CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Dengjia Shen,Hongyang Ma,Madani Khan,Benjamin S. Hsiao
Both plastic (e.g., polyvinyl chloride (PVC)) solid waste and bacteria/heavy metal ions-containing wastewater pose a severe threat to the environment, which must be addressed simultaneously by developing highly efficient and sustainable strategies. Novel cationic PVC nanofibrous membranes with high filtration and adsorption capability were fabricated by electrospinning and surface grafting, and then employed for the removal of bacteria (e.g., E. coli ) and hexavalent chromium (Cr (VI)) ions for wastewater treatment. A cationic pendant, methylimidazolium, was covalently anchored on the surface of PVC nanofibers and verified using FTIR-ATR, NMR, and SEM measurements. As a result, the optimized cationic PVC nanofibrous membrane (PVC-MIM) exhibited remarkable filtration efficiency for E. coli (LRV ≥ 6.1) from contaminated water, and a maximum adsorption capacity of 285.7 mg/g against Cr (VI). Kinetics, isotherms, and thermodynamics of the nanofibrous PVC-MIM membrane in the adsorption process were extensively investigated. The separation mechanism was proposed based on size exclusion, charged interactions, and hydrogen bonding/coordination between the membrane and the targets. Used sewer pipes and electric cables were employed as raw materials to fabricate modified nanofibrous membranes (0.9 g) to then manufacture of a spiral-wound PVC-MIM nanofibrous membrane cartridge. The resulting system exhibited a retention rate as high as 100 % when 24 L of simulated tanning wastewater containing concentrated suspended solids, oil, ammonia–nitrogen, chloride, and other pollutants were tested for a dynamic adsorption process. Furthermore, the nanofibrous membrane cartridge could be recycled ten times while the regeneration ratio remained as high as 91.0 %.
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Materials Today Communications
·
2023
·
IF 3.8
Ruoning Chu,Xiaojie Guo,Yongjun Zhang,Xiaoyu Zhao,Xiantao Xiong,Xiujuan Zhang,Fengyi Zhang,Kun Zhang,Yaxin Wang
Water containing heavy metal ions can be extremely harmful to the environment and human body, thus the development of low-cost and high-efficient adsorbents has an exciting prospect. In this study, lignin/graphene aerogels modified with polydopamine and polyethyleneimine , respectively, were successfully prepared to remove Cr(VI) from aqueous waste. The physicochemical properties of graphene aerogels (GA), lignin/graphene aerogels (LGA), polydopamine-modified lignin/graphene aerogels (LGA@PDA), polyethyleneimine-modified lignin/graphene aerogels (LGA@PEI) were investigated using FT-IR, Raman spectroscopy , XRD , XPS , SEM-EDS, and BET analysis. The results demonstrate that adsorbents have a high specific surface area, an interconnected porous structure, and a large number of oxygen-containing groups, making them particularly favorable for heavy metal adsorption. The effects of GO/lignin ratio, surface modifiers, solution pH, contact time, initial concentration and temperature on the Cr(VI) removal were investigated and compared via batch experiments. Compared with GA (138.74 ± 3.93 mg/g), the adsorption capacity of LGA with GO/LA ratio 40:1 increased to 167.66 ± 4.75 mg/g. Furthermore, the maximum adsorption capacity of LGA@PEI and LGA@PDA rose up to 209.85 ± 3.25 mg/g and 240.39 ± 3.26 mg/mg, respectively. By simulating the experimental data with different kinetic models and isotherm models, the adsorption processes of different lignin-derived aerogels were further explored under various conditions. All types of aerogels fit well with the pseudo-second-order model and Langmuir model. In addition, the XPS results confirm that the chemical reduction of Cr(VI) to Cr(III) also plays a role in the removal of Cr(VI). The results demonstrated that the removal effect of lignin-derived aerogels on Cr(VI) was greatly improved through the multi-functionalized surface modification of LGA with PDA and PEI. Furthermore, the removal efficiency of LGA@PDA and LGA@PEI for Cr(VI) remained stable after repeated regeneration. Therefore, the results of this study indicate that LGA@PDA and LGA@PEI are promising Cr(VI) adsorbents for practical applications in wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Kaini Yang,Xiangyu Wang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu
