Journal of Cleaner Production
·
2023
·
IF 11.1
Zhipan Wen,Shen Li,Ge Zhang,Runqiao Chen,Yalei Zhang,Xiaoping Liao,Gang Cheng,Rong Chen
Magnetic hollow Fe 3 O 4 -based Mg/Al layered double hydroxide (Fe 3 O 4 @SiO 2 @LDH) was successfully synthesized and subsequently the laboratory scale tests were conducted to systematically investigate the sequestration of roxarsone (ROX) and arsenate (As(V)). Owing to its abundant surface metal hydroxyl (M-OH) groups and exchangeable CO 3 2− groups in the interlayer of MgAl-LDH nanosheets , the obtained Fe 3 O 4 @SiO 2 @LDH exhibited remarkable behavior for As(V) and ROX removal. Both As(V) and ROX could be effectively immobilized at a relatively wide pH range (3–8), and the maximum adsorption capacities of As(V) and ROX were 96.47 and 71.67 mg/g, respectively. Meanwhile, the negligible mutual effect demonstrated the Fe 3 O 4 @SiO 2 @LDH can simultaneously remove inorganic and organic arsenic compounds . The competitive cations/anions (except for PO 4 3− ions) and ionic strength were negligible on As(V) and ROX removal, whereas the inhibitory effect stem from humic acid (HA) seemed to be more seriously for As(V) than that of ROX. Adsorption mechanism of As(V)/ROX were attributed to electrostatic attraction and ion/ligand exchange process, whereas hydrogen bonding and π-π interaction may also involve in the ROX removal. Furthermore, the excellent performance in fix-bed column tests and prominent reusability indicated this magnetic Fe 3 O 4 @SiO 2 @LDH was a promising candidate adsorbent and of great potential application in organic/inorganic As-contamination wastewater treatment .
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Analytical Methods
·
2019
·Vol. 11
·期 7
·955-964
·
IF 2.378
Lina Wang,Yong Li,Xike Tian,Chao Yang,Liqiang Lu,Zhaoxin Zhou,Yunjie Huang,Yulun Nie
Arsenic contamination in groundwater is a severe and major environmental problem that endangers public health. As such, a sensitive and selective methodology for the detection of this toxic metalloid must be urgently developed. Aldimine condensation reactions of p-phenylenediamine with salicylaldehyde derivatives yielded “turn-on” fluorescence probes (HBHP, HBBP and HMBP) for the detection of As(V) with high sensitivity. Among these, as a typical AIEgen, HBHP exhibits the highest detection sensitivity. The detection limit of HBHP for As(V) was calculated to be 0.88 ppb, which is due to its higher ability to form intermolecular hydrogen bonds to convert twisted intramolecular charge transfer (TICT) into planar intramolecular charge transfer (PICT) and its higher molecular planarity triggered by specific electronic effects. Job's plots and DFT theoretical studies indicate that HBHP binds to As(V) with a stoichiometry of 1 : 2, and the binding constant was determined using the Benesi–Hildebrand equation to be 4.26 × 104 M2. Commonly existing anions and cations in groundwater exhibited no interference with the selective detection of As(V). Spiking and recovery tests of HBHP in the presence of As(V) in actual water samples gave satisfactory experimental results. Our research would provide novel principles of molecular construction and materials for the detection of As(V) in groundwater.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
·
IF 6.434
Xiaohui Dai,Shuxin Zhang,Geoffrey I.N. Waterhouse,Hai Fan,Shiyun Ai
Layered double hydroxides (LDHs) are very promising adsorbents for the removal of anionic pollutants from water. However, the low adsorption efficiency and recycling difficulty of conventional LDH powders are obstacles to practical applications. Herein, a novel Zn/Fe-LDH composite sponge was successfully fabricated using a simple in-situ hydrothermal method. Characterization studies revealed that the composite sponge contained flower-like Zn/Fe LDH microspheres uniformly dispersed throughout a poly vinyl alcohol (PVA) sponge matrix. The specific surface area of the Zn/Fe-LDH composite sponge was 42.5 m 2 g −1 , approximately 5 times higher than the pristine PVA sponge (8.9 m 2 g −1 ). Adsorption experiments revealed that Zn/Fe-LDH composite sponge exhibited a much higher adsorption ability for As(V) anions and methyl orange (MO) compared with a Zn/Fe-LDH powder or the pristine PVA sponge. The maximum adsorption capacity for As(V) was found to be 85.7 mg g -1 . Furthermore, the Zn/Fe-LDH composite sponge showed high thermal stability, good mechanical stability and easy recoverability, thereby allowing reuse. Results guide the development of improved, low cost water treatment materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xin Ke,HuiPing Shao,HaiHong Liu,Wengang Liu
