APPLIED SURFACE SCIENCE
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2016
·
IF 3.15
Jie Su,Weiyuan Yao,Yue Liu,Zhongbiao Wu
A series of HZSM-5 supported CrO x catalysts at different loadings were prepared by wet impregnation method for catalytic combustion of dichloromethane (DCM) in this paper. The catalytic activity tests indicated that both DCM conversion and product selectivity varied greatly with Cr doping contents. The sample at 2 wt% loading showed the highest DCM conversion, while the selectivity toward CO/CO 2 increased at an elevated CrO x loading. The characterization results revealed that the surface acidity and the chemical states of Cr were strongly affected by the doping content. The surface acidity would decline at an elevated Cr loading owing to the interactions between surface OH groups and chromium ions. And higher surface Cr(VI)/Cr(III) ratios could be observed on the catalysts at lower CrO x doping, leading to the improvement of reducibility. The activity and selectivity of DCM catalytic degradation were found to be highly depended on the balance of surface acidity and redox property. The increased surface acidity could result in the enhancement of dissociated adsorption of DCM, which are beneficial to the catalytic activity. However, higher surface acidity meant lower Cr loading, which might lead the adsorbed intermediates incompletely oxidized and the decrease in CO x selectivity due to the limit redox ability.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Jingfang Guo,Guodong Wang,Jing Zou,Zhen Lei
In this work, chitosan modified cuprous oxide nanoparticles (Cu 2 O/CTS NPs) with Cr(VI)-specific oxidoreductase-like activity were facilely synthesized via one-step reduction method. In the presence of Cr(VI), colorless 3,3′,5,5′-tetramethylbenzidine (TMB) was rapidly oxidized to blue colored oxTMB with the aid of Cu 2 O/CTS NPs. Systematic studies including steady-state kinetics analysis, X-ray photoelectron spectra (XPS) analysis, radical trapping experiments and photoluminescence spectroscopy were conducted to investigate the catalytic mechanism, which was verified to be electron transfer and active species-involved redox reaction. Based on promoted catalytic oxidation of TMB, a selective and sensitive colorimetric method for fast detection of Cr(VI) was proposed. Under the optimal conditions, this colorimetric method exhibited a wide linear range (0.01–35 μM), low limit of detection (0.5 nM) and short assay time (1 min). In addition, test strip for visual detection of Cr(VI) was constructed by processing the Cu 2 O/CTS NPs+TMB+Cr(VI) sensing system on paper. With the aid of smartphone, a detection limit of 312 nM was achieved within 5 min, showing great potential for on-site detection. Moreover, the method was applied to detect Cr(VI) in spiked tap and lake water samples, the good recoveries (96.10%−103.13%) and low relative standard deviations (1.03%−3.25%) demonstrated the feasibility of the assay.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Fenglei Liu,Linkai Si,Baowei Hu
Herein, we proposed a novel chitosan-induced self-assembly strategy to construct three-dimensional magnetic MXenes/chitosan composites to eliminate U(VI)/Cr(VI). Spectroscopic analysis elucidated that the magnetic composites exhibited a three-dimensional network structure, and the abundant –OH and –NH 2 groups played a pivotal role in boosting elimination performance of the composites. Batch experiment demonstrated that the synergistic effect of the amino and hydroxyl groups contributed greatly to adsorption, and the maximum adsorption capacity of U(VI) and Cr(VI) was up to 106.2 and 83.1 mg/g, respectively. Meanwhile, the kinetic studies showed that an obvious transition between diffusion control and mass transfer control, and the adsorption behavior was endothermic and spontaneous. Furthermore, a comprehensive synergistic adsorption mechanism was proposed based on the systematic spectra analysis. Namely, the target contaminant was rapidly immobilized on the 3D composites via electrostatic interaction, then the U(VI) was complexed with the amino groups, while a part of Cr(VI) was reduced to Cr(III) by the hydroxyl groups. Thus, this study not only paved the way for mitigating the increasing heavy metal/radionuclide contamination, but also promoted the application of MXexes-based materials in the field of environmental remediation.
