JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Xize Min,Caiyun Han,Liu Yang,Chundi Zhou
Fly ash and arsenic species have been regarded as contaminants that pollute the environment. Herein, low alumina fly ash (LAFA) was utilized to fabricate the As(V) and As(III) adsorbent via combining the routes of alkali fusion and incipient-wetness impregnation. The characterization results suggested that the grafted ferric citrate was coordinated to LAFA by substituting a Si 4+ to a Fe 3+ , and the compound monosodium citrate was observed. Based on the XPS analysis , the C–O and –COO - groups of monosodium citrate played the significant role in uptaking As(V) and As(III) species by chemical complexation, the FeOOH adsorbed As(V) and As(III) species via ion-exchange, and the Fe 2 O 3 oxidize As(III) into As(V). Additionally, it was observed that the As(V) removal performance by adsorbent prepared with different modifiers was in the order of FeC 6 H 5 O 7 (ca. 93.7%) > C 6 H 8 O 7 (84%) > HCl (73%). And then, the optimal adsorbent synthesis condition for As(V) uptake was explored at ferric citrate loaded LAFA with 1:1 mass ratio (fly ash to NaOH) under temperature 923 K. The maximum monolayer adsorption capacities of the optimal adsorbent were 2725.0 μgAs(V)/g and 2281.9 μgAs(III)/g, and the removal efficiency of As(V) and As(III) was near 100% for their initial concentrations below 500 ppb, where the residual arsenic concentration met the required standard in drinking water (lower than 10 ppb).
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Journal of Water Process Engineering
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2022
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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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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Huimin Hu,Qiwu Zhang,Chao Wang,Min Chen,Qian Wang
Soluble Fe(IV) has been proposed as primary reactive species in advanced oxidation technology, however, Fe(IV) in solid-state oxidant is rarely reported. This study reports a facile synthesis of CaMn 1-x Fe x O 3 (0.1 ≤ x ≤ 0.7) containing high ratio of Fe(IV) by low-temperature calcination of the ball milling precursor and evaluates its adsorption-oxidation performances of As(III). Although Fe(IV) and Mn(IV) inside CaMn 1-x Fe x O 3 both act as electron acceptor species, with × for Fe ratio increased, charge transport capability and oxidation performance of As(III) to As(V) of the CaMn 1-x Fe x O 3 materials can be raised dramatically with more iron incorporated. With sample CaMn 0.3 Fe 0.7 O 3 , the maximal adsorption capacity for As(III) reaches 120.78 mg/g with the ratio of oxidized As(V) as high as 86.4% in a wide pH range of 2 ∼ 10. More importantly, excellent cyclability and stability are observed and 83% of the initial adsorption-oxidation capacity still retains even after 5 cycles, and leaching concentrations of the metal ions (Fe/Mn) are far below the emission standard (0.5 mg/L). With an aid of environment-friendly ball milling process, the idea to obtain high valent Fe by a simple incorporation into a specific crystalline structure of perovskite offers a new approach for synthesizing active oxidizing species of Fe(IV). Further, the synthesis of solid oxidants would transform the redox reactions from a liquid phase reaction process to a solid–liquid reaction process, which could be conducive to the occurrence of in-situ oxidation and fixation of pollutants to reduce their mobility, and much contribution is expected to the development of advanced oxidization process in wastewater treatment using the easy handling solid-state oxidants.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Guiyuan Cai,Yu Tian,Daikun Li,Jun Zhang,Lipin Li,Qinyu Wang,Huihang Sun,Haoran Zhang,Pu Wang
