVI, the generation of the metastable intermediate Cr(V) was verified by probe compounds, electron spin resonance and UV–visible spectroscopy, and further experiments demonstrated that the generation of •OH was closely related to Cr(V) and promoted the oxidative degradation of the coexisting 2,4-DCP. Quenching experiments with the addition of specific scavengers indicated that •OH was the active species directly dominating the oxidative degradation of 2,4-DCP, whereas Cr(V) was indirectly involved in the degradation of 2,4-DCP by promoting the generation of •OH. In addition, the increase of solution pH negatively affected the degradation of 2,4-DCP in the composite polluted system, mainly due to the hindered generation of •OH in the alkaline environment. This work provided theoretical support for the promising application of gBC@nZVI in real environments contaminated with a combination of Cr(VI) and chlorophenols.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 7
·1-11
·
IF 6.232
Guo Hao,Wu Ning,Xue Rui,Liu Hui,Wang Mingyue,Yao Wenqin,Wang Xiaoqiong,Yang Wu
An Eu(III)-functionalized strontium-organic framework (Eu 3+ @Sr-MOF) was synthesized by encapsulating Eu 3+ ions into the pores of Sr-MOF via postsynthetic modification (PSM) and fully characterized by XRD, SEM, EDS, FTIR, and TGA. The luminescent properties of Eu 3+ @Sr-MOF were measured and investigated in detail, which demonstrated that Eu 3+ @Sr-MOF not only possessed excellent water and chemical stabilities in a wide pH range (5–10) but also displayed red luminescence with excitation/emission maxima at 332/617 nm. The Eu 3+ @Sr-MOF can be considered as a highly selective and sensitive recyclable luminescence probe for sensing Cr(III) and Cr(VI) based on strong luminescence quenching effects; it can be recycled at least five times. The luminescence probe for Cr 3+ , CrO 4 2− , and Cr 2 O 7 2− shows low detection limits (0.15 μM, 0.17 μM, and 0.13 μM, respectively), relatively broad linear ranges (0.6–150 μM, 0.1–200 μM and 0.4–180 μM, respectively), and high quenching constants K SV . The signals can be observed by the naked eye under UV light of 365 nm. The method was applied to the determination of total Cr in environmental water samples.
Graphical abstract
研究领域:
分析化学
·
环境科学
·
材料科学
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MOLECULES
·
2019
·Vol. 24
·期 20
·3718
·
IF 3.06
Mao-Long Chen,Shu-Yang Zhou,Zhou Xu,Li Ding,Yun-Hui Cheng
MIL-100(Fe, Cr) and MIL-101(Cr) were synthesized by the hydrothermal method and applied to the adsorptions of five aromatic amines from aqueous solutions. These three metal-organic frameworks (MOFs) were well characterized by powder X-ray diffraction (PXRD), scanning electron microscope (SEM), transmission electron microscope (TEM), thermogravimetric analysis (TGA) and surface area analysis. The adsorption mechanism of three MOFs and the effects of the structures of MOFs on the adsorption of aromatic amines were discussed. The results show that the cavity system and suitable hydrogen bond acceptor were important factors for the adsorption for five aromatic amines of aniline, 1-naphthalamine, o-toluidine, 2-amino-4-nitrotoluene and 2-nitroaniline: (a) the saturated adsorption capacity of aniline, 1-naphthylamine and o-toluidine on MIL-100(Fe) were 52.0, 53.4 and 49.6 mg/g, respectively, which can be attributed to the intermolecular hydrogen bond interaction and cavity system diffusion. (b) The adsorption capacity of 2-nitroaniline and 2-amino-4-nitrotoluene on MIL-101(Cr) were 54.3 and 25.0 mg/g, respectively, which can be attributed to the more suitable pore size of MIL-101(Cr) than that of MIL-100(Fe, Cr). The MOFs of MIL-100(Fe) and MIL-101(Cr) can be potential materials for removing aromatic amines from aqueous solutions.Keywords:metal-organic framework;adsorption;aromatic amines;aniline;1-naphthalamine;o-toluidine;2-amino-4-nitrotoluene;2-nitroaniline
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Peiyuan Xiao,Junqing Xu,Hongliang Shi,Fengyang Du,Huanzheng Du,Guangming Li
The simultaneous reduction of Cr(VI) and sequestration of the resulting Cr(III) in one process is highly desirable as a cost-effective and environmental-friendly approach for the decontamination of Cr(VI)-polluted wastewater. However, most of the existing adsorptive materials are only effective in low pH environments (pH = 1–3), severely restricting the adsorption efficiency and cost effectiveness. Herein, we proposed a chitosan-based magnetic porous microsphere (PPy@PMCS) for simultaneous Cr(VI) reduction and Cr(III) sequestration in a wide pH range. Benefiting from its abundant interaction sites, Cr(VI) was effectively adsorbed on the surface and then immediately reduced to Cr(III) with much lower toxicity. Most importantly, the resulting Cr(III) was in-situ sequestrated by the complexation of chitosan matrix. As a result, PPy@PMCS exhibited a maximum Cr(VI) adsorption capacity of 330.42 mg/g at pH 2.0 and an adsorption capacity of 167.82 mg/g even at near neutral pH (6.0), which is superior to most reported adsorbents. Furthermore, the exhausted PPy@PMCS can be rapidly separated from solutions under an external magnetic field and facilely regenerated. The proposed novel biopolymer-based material shows great application potentials in wastewater treatment.