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TALANTA
·
2017
·
IF 4.162
Li Liang,Xinghua Wang,Ying Sun,Pinyi Ma,Xinpei Li,Huilan Piao,Yanxiao Jiang,Daqian Song
The metal-organic framework (MOF) functionalized magnetic graphene oxide/mesoporous silica composites (Fe 3 O 4 @SiO 2 -GO/MIL-101(Cr)) were synthesized and utilized as magnetic solid-phase extraction (MSPE) adsorbent for the extraction of seven triazine herbicides (terbuthylazine, secbumeton , terbumeton , atraton , atrazine , prometon and trietazine) in rice samples. Several experimental parameters, including type and volume of extraction solvent, amount of MIL-101(Cr), extraction time, volume of desorption solvent and desorption time were investigated and optimized. The limits of detection (LODs) of seven triazine herbicides obtained by using the proposed MSPE method combined with high performance liquid chromatography (HPLC) were in the range of 0.010–0.080 µg kg −1 . The recoveries of the triazine herbicides in spiked rice samples ranged from of 83.9–103.5% with the relative standard deviations lower than 8.7%. The intra and inter-day (n = 6) precisions for all triazine herbicides at the spiked level of 100.0 µg kg −1 were 1.4–5.9% and 2.6–7.8%, respectively.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2017
·
IF 3.154
Tiantian Luo,Xike Tian,Chao Yang,Wenjun Luo,Yulun Nie,Yanxin Wang
In this study, polyethylenimine-functionalized corn bract (PEI–CB) was first used to remove aqueous Cr(VI) via the “waste control by waste” concept. The results indicated that PEI–CB had an excellent performance for Cr(VI) removal and the maximum removal capacity was 438 mg/g. The adsorption of Cr(VI) was fitted to the Langmuir model, and kinetics of uptake could be described by a pseudo-second-order rate model well. Amine was proven to be the active center for Cr(VI) adsorption and partial reduction to Cr(III), while removal efficiency was enhanced at a lower pH value and higher temperature. Besides, nanosized Cr2O3 with a high purity was obtained by simple calcination of a Cr(VI)-laden adsorbent. Hence, this study provided a novel strategy for Cr(VI) wastewater remediation and pure Cr2O3 recovery. Prepared PEI–CB was then a promising alternative of low cost for replacement of the current expensive absorbent of removing Cr(VI) from wastewater from the view of sustainability.
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Processes
·
2025
·Vol. 13
·期 1
·156
·
IF 2.8
Ting Guan,Liang Fang,Fang Wu,Yongxia Yang
NiFe-layered double hydroxide (NiFe-LDH) and La-, Mo- or W-doped NiFe-LDH microparticles (NiFeX-LDH, X = La, Mo, W) were synthesized via the co-precipitation method. Their adsorption characteristics were evaluated by the removal of methyl orange (MO) and hexavalent chromium (Cr6+). The effects of the metal ion doping type, doping concentration (0–3at%), pH and temperature on the MO adsorption properties were systematically studied. The results show that W-doped NiFe-LDH exhibits superior MO removal capacity compared to undoped or La- or Mo-doped NiFe-LDH at the same 1at% doping level, which is attributed to the increased layer charge density and strong affinity for the π-electron systems of MO molecules. The NiFeW-LDH-1at% sample demonstrated the best MO adsorption performance within the W-doping range of 0–3at%, achieving a superior adsorption capability of 666.67 mg/g with a significantly shorter equilibrium time (10–120 min) compared to the similar LDH. NiFeW-LDH-1at% showed promising reusability, with its adsorption efficiency remaining 78.3% of its initial level after five adsorption–desorption cycles. The MO uptake onto NiFeX-LDH was attributed to the combined effect of anion exchange and the attraction of layer charge. In addition, the adsorption of NiFeW-LDH-1at% matched well with the Langmuir isotherm model and pseudo-second-order kinetic model, indicating a monolayer and chemical adsorption. Furthermore, NiFeW-LDH-1at% effectively adsorbed of Cr2O72−in the aqueous solution, revealing that W doping significantly enhances Cr(VI) removal performance. The maximum theoretical adsorption capacity onto NiFeW-LDH-1at% reached 63.25 mg/g, which was notably higher than that of the pristine NiFe-LDH adsorbent (53.56 mg/g). Overall, the W-doped NiFe-LDH material, as a low-cost and highly efficient adsorbent, shows great potential for wastewater treatment application.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Tian Zhao,Saiqun Nie,Pengcheng Xiao,Shilin Peng,Jiayao Chen,Jiangrong Yu,Fuli Luo,Yi Chen
The formation of zinc dendrites and by-products significantly affects the cycling performance of aqueous zinc-ion batteries (AZIBs). This study presents the first application of MIL-101(Cr) as a separator material in AZIBs, investigating the impact of various MIL-101(Cr) morphologies in cellulose-based separators on battery performance. The findings demonstrate that separators incorporating spherical MIL-101(Cr) morphology considerably enhance ion conductivity and the transport rate of Zn 2+ ions while effectively inhibiting corrosion reactions and dendrite growth. Notably, the spherical MIL-101(Cr)-based separator exhibited more than double the cycle life of Zn//Zn symmetric cells compared to those made from octahedral and nano-fusion morphologies, achieving over 750 h of operation. Additionally, a Zn//MnO₂ full cells utilizing this separator achieved a remarkable capacity retention of 83.6 % after 400 cycles, with a close-to-100 % Coulombic efficiency. This research underscores the critical role of MIL-101(Cr) morphology in enhancing the performance of AZIB separators, paving the way for innovative designs in future metal-organic framework (MOF)-based separators.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 8