Here, we prepared a novel nanostructured Fe–Cu–Mn composite oxide (FCMO x ) adsorbent using an ultrasonic coprecipitation method. The maximum adsorption capacity of As(III) and As(V) reached 158.5 and 115.2 mg/g under neutral conditions, respectively. The effects of several environmental factors (coexisting ions, solution pH, etc.) on the removal of inorganic arsenic using FCMO x were studied through batch experiments. The results showed that except for PO 4 3– and high initial pH, it was not significantly affected by ionic strength and other existing anions, implying a higher selectivity and adaptability. Combined with EPR, FTIR, and XPS analysis, we concluded that the Cu component and the reactive oxygen species (ROS) it generates played a decisive role in maintaining the stability of the redox cycle between Mn(IV)/Mn(III)/Mn(II) and enhancing the oxidation efficiency of As(III). Meanwhile, the adsorption mechanism of As(V) was mainly through the replacement of the FCMO x surface –OH to form stable inner-sphere arsenic complexes, while the removal mechanism of As(III) may involve the process of synergistic oxidation and chemisorption coupling. Additionally, the effective removal of As from the simulated As-contaminated water and its satisfactory reuse performance make FCMO x adsorbents favorable candidates for the removal of As-contaminated water in the future.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Huimin Hu,Qiwu Zhang,Chao Wang,Min Chen,Mengfei Chen
Iron manganese oxide resources are widely derived from the geological structure , and their combinations play an important role in the migration and transformation of arsenic. Iron oxide and manganese oxide exist generally in a mixed state in Fe-Mn oxides synthesized via the well studied co-precipitation methods using potassium permanganate and manganese/iron sulfates. Herein, a newly designed Fe-Mn-O compositing oxide with Fe-MnO 2 , Mn-Fe 2 O 3 , (Fe 0.67 Mn 0.33 )OOH solid solution and FeOOH as the main components, simply through solvent-free mechanical ball milling pyrolusite (MnO 2 ) and ferrihydrite (FeOOH) together has been reported. Atomic-scale integrations by doping Fe and Mn with each other were detected and an adsorption-oxidation bifunctionality was achieved, where Fe-doped MnO 2 served as oxidizer for As(III) and amorphous/ground FeOOH acted as adsorbent first for As(III) and then As(V) from the oxidization. The maximal adsorption for As(III) could reach 44.99 mg/g and over 82.5% of As(III) was converted to As(V). More importantly, high removal ability of arsenic worked in a wide pH range of 2–10.5%, and 87.2% of its initial adsorption-oxidation capacity could be kept even after 5-cycles reuse for treating 20 mg/L As(III) with a dosage at 1 g/L. Together with the enhanced adsorption capacity by the milled FeOOH, surface electron transfer efficiency of the developed Fe-MnO 2 surrounded with Mn-Fe 2 O 3 has been studied for the first time to understand the oxidization effect to As(V). Besides the environment-friendliness of ball milling method, the prepared sample is quite stable without noticeable metal release into solution. Mechanism studies of arsenic removal by the as-prepared Fe-Mn-O oxide provide a new direction for improving the oxidation efficiency of MnO 2 to As(III) based on the widely available cheap Mn and Fe oxides, contributing to the development of advanced oxidization process in the treatment of waste water.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Yi Peng,Juntao Wang,Ying Yan,Wenlei Wang,Hongbo Xiao
In this work, a high content of pyrrole nitrogen carbon nitride (HPCN)-SnS 2 has been successfully constructed with −C═Sn− chemical bond as the interface framework. The charge state of Sn species was adjusted by β particles to obtain controllable sulfur defects onto the HPCN-SnS 2 through electron beam irradiation (EBI). The composites exhibited excellent photocatalytic oxidation capacity of As(Ⅲ) and adsorption capacity of As(Ⅴ). It is confirmed that the optimized HPCN-SnS 1.38 can remove the total As concentrations below 0.40 mg/L within 80 min. Additionally, the effect of various conditions (pH value and type of anions) was evaluated using degradation experiments, and HPCN-SnS 1.38 could be reused at least 5 times without an obvious reduction in the photocatalysis and adsorption performances. Based on the experimental results, the photocatalytic mechanism of As(Ⅲ) by HPCN-SnS 2 after electron beam irradiation was studied. Free radical quenching experiments and electron paramagnetic resonance (EPR) showed that the oxidation of As(III) under visible light is mainly controlled by •O 2 − and •OH, and •OH is converted from •O 2 − under acidic conditions.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Chao Shan,Hui Liu,Ming Hua,Bingcai Pan