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JOURNAL OF MOLECULAR LIQUIDS
·
2017
·
IF 3.648
Qianwei Liang,Junjie Geng,Hanjin Luo,Wei Fang,Yuwei Yin
In the present study, a novel magnetic Cr(VI) ion-imprinted polymer (MGOIIP) was prepared by a sol-gel process for fast and selective adsorption of Cr(VI) anions from aqueous solutions. In the synthesis process, 4-vinyl pyridine (4-VP) and 2-hydroxyethyl methacrylate (HEMA) were used as functional monomer and co-monomer; ethylene glycol dimethacrylate (EGDMA) and N , N -azoisobisbutyronitrile (AIBN) were used as cross-linker and initiator, respectively; acetone was selected as solvent. Fe 3 O 4 @SiO 2 nanoparticles were introduced for separating adsorbents from the aqueous solution conveniently, and graphene oxide (GO) could prevent Fe 3 O 4 @SiO 2 particles from aggregating. Some different techniques including Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), SEM-energy dispersive spectroscopy (SEM-EDS), X-ray diffraction (XRD) and thermogravimetric analysis (TGA) were used to confirm the successful synthesis of ion-imprinted polymer on the surface of Fe 3 O 4 @SiO 2 /GO nanoparticles. The obtained magnetic ion-imprinted polymer has a high adsorption capacity (up to 311.95 mg/g) for Cr(VI) anions at an optimal pH of 2.0, and the adsorption equilibrium can be reached within 3 min. The adsorption process can be fitted well with Langmuir isotherm model and the pseudo-second-order kinetic model . Moreover, the results showed that MGOIIP has excellent selectivity and good regeneration ability. The prepared MGOIIP exhibited a satisfactory recovery for Cr(VI) anions in tap, river and lake water samples.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2016
·
IF 3.976
Zunwei Chen,Shufang Song,Yuezhong Wen
The priority pollutant chromium (Cr) was ubiquitous and great efforts have been made to reduce Cr (VI) into less-toxic Cr (III) by alga for the convenient availability and low expense. However, the functional role of organelle inside the algal cell in Cr (VI) reduction was poorly understood. In this study, organelles in green algae Chlorella vulgaris were extracted and further decorated for Cr (VI) reduction tests. Results showed that the chloroplast exhibited not only adsorption ability of total Cr (21.18% comparing to control) but also reduction potential of Cr (VI) (almost 70% comparing to control), whose most suitable working concentration was at 17 μg/mL. Furtherly, the isolated thylakoid membrane (ITM) showed better Cr (VI) reduction potential with the presence of sodium alginate (SA), even though the Hill reaction activity (HRA) was inhibited. As for photosystem II (PSII), the addition of mesoporous silica SBA-15 enhanced the reduction ability through improving the light-harvesting complex (LHC) II efficiency and electron transport rate. On the whole, the reduction ability order of the three kinds of materials based on chloroplast in C. vulgaris was PSII@SBA-15 > Chloroplast > ITM@SA. The attempt made in this study to reduce the Cr (VI) with C. vulgaris organelles might not only offer basement to detect the potential action mechanism of Cr (VI) reduction by C. vulgaris but also provide a new sight for the scavenge of heavy metal with biological materials.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2012