·1-12
·
IF 5.3
Ruan Ya,Li Qiulan,Yang Dezhi,Yang Yaling
Copper selenide nanoparticles (CuSeNP) were synthesized using histidine, ethylenediamine, and sodium selenate as precursors by one-step microwave digestion methods. The as-prepared CuSeNPs exhibit excellent catechol oxidase mimic enzyme and catalase (CAT)-like activities. Dopamine (DA) can be oxidized to aminochrome with H 2 O 2 by CuSeNPs, and the intermediate product aminochrome can further react with α -naphthol to yield a highly fluorescent derivative. It was confirmed that Cr(III) could adsorb on the surface of CuSeNPs and inhibit the production of semiquinone radicals in the reaction system, and the catalytic activity of CuSeNPs was inhibited. The detection mechanisms, kinetics, and catalytic properties of CuSeNPs were systematically investigated. As a result, a novel fluorescence method for the assay of Cr(III) was established. The feasibility of CuSeNP nanozyme in detecting speciation Cr(III) in food samples was explored with satisfactory results. It showed the obvious potential for developing effective and dependable fluorescent detection method for protecting food safety. Graphical Abstract
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TALANTA
·
2024
·
IF 5.6
Shengyuan Zhang,Haiyan Li,Dezhi Yang,Yaling Yang
In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)–NH 2 ) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)–NH 2 performs dual functions: the 2-aminoterephthalic acid (NH 2 -BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3′,5,5′- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)–NH 2 because of the reduction of Fe 3+ by AA, resulting in release of NH 2 -BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)–NH 2 + AA system will be decreased due to the competitive reduction of Fe 3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)–NH 2 as it boosts the electron transfer rate between Fe 3+ and Fe 2+ . Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5–750 μg/L and 13.3–1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuxin Wang,Yueqi Chen,Fengjun Shan,Tingting Zhang,Zhenbin Zhang,Meijun Liu
Hexavalent chromium (Cr(VI)) pollution in aquatic environments has triggered constant worries. As one of the popular adsorbents, graphene oxide (GO) still confronts shortcomings in the Cr(VI) removal, including easy aggregation, limited adsorption amounts, monotonous type of functional groups, constant negative charge and unable valence conversion. Herein, L-glutamic acid (L-Glu) was utilized for GO functionalization through the solvothermal method to fabricate L-Glu/GO with the trait of anti-stacking for overcoming the above-mentioned drawbacks. Results proved that L-Glu/GO possessed the relatively large specific surface area and average pore diameters, various functional groups and variable surface charges. The as-prepared L-Glu/GO exhibited satisfying adsorption amounts with the changeable acid environment, adsorbent dosages and initial Cr(VI) concentrations. Besides, Cr(VI) adsorption process conformed to the pseudo-second-order kinetic model and the Langmuir isotherm model with q m for Cr(Ⅵ) of 71.12 mg·g –1 , almost 27 times higher than that of GO (2.64 mg·g –1 ) in pH = 2. The adsorption thermodynamics result portrayed the adsorption process was a spontaneous endothermic process. Additionally, L-Glu/GO possessed excellent reusability with q e of Cr(Ⅵ) of 57.19 mg·g –1 after five cycles, with the economic cost of ¥0.498·g –1 . More importantly, Cr(VI) was changed into Cr(III) during adsorption to accomplish the toxicity elimination due to existence of amine groups from L-Glu. On the whole, pore filling, anion-π interaction, electrostatic interactions, adsorption-reduction and coordination interaction jointly contributed to the Cr(VI) adsorption. This work provided the strategy for effectively enhancing the Cr(VI) adsorption capacity of GO and deepened the adsorption mechanism towards hazardous metal ions elimination.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tong Hu,Wenjun Zhou,Haijiao Xie
Lattice engineering of Fe 0 based on heteroatom doping holds great promise in water purification owing to their tunable geometric and electronic structure. However, there is limited understanding of how nitrogen atom in Fe 0 lattice structure affects its local microenvironment and corresponding reactivity toward target contaminants. Herein, microscale zero-valent iron with interstitial N doping (N-mZVI) was successfully prepared by a facile mechanochemical method for heavy metal pollution control. N-mZVI exhibited excellent reactivity for Cr(VI) elimination, and both removal efficiency and conversion rate could reach 100 %, which was 8.06 and 2.73 times higher than that of pristine ball milled mZVI, respectively. Besides, the rate constant of various heavy metals sequestration (Cr(VI), Ni(II), Pb(II), Cu(II), and Cd(II)) over N-mZVI was 61.3 ∼ 115.6-fold faster than that of pristine ball milled mZVI. N-mZVI was also demonstrated to be pH-universal, long-term stability, and environmental applicability. Experimental results and theoretical calculations indicated that tensile strain induced by interstitial N doping expanded Fe 0 lattice and weakened the lattice Fe-Fe interaction, thus significantly accelerating electron transport dynamics in Fe 0 core. Meanwhile, iron nitride species on the surface of N-mZVI promoted electron transfer from iron shell layer to heavy metals. This work comprehensively investigates the structure–property relationships of lattice engineering-based N-mZVI, and provides a new insight into rational design of modified mZVI with high reactivity.
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