The development of catalysts for oxidation of aqueous contaminants has long been relying on trial-and-error strategies due to lack of activity-tuning principles. Herein, Fenton-like oxidation of As(III) as a chemisorbed model contaminant over a series of fabricated CexTi1-xO2 catalysts with tunable structures was investigated. The activity of CexTi1–xO2 showed a volcano-shape dependency on Ce molar fraction, peaking at Ce0.25Ti0.75O2 (x = 0.25) with 6.32–6.36 times higher activity and 2.67–2.94 times higher specific activity compared with CeO2 and TiO2. The non-radical surface hydroperoxo complexes were experimentally substantiated as the dominant oxidant species on Ce0.25Ti0.75O2, which enabled a high efficiency of H2O2 utilization (99.1%). Under the verified Langmuir–Hinshelwood mechanism, the microkinetic model for the catalytic oxidation was established, and thus, the quantitative relationship between activity and adsorption energies for bimolecular chemisorption reactions was elucidated. Theoretically, a catalyst with identical adsorption energies toward both chemisorbed reactants tends to obtain the highest activity. Through DFT calculation, the highest activity of Ce0.25Ti0.75O2 was rationally interpreted by the balanced adsorption energies toward As(III) and H2O2, which was attributed to the shifted electronic density of states induced by Ce doping. This study provides a potent strategy to tune the catalytic activity of bimolecular chemisorption reactions.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ziwei Gao,Tao Zhang,Md. Nahid Pervez,Guojuan Qu,Wei Jin,Yaping Zhao
Materials combing catalytic and adsorption dual active sites are very important for arsenite (As(III)) due to its high mobility in water. Therefore, in this study, a bifunctional walnut-like Co-doped La(OH) 3 composites (Co-La) with independent catalytic sites and post-formed adsorption sites were synthesized via a simple hydrothermal method. Nearly 100% As(III) removal can be achieved in Co-La and peroxymonosulfate interaction systems (Co-La/PMS) within 10 min at the molar ratio of PMS to As(III) of 1.2. The results indicate that the combined Co-La adsorption system demonstrated superior performance compared to the Co-La adsorption alone. Precisely, the maximum removal capacity of the system was measured at 243.90 mg·g −1 , and the pseudo-first-order kinetic rate constant ( k 1 ) was determined to be 1.0771 min −1 . These values were significantly greater than those observed for Co-La adsorption alone. Notably, the kinetic rate constant was 239 times faster, and the removal capacity was 4.6 times higher in the combined system. The fast kinetics of As(III) elimination can be elucidated by the production of reactive oxygen species (ROS) such as S O 4 · - , •OH, O 2 · - and 1 O 2 , which expedite the conversion of As(III) into arsenate (As(V) in this particular system. Meanwhile, the increase in adsorption capacity is ascribed to the fact that PMS can drive La(OH) 3 of Co-La to transform into transition states La 2 SO 4 (OH) 4 , thus generating a new exchangeable adsorption site for As(V). A fixed membrane reactor assembled with Co-La was utilized to achieve a near-complete removal of As(III) within 3 min. The Co-La/PMS systems demonstrate exceptional effectiveness in eliminating arsenic from water across diverse real-water metrics, offering a unique perspective and technological progress in purifying water contaminated with arsenic.