Nano zero-valent iron (NZVI) is an ideal material for treating chromium (VI). However, the NZVI's low loading and corrosion susceptibility in acidic Cr-containing industrial wastewater is the most pressing issue. Therefore, it is necessary to explore a method to construct novel NZVI composites with high loading, corrosion resistance, and outstanding activity. In this study, green 2-mercaptobenzimidazole (MBI) was employed for the first time as a corrosion inhibitor for NZVI to form a protective coating through chemisorption, thus blocking the corrosion of NZVI by reaction medium. Meanwhile, a novel multiphase green crystallization-assisted pore formation freeze-drying method was constructed to synthesize UiO-66-NH 2 regulated 3D network porous polyacrylonitrile (PAN) cryogel film for stabilizing NZVI, which is intended to remove Cr(VI) effectively and without secondary contamination. The synthesized MBI-Fe 0 @MOF/PAN possessed prominent activity, corrosion resistance, and considerable NZVI loading (45.9 mg/g). The Cr(VI) removal could still reach 82.7 % after 6 cycles, and the level of total dissolved iron ions was lowered to 0.255 mg/L. MBI-Fe 0 @MOF/PAN for rapid removal of Cr(VI) may be ascribed to the synergistic reaction of rapid protonation of MBI and strong reduction of NZVI. This study constructed the MBI corrosion-resistant interface and 3D PAN cryogel film concepts not only to broaden the horizons of designing efficient NZVI catalytic materials but also to promote the development of treatment technologies for acidic Cr-containing industrial wastewater.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
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IF 8.2
Jingjing Zuo,Shenghua Lv,Shan Liang,Shanshan Zhang,Jialin Wang,Dequan Wei,Leipeng Liu
The design and development of a rapid and quantitative method for the detection of heavy metal ions is of great importance for environmental protection. We have prepared a 1,8-Naphthalimide modified cellulose composite fluorescent hydrogel (CENAEA/PAA) with a stereo double network structure. Characterized by excellent hydrogel functional structure and fluorescence detection performance, it can efficiently and selectively identify and detect Cr(VI) with linear quenching in the range of 0–400 μmol/L and detection limit of 0.58 μmol/L for Cr(VI). The results show that the CENAEA/PAA can effectively adsorb Cr(VI) with a maximum adsorption capacity of 189.04 mg/g. Finally, the morphological characteristics , chemical structure, fluorescence properties and adsorption behavior of CENAEA/PAA were analyzed and fitted well with the pseudo-second-order model and Freundlich model. Thus, the present work provides a green and sustainable approach for the synthesis of a functional material that can be used for the detection and adsorption of heavy metal ions.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Yueyang Wang,Mingzhu Jin,Weiwei Lu,Fangfen Jing,Xinyang He,Jianchao Xie,Rongtai Yu
The mechanism from the molecular level and the selectivity for the removal of metal ions from aqueous has become a hotspot in current water treatment . In this study, a sulphydryl-modified hollow polymer adsorbent was designed with intrinsic amine and grafted sulphydryl groups for efficient uptake of Cr(VI), As(III), Cd(II), and Pb(II) by taking advantage of their properties of abundant functional groups, discrete hollow chambers, and high porosity. Interestingly, the benzenoid amine/quinoid imine functional groups have a stronger affinity for Cr(VI) than Cd(II) or As(III) and Pb(II). The formation of approximately 65.7% Cr(III) indicates the redox reaction from Cr(VI) to Cr(III). The electron-donating comes from benzenoid amine and oxidized to quinoid imine or protonated oxidized nitrogen units (-N = + ) with Cr(VI) reduced to Cr(III) for the increase of more than double of quinoid imine and a new functional group of -N = + . Ion exchange between –COO - groups and As(III)/Cd(II), the chelation of –SH groups for Pb(II)/As(III) are plausible mechanisms.