In this study, an Fe-La-CS adsorbent with a reticulated structure was prepared by an in situ method, which was able to adsorb arsenate efficiently over a wide pH range of 3–11. The incorporation of iron and lanthanum ions broadened the tolerant pH range of the adsorbent compared with chitosan beads (CS). Arsenic was mainly present in the pH range of 3–9 as two forms, H 2 AsO 4 − and HAsO 4 2− . Calculations using the density-functional theory (DFT) showed that in the Ligand interactions and electrostatic interactions dominate in the pH range, with surface precipitation, and hydrogen bonding interactions playing a facilitating role. The background ions mainly compete with arsenic adsorption for electrostatic interaction sites. However, due to the different valence states of the background ions, the competition intensity is different. Such as low valence state representative ions Na + , K + competitiveness is weak, and arsenic competition adsorption first occupy different adsorption sites, therefore, from the quantum chemistry and molecular dynamics point of view of Na + , K + on arsenic adsorption almost no effect. Cl − , SO4 2− will have some influence on arsenic adsorption because of the same charge with arsenic, but the charged amount is smaller than arsenic and the molecular structure is different from that of arsenic, so the influence is not very big. In summary, the material design of Fe-La-CS adsorbent has great potential and theoretical significance for selective purification of heavy metal wastewater at wide pH.
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Desalination and Water Treatment
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2024
·
IF 1
Shifeng Li,Tiankuo Zang,Xiaoyun Yang,Min Xiao,Haibo Wang,Shuhua Yao,Zhongliang Shi
The utilization of waste melamine-formaldehyde foam to produce value-added carbon foam has been identified as a promising approach to polymer recycling. Nickel-Iron layered double hydroxides (NiFe-LDHs) and its complex oxides (NiFe 2 O 4 ) were synthesized in this study through a hydrothermal method, growing in situ on the above-mentioned carbon foam substrate. Comparative analysis revealed that CF@NiFe 2 O 4 exhibited superior removal efficiency compared to CF@NiFe-LDHs. Furthermore, arsenate adsorption on CF@NiFe-LDHs and CF@NiFe 2 O 4 conformed more to the pseudo-second-order model; meanwhile, the isothermal adsorption characteristic fitted the Langmuir isothermal model better. The negative ΔG (free energy changes, <−37.68 kJ/mol) and positive ΔH (enthalpy change, 7.64 kJ/mol) indicate that it is spontaneous and endothermic for As(V) to adsorb on CF@NiFe 2 O 4 . Potential mechanisms such as surface complexation, electrostatic interaction, and hydrogen bonding were suggested. This innovative approach offers a novel method for utilizing LDHs-based adsorption materials and recycling waste polymers.
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Journal of Physical Chemistry C
·
2012
·
IF 4.805
Bang-Jing Zhu,Xin-Yao Yu,Yong Jia,Fu-Min Peng,Bai Sun,Mei-Yun Zhang,Tao Luo,Jin-Huai Liu,Xing-Jiu Huang
Iron and 1,3,5-benzenetricarboxylic (Fe–BTC) metal–organic coordination polymers are synthesized via a simple solvothermal method. The as-synthesized Fe–BTC polymers exhibit gel behavior, which is stable in common organic solvents or in water. The Fe–BTC polymer as an adsorbent for arsenic removal from water is tested. The kinetics and thermodynamics of arsenic adsorption by the Fe–BTC polymer in aqueous solution are investigated comprehensively. The effect of pH on the adsorption is also investigated. Kinetic studies show that the kinetic data are well described by the pseudo-second-order kinetic model. The thermodynamic analysis indicates that the adsorption is spontaneous. The adsorption isotherms can be well described with the Langmuir equation. The Fe–BTC polymers show relatively high arsenic adsorption capacity, more than 6 times that of iron oxide nanoparticles with a size of 50 nm and 36 times that of commercial iron oxide powders. Hence, the as-synthesized Fe–BTC polymers possess relatively high stability and better adsorption characteristic than nanomaterials simultaneously. It also can be considered as a new method to conquer the dilemma between the excellent properties from nanoscale effect and the aggregation of small size particles in the adsorption application of nanoparticle materials.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77851-77863
·
IF 5.19
Jiang Changjin,Zhang Ting,Li Shuhui,Yang Zhaoguang
