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Huijuan Liu - One of the best experts on this subject based on the ideXlab platform.
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removal of p Arsanilic Acid and phenylarsonic Acid from water by fenton coagulation process influence of substituted amino group
Environmental Science and Pollution Research, 2021Co-Authors: Qiang Peng, Huijuan LiuAbstract:Phenylarsonic Acid compounds, which were widely used in poultry and swine production, are often introduced to agricultural soils with animal wastes. Fenton coagulation process is thought as an efficient method to remove them. However, the substituted amino group could apparently influence the removal efficiency in Fenton coagulation process. Herein, we investigated the optimal conditions to treat typical organoarsenic contaminants (p-Arsanilic Acid (p-ASA) and phenylarsonic Acid (PAA)) in aqueous solution based on Fenton coagulation process for oxidizing them and capturing the released inorganic arsenic, and elucidated the influence mechanism of substituted amino group on removal. Results showed that the pH value and the dosage of H2O2 and Fe2+ significantly influenced the performance of the oxidation and coagulation processes. The optimal conditions for removing 20 mg L-1-As in this research were 40mg L-1 Fe2+ and 60mg L-1 H2O2 (the mass ratio of Fe2+/H2O2 = 1.5), initial solution pH of 3.0, and final solution pH of 5.0 adjusting after 30-min Fenton oxidation reaction. Meanwhile, the substituted amino group made p-ASA much more easily be attacked by ·OH than PAA and supply one more binding sites for forming complexes with Fe3+ hydrolysates, resulting in 36% higher oxidation rate and 7% better coagulation performance at the optimal conditions.
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the removal efficiency and insight into the mechanism of para Arsanilic Acid adsorption on fe mn framework
Science of The Total Environment, 2017Co-Authors: Tista Prasai Joshi, Gong Zhang, Ruiping Liu, Rashmi Koju, Huijuan LiuAbstract:Para Arsanilic Acid (p-ASA) is extensively used as feed additives in poultry industry, resulting contaminates soil and natural water sources through the use of poultry litter as a fertilizer in croplands. Thus, removal of p-ASA prior to its entering environments is significant to control their environmental risk. Herein, we studied Fe-Mn framework and cubic Fe(OH)3 as promising novel adsorbents for the removal of p-ASA from aqueous solution. The chemical and micro-structural properties of Fe-Mn framework and cubic Fe(OH)3 materials were characterized by X-ray diffraction patterns (XRD), nitrogen adsorption (SBET), zeta (ζ-) potential, scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectra (XPS). The maximum adsorption capacity for p-ASA on Fe-Mn framework and cubic Fe(OH)3 was determined to be 1.3mmolg-1 and 0.72mmolg-1 at pH4.0, respectively. Adsorption of p-ASA decreased gradually with increasing pH indicated that adsorption was strongly pH dependent. Azophenylarsonic Acid was identified as an oxidation intermediate product of p-ASA after adsorption on Fe-Mn framework. Plausible removal mechanism for p-ASA by Fe-Mn framework was proposed. The obtained results gain insight into the potential applicability of Fe-Mn framework, which can be potentially important for the removal of p-ASA from water.
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transformation of para Arsanilic Acid by manganese oxide adsorption oxidation and influencing factors
Water Research, 2017Co-Authors: Tista Prasai Joshi, Gong Zhang, Hanyang Cheng, Ruiping Liu, Huijuan LiuAbstract:Aromatic organoarsenic compounds tend to transform into more mobile toxic inorganic arsenic via several processes, and can inadvertently spread toxic inorganic arsenic through the environment to water sources. To gain insight into the transformation mechanisms, we herein investigated how the process of para Arsanilic Acid (p-ASA) transformation works in detail on the surface of adsorbents by comparing it with phenylarsonic Acid (PA) and aniline, which have similar chemical structures. In contrast to the values of 0.23 mmol g−1 and 0.68 mmol g−1 for PA and aniline, the maximum adsorption capacity was determined to be 0.40 mmol g−1 for p-ASA at pH 4.0. The results of FTIR and XPS spectra supported the presence of a protonated amine, resulting in a suitable condition for the oxidation of p-ASA. Based on the combined results of UV-spectra and UPLC-Q-TOF-MS, we confirmed that the adsorbed p-ASA was first oxidized through the transfer of one electron from p-ASA on MnO2 surface to form a radical intermediate, which through further hydrolysis and coupling led to formation of benzoquinone and azophenylarsonic Acid, which was identified as a major intermediate. After that, p-ASA radical intermediate was cleaved to form arsenite (III), and then further oxidized into arsenate (V) with the release of manganese (Mn) into solution, indicating a heterogeneous oxidation process.