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TALANTA
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2016
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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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JOURNAL OF HAZARDOUS MATERIALS
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2017
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IF 6.065
Zhangtao Li,Lu Wang,Jun Meng,Xingmei Liu,Jianming Xu,Fan Wang,Philip Brookes
Nanoscale zero-valent iron (NZVI) has a high adsorption capacity for heavy metals, but it forms aggregates easily. In this study, zeolite-supported nanoscale zero-valent iron (Z-NZVI) was synthesized from a simplified liquid-phase reduction of iron(III) salts which simultaneously adsorbed As(III), Cd(II) and Pb(II) from aqueous solution and soil. Scanning electron micrographs showed that aggregation was eliminated and the NZVI evenly dispersed onto the surface of zeolite. FTIR spectra reveal that NZVI was protected from oxidization on the surface of Z-NZVI. XRD and XPS patterns confirmed the formation of Cd(OH) 2 , Pb 0 , and FeAsO 4 in Z-NZVI after adsorption. The experimental maximum adsorption capacity of Z-NZVI was 11.52 mg As(III)/g, 48.63 mg Cd(II)/g, and 85.37 mg Pb(II)/g at pH 6, respectively, much higher than that of zeolite. Batch experiments indicate that various adsorption mechanisms including electrostatic adsorption, ionic exchange, oxidation, reduction, co-precipitation, and complexation coexisted with the selected heavy metals. Due to the formation of multiphase compounds on the Z-NZVI, the synergy and competition among heavy metals were concurrent. Most arsenic, cadmium and lead in the soil samples were immobilized after mixing with 30 g/kg Z-NZVI. These results suggest that Z-NZVI has great potential for treating water and soil multi-contaminated with heavy metals.
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Jihong Chen,Xiaoyu Dong,Dali Zhuo,Jiayuan Tang,Xiaoli Xiong,Hong Luo,Zhirong Zou
Metal-organic frameworks (MOFs) are porous materials that constructed by various metal nodes and organic ligands, taking the advantages of high porosity, large specific surface areas and more reactive sites etc. However, the applications of MOFs in hydride generation (HG)/chemical vapor generation (CVG)-colorimetric systems are rare. Herein, a series of silver-based MOFs (Ag-MOFs) were synthesized and served as substrates for As(III) and S 2- colorimetric analysis. As(III) and S 2- were converted into its volatile species (AsH 3 and H 2 S) via HG and CVG process, respectively, providing merits of low matrix interferences (selectivity) and high vapor generation efficiency (sensitivity). Ag-MOF-3 exhibits the best performances for As(III) and S 2- analysis, its reaction mechanisms were further explored. Ag nanoparticles (redox reaction) and Ag 2 S nanoparticles (combination reaction) were formed after Ag-MOF-3 reacted with AsH 3 and H 2 S, respectively, leading to color change from light yellow to black. The variation was recognized by naked eye and smartphone. Standard cards/curves of visual method and smartphone RGB method were thus established for As(III) and S 2- . It is a potential analytical method for on-site and rapid analysis of As(III) and S 2- with merits of low-cost, easy-to-use and portability.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Ge Zhang,Huifen Yang,Tong Zhao,Xuan Li,Yichen Zhou,Song Guo
The thermal adsorption residue (TDR) from oil sludge co-contaminated soil was employed to remove As(III), Zn(II), Cu(II), Cd(II) in aqueous solution. The results showed that the TDR could efficiently neutralize the acid and adapt to the extensive pH. The adsorption of four heavy metals on TDR could be divided into three stages. The maximum adsorption capacity were 86.59, 249.07, 339.88, 322.86 mg·g −1 for As(III), Zn(II), Cu(II), Cd(II), respectively. The coexistence of Zn(II)/Cu(II)/Cd(II) could promote As(III) removal but As(III) led to decreasing of Zn(II)/Cu(II)/Cd(II) adsorption capacity in binary system. There was a significant competitive adsorption on TDR among the three cations which followed the selectivity sequence of Cu(II)>Zn(II)>Cd(II). The SEM-EDS, XRD, FTIR and XPS analyses demonstrated that the As(III) was removed via formation of Ca-As precipitation, and the Zn(II), Cu(II), Cd(II) were removed through precipitating as hydroxides/carbonates/silicates combining with ion exchange. Specially, the Cu(II) mainly precipitated in the form of Cu 4 (SO 4 )(OH) 6 ⋅2H 2 O and Cu 4 (OH) 6 SO 4 under sulfuric acid solution environment. Overall, this study indicates the potential of TDR as a cost-effective adsorbent in acid heavy metals contaminated wastewater treatment .
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