Fe(III)-chitosan and Fe(III)-chitosan-CTAB composites were prepared using an ionotropic gelation method. Various techniques were used to analyze the morphology, structure, and property of the adsorbents, including SEM, EDS, FT-IR, XPS, and zeta potential. Compared with Fe(III)-chitosan, Fe(III)-chitosan-CTAB was more effective for As(V) adsorption at a wide range of pH (3.0–8.0). The adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB could reach equilibrium in 20 min, and their maximum adsorption capacities were 33.85 and 31.69 mg g ‒1 , respectively. The adsorption kinetics was best described by the pseudo-second-order model ( R 2 = 0.998 and 0.992), whereas the adsorption isotherm was fitted well by the Freundlich model ( R 2 = 0.963 and 0.987). The presence of H 2 PO 4 – significantly inhibited the adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB, and humic acid also led to a slight decrease in As(V) adsorption by Fe(III)-chitosan-CTAB. Over 94% of As(V) at the initial concentration of no more than 5 mg L –1 was removed from real water by the two adsorbents. 1% (w/v) NaOH solution was determined to be the most suitable desorption agent. Fe(III)-chitosan and Fe(III)-chitosan-CTAB still maintained their initial adsorption capacities after five adsorption–desorption cycles. Based on different characterization results, both electrostatic attraction and surface complexation mechanisms played important roles in As(V) adsorption on Fe(III)-chitosan and Fe(III)-chitosan-CTAB.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Longwei Yin,Longjie Liu,Shen Lin,Gary Owens,Zuliang Chen
Arsenic (As) is a contaminant of global concern due to its negative impact on environmental systems, where As occurs mainly as two inorganic species, arsenite (As(III)) and arsenate (As(V)). Thus the simultaneously removal of both As(III) and As(V) from groundwater is a challenging issue. In this paper, zero-valent iron nanoparticles ( n ZVI) with high surface-active sites were used to simultaneously remove both As(III) and As(V) species from groundwater with removal efficiencies >99.9% for an initial concentration 100 μg L −1 . Ion chromatography atomic fluorescence (IC-AFS) analysis indicated that during removal As(III) was oxidized to As(V), while X-ray photoelectron spectroscopy (XPS) showed that the As species were adsorbed on to the surface of n ZVI by a complexation reaction. Furthermore, thermodynamic studies of the adsorption process indicated that adsorption was a spontaneous and endothermic chemisorption process. Finally, practical removal of both As species by n ZVI from real groundwaters was demonstrated with removal efficiencies of 99.9 and 70.9% for As(V) and As(III), respectively. The presence of other coexisting ions affected the removal efficiency, with phosphate and carbonate decreasing the removal efficiencies of both As(III) and As(V) due competition with active binding sites on the surface of n ZVI. Overall, this work demonstrated that n ZVI was a promising adsorbent for the practical removal of inorganic As species from complex environmental matrices such as groundwater.
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CHEMOSPHERE
·
2018
·
IF 4.427
Zhipan Wen,Yalei Zhang,Gang Cheng,Yingru Wang,Rong Chen
In this study, nanosized ordered magnetic mesoporous Fe-Ce bimetal oxides (Nanosized-MMIC) with highly well-ordered inner-connected mesostructure were successfully synthesized through the KIT-6 template method. This Nanosized-MMIC displayed excellent adsorption capacities for As(V), Cr(VI) and AO7, and the corresponding calculated maximum adsorption capacities of material were 111.17, 125.28 and 156.52 mg/g, respectively. As(V) and Cr(VI) removal by Nanosized-MMIC were slightly dependent on the ionic strength but highly solution pH-dependent, the coexistent silicate and phosphate ions competed remarkably with both As(V) and Cr(VI) for the adsorption active site. Mechanisms indicated As(V) and Cr(VI) formed inner-sphere complexes on Nanosized-MMIC interface via the electrostatic interaction and surface complexation, while the total organic carbon (TOC) change demonstrated that AO7 could be removed completely and no organic intermediates formed through the adsorption process. In addition, Nanosized-MMIC also possessed superior adsorption performance in As(V)/Cr(VI)-AO7 binary systems, and the reusable and regeneration properties indicated that the obtained nanomaterials could maintain at a comparatively high level after several recycling. Finally, fixed-bed experiments suggested the Nanosized-MMIC was expected to have a promising excellent nano-adsorbent with high application potential for co-existed toxic heavy metals and organic dyes removal in practical wastewater treatment .