·Vol. 18
·期 51
·16491-16497
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IF 5.925
Fan Qin,Guangfang Li,Runming Wang,Jiliang Wu,Hongzhe Sun,Rong Chen
Graphical Uniform Bi 2 O 3 and (BiO) 2 CO 3 nanotubes were synthesized by a solvothermal method without involving any surfactants or templates. The synergistic effect of ethylene glycol and urea played a critical role in the formation of the tubular structure. The Bi 2 O 3 and (BiO) 2 CO 3 nanostructures not only exhibited excellent Cr VI -removal capacity, but also displayed high photocatalytic efficiency for the degradation of Rhodaine B under visible-light irradiation (see figure). Uniform bismuth oxide (Bi 2 O 3 ) and bismuth subcarbonate ((BiO) 2 CO 3 ) nanotubes were successfully synthesized by a facile solvothermal method without the need for any surfactants or templates. The synergistic effect of ethylene glycol (EG) and urea played a critical role in the formation of the tubular nanostructures. These Bi 2 O 3 and (BiO) 2 CO 3 nanotubes exhibited excellent Cr VI -removal capacity. Bi 2 O 3 nanotubes, with a maximum Cr VI -removal capacity of 79 mg g −1 , possessed high removal ability in a wide range of pH values (3–11). Moreover, Bi 2 O 3 and (BiO) 2 CO 3 nanotubes also displayed highly efficient photocatalytic activity for the degradation of RhB under visible-light irradiation. This work not only demonstrates a new and facile route for the fabrication of Bi 2 O 3 and (BiO) 2 CO 3 nanotubes, but also provides new promising adsorbents for the removal of heavy-metal ions and potential photocatalysts for environmental remediation.
研究领域:
材料科学
·
环境科学
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Dongsheng Xie,Shasha Chu,Shihua Zhang,Andrei Ivanets,Lijuan Zhang,Xintai Su
Electroplating sludge (ES) is a typical industrial hazardous waste , which contains multitudes of valuable transition metal resources. Hence, there is an urgent need for a method which can not only effectively detoxify, but also reasonably reuse ES resources. In this work, we synthesized Cr-doped ferrite catalyst (HT-ES) derived from Cr-containing ES v ia hydrothermal treatment, and applied it for the degradation of tetracycline (TCH). After hydrothermal treatment, the HT-ES with double metal oxide structure and large specific surface area (168.3 m 2 g −1 ) was obtained. The removal percentage of TCH could reach 90.79%, under the optimum conditions derived by response surface methodology . Experimental results demonstrated that HT-ES also exhibited high resistance to water impurities (i.e., Cl - , HCO 3 - , NO 3 and humic acid) and perfect reusability. The electron spin resonance and radical quenching experiments revealed that SO •- 4 , •OH and O •- 2 radicals appeared in the TCH degradation reaction system. Finally, a probable degradation mechanism of TCH was proposed based on the experimental results. This work not only achieved the stabilization of Cr-containing ES, but also obtained an excellent catalyst for the removal of TCH, realizing the goal of treating waste with waste.