Ivan P Pozdnyakov - One of the best experts on this subject based on the ideXlab platform.
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synergetic effect of potassium persulfate on photodegradation of para Arsanilic Acid in fe iii oxalate system
Journal of Photochemistry and Photobiology A-chemistry, 2021Co-Authors: Yuliya E Tyutereva, Victor F Plyusnin, Petr S Sherin, E V Polyakova, V P Grivin, Olga V Shuvaeva, Ivan P PozdnyakovAbstract:Abstract The p-Arsanilic Acid (p-ASA) is widely used in agriculture as a food additive to control parasites. It leaves the body almost unchanged and is subsequently destroyed by environmental factors with the formation of toxic forms of inorganic arsenic. UVA irradiation of p-ASA with the addition of the Fe(III) oxalate complex leads to an effective photodegradation of the target compound. However, this method needs high concentrations of reagents and the keeping high [oxalate]:[Fe(III)] ratio to maintain proper efficiency of Fe(III) oxalate system. In this work, to overcome these problems, potassium persulfate (PS) was used as an additional oxidizer to improve Fe(III) oxalate system. It was found that the sulfate radical produced upon PS activation reacts readily with both neutral and monoanionic forms of p-ASA yielding corresponding organic cation radical, bimolecular rate constants are (7.3 ± 0.6) × 109 and (2.4 ± 0.4) × 109 M-1s-1, accordingly. Addition of 1 mM of PS reduces to one order (from 1.6 to 0.12 mM) the working concentration of oxalate and allows to achieve the complete degradation of both p-ASA and organic byproducts to inorganic As(V). Also the proposed approach demonstrates high efficiency in a wide range (from
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photodegradation of para Arsanilic Acid mediated by photolysis of iron iii oxalate complexes
Chemosphere, 2020Co-Authors: Yuliya E Tyutereva, Victor F Plyusnin, Petr S Sherin, E V Polyakova, Olga S Koscheeva, V P Grivin, Olga V Shuvaeva, Ivan P PozdnyakovAbstract:Abstract Organic arsenicals are important environment pollutants due to wide use in livestock and toxicity of degradation products. In this work we report about the efficient photodegradation of the p-Arsanilic Acid (p-ASA) and its decomposition products in the Fe(III)-oxalate assisted approach under nature-relevant conditions. At neutral pH under near-visible UV irradiation the Fe(III) oxalate complexes generate the primary oxidizing intermediate, OH radical (the quantum yield of ϕOH ∼ 0.06), which rapidly reacts with p-ASA with high rate constant, (8.6 ± 0.5) × 109 M−1s−1. Subsequent radical reactions result in the complete photooxidation of both p-ASA and basic aromatic photoproducts with the predominant formation of inorganic arsenic species, mainly As(V), under optimal conditions. Comparing with the direct UV photolysis, the presented Fe(III)-oxalate mediated degradation of p-ASA has several advantages: higher efficiency at low p-ASA concentration and complete degradation of organic arsenic by-products without use of short-wavelength UV radiation. The obtained results illustrate that the Fe(III)-oxalate complexes are promising natural photosensitizers for the removal of arsenic pollutants from contaminated waters.
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uvc induced photodegradation of p Arsanilic Acid assisted by humic substances
Mendeleev Communications, 2019Co-Authors: Yuliya E Tyutereva, Peter S Sherin, Zizheng Liu, Victor F Plyusnin, Ivan P PozdnyakovAbstract:Quantum yields of indirect UVC photodegradation of p-Arsanilic Acid (a widely used phenylarsonic feed additive) caused by the photolysis of humic substances were measured. The acquired results demonstrate that the efficiency of such decomposition of p-Arsanilic Acid is comparable with that of its direct UVC photolysis due to the participation of active intermediates generated during the photolysis of humic substances. These results could be important for understanding the fate of p-Arsanilic Acid during an UVC disinfection of wastewaters containing natural humic substances.