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LANGMUIR
·
2023
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IF 3.9
Yueyang Wang,Weiwei Lu,Fangfen Jing,Mingzhu Jin,Xinyang He,Yuchen Xue,Yajun Hu,Rongtai Yu
The development of efficient adsorbents for heavy metal pollution, especially five toxic heavy metals, has attracted great research interest. Polymer-based adsorbents have aroused research value for their abundant functional groups and high porosity to the ability to capture metal ions. We designed a sulfhydryl-functionalized polymer microcomposite to take up Cr(VI), As(III), Cd(II), and Pb(II). The adsorption capacity achieved was 64.2 mg g–1 for Cr(VI), 44.9 mg g–1 for As(III), 35.5 mg g–1 for Cd(II), and 18.2 mg g–1 for Pb(II). Langmuir and Sips isotherm model is dominant for As(III), Cd(II), and Pb(II) adsorption. Pseudo-second-order kinetic models can better describe the adsorption behavior of Cr(VI), implying that chemisorption is accompanied by Cr(VI) adsorption. Cr(VI) simultaneous reduction to Cr(III) through the benzenoid amine oxidate pathway was the dominant mechanism, precipitation for Cd(II) adsorption was convinced, and chelation between As(III)/Pb(II) and─SH group and complexation between Pb(II) and C═O or benzene hydroxyl were a plausible mechanism for As(III) and Pb(II) adsorption.
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高影响因子
MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 3
·1-12
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IF 5.833
Yao Chixuan,Liu Qingrun,Zhao Ning,Liu Jing-Min,Fang Guozhen,Wang Shuo
A simple dual-colour fluorescent nanoprobe has been designed composed of blue and yellow emission carbon quantum dots (CQDs). This system is inexpensive and easy to operate and was successfully employed for on-site measurements based on a smartphone app. The designed nanoprobe exhibited increased selectivity for Cr(VI), leading to a double stable response of the two CQDs. The dual-emission nanoprobe showed blue-violet fluorescence upon UV irradiation, and the fluorescent emission peaks were located at 418 nm and 552 nm. The blue light emission of CQDs was quenched with increasing Cr(VI) concentration due to the inner filter effect, whereas the yellow light emission was enhanced due to the aggregation-induced emission effect. The different responses of the dual emissions to Cr(VI) resulted in a fluorescent colour variation, thus enabling facile macroscopic visualization. With a smartphone, the change in the fluorescence colour could be observed more apparently than that of a single fluorescence nanoprobe, and the response increased linearly so that the nanoprobe could be applied to instantaneous measurements. Furthermore, the dual-emission nanoprobe was successfully employed for analysing food and water samples. Accurate concentrations were obtained by constructing a calibration plot using a fluorescence spectrometer and a smartphone app; the recoveries were 81.6% to 107.7%, and the relative standard deviation was below 3.6%. Therefore, this smartphone-integrated dual-emission detection system is promising as a new portable method for the on-site measurement of Cr(VI) ions. Graphical abstract
* Y-CQDs: yellow emission carbon quantum dots. B-CQDs: blue emission carbon quantum dots. B/Y-CQDs: a mixture of B-CQDs and Y-CQDs.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chen Wang,Chao Xiong,Yali He,Chen Yang,Xiteng Li,Jianzhong Zheng,Shixing Wang
A novel magnetic Zr-MOF named Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI was synthesized by modifying UiO-66-NH 2 with Ni 0.6 Fe 2.4 O 4 and polyethyleneimine and its sorption characteristics for two representing heavy metals Pb(II) and Cr(VI) in water were examined. This material showed good thermal stability and was sufficiently magnetic to allow effective solid-liquid separation. The material had a maximum adsorption capacity of 273.2 mg/g for Pb(II) at pH 4.0 and 428.6 mg/g for Cr(VI) at pH 3.0, as obtained from the model fitting by the Hill equation. The sorption kinetics for both heavy metals on the material was fast, with