研究领域:
环境科学
·
催化材料
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GEOCHIMICA ET COSMOCHIMICA ACTA
·
2019
·
IF 4.258
Guojun Chen,Yanan Bai,Raymond Jianxiong Zeng,Liping Qin
Chromium isotopes are promising for monitoring and quantifying the extent of microbial Cr(VI) reduction. However, the mechanisms and factors that influence Cr isotope fractionation are not well understood. In the present study, we investigated the effects of different metabolic pathways and various environmental parameters on Cr isotope fractionation during Cr(VI) reduction by the extremely thermophilic bacterium Caldicellulosiruptor saccharolyticus . The Cr isotopic compositions were measured on unreacted Cr(VI) in the remaining solution. The reaction product is isotopically lighter than the reactant. The Cr isotope composition for remaining Cr(VI) in the solution followed a Rayleigh fractionation trend and thus became increasingly isotopically heavier as the reduction of Cr(VI) proceeded. Cr(VI) reduction mainly occurs on the cell surface by Ni–Fe hydrogenase; however, in the presence of CuCl 2 , the activity of Ni–Fe hydrogenase was inhibited, and Cr(VI) was reduced inside the cells. We found that despite different Cr(VI) reduction locations, Cr isotope enrichment factors ( ε = ( α − 1) × 1000, where α is the fractionation factor) were identical within uncertainty for experiments with and without CuCl 2 (−2.72 ± 0.67‰ and −2.92 ± 0.14‰, respectively). When added to the cell cultures, neutral red (NR) functioned as an electron carrier that enabled bacteria to drive the electron transfer processes. The ε values were also similar for experiments with and without NR (−2.53 ± 0.40‰ and −2.92 ± 0.14‰, respectively). We compared these ε values to investigate the effects of different electron transport pathways and cellular Cr(VI) transfer processes, including Cr(VI) transport across the cell envelope and binding to reacting enzymes, on Cr isotope fractionation. Furthermore, the effects of various environmental parameters on Cr isotope fractionation were tested, including temperature (50 °C and 70 °C), hydrogen concentration, and different electron donors (glucose and hydrogen). The ε values were similar at both tested temperatures and stayed within the previously observed range for mesophiles ; changes in hydrogen concentration also did not affect the ε values. However, the ε values were slightly higher with hydrogen as the electron donor (−3.64 ± 0.24‰) than those with glucose as the electron donor (−2.92 ± 0.14‰). In short, the Cr enrichment factors remained unchanged despite of changing microbial Cr (VI) reduction pathways and changing temperature conditions, but may be sensitive to the electron donor type.
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ANALYTICAL SCIENCES
·
2017
·Vol. 33
·期 8
·963-967
·
IF 1.228
Sui Ning,Liu Fengya,Li Tailing,Wang Lina,Wang Tao,Liu Manhong,Yu William W.
Au nanoparticles (AuNPs) dispersed in water were stabilized by tripolyphosphate (P 3 O 10 5- ). When Cr 2 O 7 2- (Cr(VI)) was present, the AuNPs did not change; when Cr 3+ (Cr(III)) was present, the AuNPs would aggregate because of cooperative metal-ligand reaction. Aggregated AuNPs showed different color from the non-aggregated ones. Thus, a simple colorimetric assay was made using AuNPs-Cr(VI) to detect ascorbic acid (AA). Upon introducing AA to the AuNPs- Cr(VI) system, Cr(VI) was reduced to Cr(III), and the aggregation of AuNPs occurred. This colorimetric assay performed high selectivity and a linear concentration response in the range of 0.2 to 10 μM; its limit of detection was 0.15 μM.
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INORGANICA CHIMICA ACTA
·
2019
·
IF 2.433
Zhongbao Liu,Wenqi Gao,Xin Qi,Fengfei Lou,Huiwei Lang
In this article, MIL-101(Cr) powder material was successfully prepared by hydrothermal synthesis and combined with different mass fractions of CaCl 2 by immersion method to obtain MIL-101(Cr)/CaCl 2 composite materials. The physical properties of the adsorbent were determined by X-ray powder diffraction, N 2 adsorption/desorption isotherm, TGA and FTIR. The water vapor adsorption performance of MOFs was tested by a gravimetric instrument to analyze the underlying mechanism. Results indicated that the specific surface area, total pore volume, and pore size distribution of micropores and mesopores of MIL-101(Cr)/CaCl 2 composites decreased with increasing CaCl 2 content. When P/P 0 = 0.9, the water vapor equilibrium adsorption capacities of MIL-101(Cr), MIL-101(Cr)/CaCl 2 -10%, MIL-101(Cr)/CaCl 2 -20%, and MIL-101(Cr)/CaCl 2 -30% were 1.05, 0.88, 1.13, and 1.35 g/g, respectively. MIL-101(Cr)/CaCl 2 -30% agglomerated after water absorption, so MIL-101(Cr)/CaCl 2 -20% was selected as the final experimental material. The water vapor adsorption heat of MIL-101(Cr)/CaCl 2 -20% was 42–58 kJ/mol, which is close to the evaporation enthalpy of water (44 kJ/mol at 25 °C). The analysis of the adsorption kinetics showed the relatively uniform adsorption rate of MIL-101(Cr)/CaCl 2 -20%. Overall, MIL-101(Cr)/CaCl 2 -20% exhibited superior water vapor adsorption performance and have great potential for application to adsorption heat pumps.
研究领域:
材料科学
·
化学工程
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