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new insights into mechanism of direct uv photolysis of p Arsanilic Acid
Chemosphere, 2019Co-Authors: Yuliya E Tyutereva, Zizheng Liu, Victor F Plyusnin, Petr S Sherin, Marina V Parkhats, Ivan P PozdnyakovAbstract:Abstract The mechanism of direct UV photolysis of p-Arsanilic Acid (p-ASA), a widely used veterinary drug, was revised by means of laser flash photolysis coupled with high resolution liquid chromatography – mass spectrometry (LC-MS). None of p-ASA triplet state or singlet oxygen was found to directly participate in the photodegradation of p-ASA as it was assumed in previous works. Here we demonstrate that the main primary photoprocess is a monophotonic ionization (ϕion266nm = 0.032) leading to the formation of hydrated electron and corresponding anilinyl cation radical. These primary species react with dissolved oxygen yielding secondary reactive oxygen species. The final organic photoproducts, such as aminophenol and different dimeric products, originate from various reactions between these secondary species. The generation of inorganic arsenic, both As(V) and As(III), was also observed in agreement with previous works. For the first time we report the quantum yield of p-ASA photodegradation, which decreases from 0.058 to 0.035 with the excitation wavelength from 222 to 308 nm.
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kinetics and mechanisms of ph dependent direct photolysis of p Arsanilic Acid under uv c light
Chemical Engineering Journal, 2018Co-Authors: Xiangyi Shen, Zizheng Liu, Ivan P Pozdnyakov, Duanli Wang, Chuxuan Zhao, Jun XiaAbstract:Abstract The usage of p-Arsanilic Acid (ASA) in livestock and poultry farms leads to its release into the environment. The phototransformation of ASA generates toxic inorganic arsenic species and organic by-products, which affects the water security of the peripheral river basin. In this work, we have investigated the pH-dependent kinetics and mechanisms of ASA photolysis under Ultraviolet-C (UV-C) light (254 nm) irradiation in the pH range 1–11 in the absence of oxygen. The degradation rate of ASA, the ratio of the generated inorganic arsenic species, and the amount of primary organic by-products were determined under the aforesaid conditions. Our results clearly showed the pH-dependent photochemistry of ASA. The photolysis rate was low under Acidic conditions, and As(III) and p-aminophenol were the main products. With increasing pH, the photolysis rate increased significantly, and As(V) and aniline became the main products. A pH-based kinetic model has been established that allows prediction of the generation rates of As(III), As(V), p-aminophenol, and aniline according to the photolysis rate of ASA.
Hind A Alabadleh - One of the best experts on this subject based on the ideXlab platform.
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density functional theory calculations on the complexation of p Arsanilic Acid with hydrated iron oxide clusters structures reaction energies and transition states
Journal of Physical Chemistry A, 2014Co-Authors: Adrian Adamescu, I P Hamilton, Hind A AlabadlehAbstract:Aromatic organoarsenicals, such as p-Arsanilic Acid (pAsA), are still used today as feed additives in the poultry and swine industries in developing countries. Through the application of contaminated litter as a fertilizer, these compounds enter the environment and interact with reactive soil components such as iron and aluminum oxides. Little is known about these surface interactions at the molecular level. We report density functional theory (DFT) calculations on the energies, optimal geometries, and vibrational frequencies for hydrated pAsA/iron oxide complexes, as well as changes in Gibbs free energy, enthalpy, and entropy for various types of ligand exchange reactions leading to both inner- and outer-sphere complexes. Similar calculations using arsenate are also shown for comparison, along with activation barriers and transition state geometries between inner-sphere complexes. Minimum energy calculations show that the formation of inner- and outer-sphere pAsA/iron oxide complexes is thermodynamically...