adsorption equilibrium established in 60 min and 30 min for Pb(II) and Cr(VI), respectively. Model fitting of the kinetic data showed that Pb(II) and Cr(VI) sorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI followed the pseudo-second-order model. This material had good selectivity for competing ions, and still hold fairly good binding capacities after 5 times of regeneration. Adsorption mechanisms for Pb(II) and Cr(VI) by Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI were proposed by analyzing FTIR, XPS and the electrokinetic property of the material. Specifically, Pb(II) adsorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be attributed to chelation of Pb(II) with the imine/amine functional groups in the material’s matrix, while Cr(VI) adsorption might stem from a combination of electrostatic attraction, chelation and redox reaction. It seems that Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be used as a green and environmental-friendly material for heavy metals removal, particularly from acidic water streams.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Shifeng Zhao,Zhaosong Li,Haiyan Wang,Hanhan Huang,Caifeng Xia,Derui Liang,Junshan Yang,Qian Zhang,Zilin Meng
Mg-Al layered double hydroxides coated waste textile (MgAl-LDH@WT) was prepared by an in-suit method for the separation of toxic metal ions such as As(V) and Cr(VI) from soil samples. Kinetics studies of As(V)/Cr(VI) removal by MgAl-LDH@WT with different Mg/Al ratio were well described by intraparticle diffusion and pseudo-second-order model. Adsorption isotherm data of As(V)/Cr(VI) yielded a better accordance of Langmuir model, manifesting that accessible adsorption site was the main influence factor and the removal of As(V)/Cr(VI) was a charge-limited process. The adsorption capacity was 69.8 mg/g, 49.8 mg/g, 45.6 mg/g and 38.2 mg/g by Mg 2 Al-LDH@WT, Mg 3 Al-LDH@WT, Mg 4 Al-LDH@WT and LDHs, and for Cr(VI) were 27.5 mg/g, 24.9 mg/g, 19 mg/g and 6.8 mg/g, respectively. Adsorption behavior of As(V) and Cr(VI) co-existing in soil indicated that As(V) possess a preferential adsorption rather than Cr(VI) by Mg 2 Al-LDH@WT, and molecular simulation was selected to explain the results of competitive relationship by bonding energy and variation of bond length. The effect of co-existing ions, column leaching experiment and recycle experiment for practical performance assessment were also examined, and these results revealed a high stability and a good partition capability. The performance of excellent removal and convenient recovery suggested a promising strategy in anionic heavy metals contaminated soil.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Xiangke Han,Peng Li,Maowa Zhang,Jingtao Wang,Yijun Cao,Tong Zhang,Guoli Zhou,Fengli Li
The agglomeration of nanoscale carbon-based material with excellent large specific surface area and numerous active sites remains a challenging, which decreases the adsorption efficiency. Herein, a three-dimensional (3D) half-embedded architecture adsorbent membrane (ES-PAN/AHCNs) was designed to address this weakness by combining the small-sized activated hollow carbon nanospheres （AHCNs） with polyacrylonitrile (PAN) fiber. The 3D architecture precludes the agglomeration of AHCNs, while the half-embedded of AHCNs ensures structural stability of fiber adsorbents. The adsorption capacity and mechanism of ES-PAN/AHCNs membrane were investigated by using metal ions (Pb(Ⅱ), Cu(Ⅱ), Cr(Ⅲ)). Concretely, the adsorption capacity of ES-PAN/AHCNs membrane to Pb(Ⅱ), Cu(Ⅱ) and Cr(Ⅲ) were 192, 186 and 179 mg g −1 , respectively, which was more than two times than that of AHCNs. Noticeably, the significant increase of adsorption capacity mainly benefits from the 3D half-embedded architecture, owing to that pure PAN fiber has negligible adsorption capacity. Moreover, the adsorption capability of ES-PAN/AHCNs membrane retained 82.1% after twelve adsorption-desorption cycles. The strategy of fabricating 3D half-embedded adsorbent membrane substantially expands the potential for AHCNs applications in the adsorption and water purification fields.