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TALANTA
·
2016
·
IF 4.035
Qingxiang Zhou,Zhenwen Zheng,Junping Xiao,Huili Fan
The magnetic nanomaterial Fe@polyethyleneimine (Fe@PEI) was successfully synthesized and used as an effective adsorbent material for magnetic solid phase extraction(MSPE) of As(III) and As(V) from water samples. Fe@SiO 2 nanoparticles were prepared by one pot synthetic method using a borohydride reduction method, then modified with (3-chloropropyl)trimethoxysilane to obtain Fe@SiO 2 -Cl by chloropropylation, which was reacted with PEI to achieve Fe@polyethyleneimine (Fe@PEI). The microstructure and morphology of Fe@PEI were characterized by transmission electron microscoscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), and X-ray diffraction (XRD). The experimental results showed that Fe@PEI demonstrated excellent adsorption for As(III) and As(V). Based on this fact, the determination method for these two arsenic species earned good limits of detection (LODs) of 0.002 μg L −1 and wide calibration curves in the concentration range from 0.008 to 0.2 μg L −1 . The precisions of As (III) and As (V)were 1.95% and 2.55% (RSD, n =6), respectively. The proposed method was validated with real samples and the spiked recoveries were in the range of 82.7–98.3% and the accuracies were in the range of 2–13.3%. The results demonstrated that the developed MSPE method had good advantages such as simplicity, rapid separation, low cost, easy to reuse and high-quality analytical performances, which made it attractive for rapid and efficient extraction of inorganic arsenic species in the environmental water samples.
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Environmental Science-Nano
·
2018
·Vol. 5
·期 11
·2570-2578
·
IF 6.087
Xinwen Ou,Xueming Liu,Weizhen Liu,Wencong Rong,Jingyuan Li,Zhang Lin
The surface defects of adsorbents are generally considered to be the active sites for adsorbates, and the adsorption behaviors of a variety of pollutants in wastewater are strongly influenced by the surface defects of the adsorbents. With simple chemical and structural properties, nano-Mg(OH)2 exhibits a high adsorption affinity and selectivity to heavy metals from wastewater. The insight into the surface complex structures of heavy metals on the Mg(OH)2 surface is fundamental for both the mechanism and application of defective adsorbents in wastewater treatment. In this study, the impact of surface defects of Mg(OH)2 nanoplates on the structure, energy, and adsorption amounts of toxic heavy metal oxyanions (HAsO42− and CrO42−) was investigated by combining the first-principles calculations and batch experiments. The first-principles calculations illustrated that the heavy metal oxyanions can be steadily incorporated into the surface defects to form inner-sphere complexes. The incorporated heavy metal oxyanions have strong charge–charge and chemical bonding interactions with the surface defect sites, which are much stronger than the hydrogen bonding interactions with the surface OH sites. Moreover, the adsorption affinity of surface defects towards heavy metal oxyanions is stronger than that towards other oxyanions (e.g. SO42− and NO3−), indicating the high adsorption selectivity of heavy metal oxyanions over other oxyanions. Batch adsorption experiments verified that the adsorption of defect-rich Mg(OH)2 adsorbents towards heavy metal ions, e.g., As(V) and Cr(VI), was favorable even under the condition of low concentration (mg L−1 level). These findings reveal the significance of surface defects of Mg(OH)2 for extracting As(V) and Cr(VI) from low-concentration solutions. The proposed strategy of surface defect-fabrication should provide a useful insight into designing effective adsorbents for the selective extraction of heavy metal oxyanions at low concentration.
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JOURNAL OF POLYMER RESEARCH
·
2016
·Vol. 23
·期 9
·1-9
·
IF 1.969
Kong Zhiyun,Wu Xiaoqing,Wei Junfu,Zhang Huan,Cui Li
The hydrophilic fibers based on 2-(dimethylamino)ethyl methacrylate (DMAEMA) which could remove Cr(VI) ions rapidly were prepared by UV-irradiation induced grafting of DMAEMA through pre-coating photoinitiator on the fibers and modifying with bromoethane(BE). The FTIR, FESEM, XPS, TG-DTG and contact angle spectra manifested that DMAEMA was grafted onto the surface of PP fibers and subsequently was quaternized. The maximum grafting degree (22.9 %) and exchange capacity of DMAEMA (1.2 mmol g −1 ) was obtained when PP fibers was immersed in BP concentration of 0.3 % for 4 h, irradiated with the DMAEMA concentration of 100 % and irradiation time of 20 min, and then was modified with BE. The modified fibers of PP-g-DMAEMA with bromoethane were proved to remove Cr(VI) and As(V) with removal rate of 97.3 % and 96.2 % within 10 min, respectively. The prepared fibers have potential application for the removal of Cr(VI) and As(V) from wastewater highly and rapidly.
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