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Journal of Environmental Sciences
·
2020
·
IF 4.302
Kai Liu,Fangbai Li,Qingwen Tian,Chengrong Nie,Yibing Ma,Zhenlong Zhu,Liping Fang,Yuanying Huang,Siwen Liu
Paddy soil and irrigation water are commonly contaminated with hexavalent chromium [Cr(VI)] near urban industrial areas, thereby threatening the safety of agricultural products and human health. In this study, we develop a porous and high specific area bone char (BC) to support nanoscale zero-valent iron (nZVI) and apply it to remediate Cr(VI) pollution in water and paddy soil under anaerobic conditions. The batch experiments reveal that BC/nZVI exhibits a higher removal capacity of 516.7 mg/(g•nZVI) for Cr(VI) than nZVI when normalized to the actual nZVI content, which is 2.8 times that of nZVI; moreover, the highest nZVI utilization is the nZVI loading of 15% (BC/nZVI15). The Cr(VI) removal efficiency of BC/nZVI15 decreases with increasing pH (4 – 10). Coexisting ions (phosphate and carbonate) and humic acid can inhibit the removal of Cr(VI) with BC/nZVI15. Additionally, BC exhibits a strong advantage in promoting Cr(VI) removal by nZVI compared to the widely used biochar and activated carbon. Our results demonstrate that reduction and coprecipitation are the dominant Cr(VI) removal mechanisms. Furthermore, BC/nZVI15 shows a significantly higher reduction and removal efficiency as well as a strong anti-interference ability for Cr(VI) in paddy soil, as compared to nZVI. These findings provide a new effective material for remediating Cr(VI) pollution from water and soil.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Mengtian Jia,Yanyan Zhu,Dong Guo,Xiaogang Bi,Xiaohong Hou
Core-shell magnetic Fe 3 O 4 @MIL-101(Cr) nanoparticles were synthesized via layer-by-layer self-assembly method. Using Fe 3 O 4 @MIL-101(Cr) as support, Fe 3 O 4 @MIL-101(Cr)@MIP was prepared with phenytoin as template, acrylamide as functional monomer , ethylene glycol dimethacrylate as cross-linker, methanol and acetonitrile as porogen , azoisobutyronitrile as initiator. The materials were characterized by a serious of characterization experiments. The prepared Fe 3 O 4 @MIL-101(Cr)@MIP was demonstrated to possess good separability, large adsorption capability, excellent adsorption selectivity , good durability and reusability via adsorption experiments. Subsequently, a magnetic solid phase extraction method (MSPE) based on Fe 3 O 4 @MIL-101(Cr)@MIP combined with high performance liquid chromatography-ultraviolet detector (HPLC-UV) was established for the determination of phenytoin sodium in plasma samples. Experimental parameters including pH, the amount of adsorbent, extraction time, elution conditions, the concentration of NaCl were investigated to optimize extraction process. The method was validated. The linearity was observed in the range of 0.05–40 μg mL −1 with a lower limit of quantification of 0.05 μg mL −1 . The calibration equations were y = 0.2514x + 0.0319 ( r 2 = 0.9938), y = 0.2888x + 0.0472 ( r 2 = 0.9943), y = 0.2565x + 0.0418 ( r 2 = 0.9976), respectively. The recoveries ranged from 89.2 to 94.3%, intra- and inter-day precision (RSDs) ranged from 2.1 to 9.7% and 2.9–9.2%, respectively. The established MSPE-HPLC-UV method was time-saving, sensitive, accurate, environmental friendly, and drastically reduced the complex matrix interferences. The established method was successfully applied for phenytoin sodium determination in real plasma samples, providing new directions for therapeutic drug monitoring.
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