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atr ftir studies on the nature of surface complexes and desorption efficiency of p Arsanilic Acid on iron oxyhydr oxides
Environmental Science & Technology, 2009Co-Authors: Matthew Chabot, Tuan Hoang, Hind A AlabadlehAbstract:The fate of organoarsenicals introduced to the environment through the application of arsenic-contaminated manure has attracted considerable attention after the recent implementation of the latest maximum contaminant level (MCL) of total arsenic in drinking water by the U.S. Environmental Protection Agency (EPA). We report herein detailed spectroscopic analysis of the surface structure of p-Arsanilic Acid (p-AsA) adsorbed on Fe-(oxyhydr)oxides using attenuated total internal reflectance Fourier transform infrared spectroscopy (ATR-FTIR). Spectra of p-AsA(ads) were collected in situ as a function of pH and ionic strength and using D20 at 298 K in flow mode. Results indicate the formation of inner-sphere complexes, which are likely monodentate and become protonated under Acidic pH(D). We also examined the desorption efficiency of p-AsA(ads) due to flowing electrolyte and phosphate solutions as low as 0.1 mol/m3 (3 ppm P) by collecting ATR-FTIR spectra as a function of time. Our results suggest that aqueous phosphate is an efficient desorbing anion of p-AsA(ads), which has implications on its bioavailability and mobility in geochemical environments.
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adsorption thermodynamics of p Arsanilic Acid on iron oxyhydr oxides in situ atr ftir studies
Environmental Science & Technology, 2008Co-Authors: Sarah G S Depalma, Scott Cowen, Tuan Hoang, Hind A AlabadlehAbstract:The organoarsenical p-Arsanilic Acid (p-AsA) is used in the U.S. poultry industry as a feed additive and its structure resembles one of the stable biodegradation products of Roxarsone (ROX) in anaerobic environments. With the implementation of recent EPA MCL of total arsenic in drinking water (10 ppb), thereareconcernsaboutthefate of organoarsenicals introduced to the environment through the application of arsenic-contaminated manure. We report herein, for the first time, the thermodynamics of p-AsA binding to Fe-(oxyhydr)oxides using ATR-FTIR. ATR-FTIR spectra were used to quantify surface coverage of p-AsA, p-AsA(ads), by analyzing the broadband assigned to v(As-O) at 837 cm(-1). Adsorption isotherms were measured in situ at 298 K and pH 7 in the concentration range 1 microM to 40 mM. Values of Keq were obtained from Langmuir model fits and they range from 1411 to 3228 M(-1). We also determined the maximum adsorption capacities of Fe-(oxyhydr)oxides to p-AsA, and they range from 1.9 x 10(13) to 2.6 x 10(13) molecules/cm2. Our results suggest that p-AsA is more mobile than methylated and inorganic forms of arsenic and that the transport of nanoparticles with p-AsA(ads) might play a role in its mobility in geochemical environments.
Shoujun Yuan - One of the best experts on this subject based on the ideXlab platform.
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influence of Arsanilic Acid cu 2 po 4 3 and their interaction on anaerobic digestion of pig manure
Frontiers of Environmental Science & Engineering in China, 2018Co-Authors: Rui Tang, Shoujun Yuan, Wei WangAbstract:Arsanilic Acid (ASA), copper ion (Cu2+) and phosphate (PO4 3–) are widely used as feed additives for pigs. Most of these three supplemented feed additives were excreted in feces and urine. Anaerobic digestion is often used for the management of pig manure. However, the interaction of ASAwith Cu2+ or PO4 3– on anaerobic digestion is still not clear. In this study, the influence of ASA, Cu2+, PO4 3– and their interaction on anaerobic digestion of pig manure and the possible mechanisms were investigated. The initial concentrations of ASA, Cu2+ and PO4 3– were 0.46 mM, 2 mM and 2 mM in the anaerobic digester, respectively. The methanogenesis was severely inhibited in the assays with only ASA addition, only Cu2+ addition and ASA + PO4 3– addition with the inhibition index of 97.8%, 46.6% and 82.6%, respectively, but the methanogenesis inhibition in the assay with ASA + Cu2+ addition was mitigated with the inhibition index of 39.4%. PO4 3– had no obvious impacts on the degradation of ASA. However, Cu2+ addition inhibited the degradation of ASA, and mitigated the methanogenesis inhibition. The existence of ASA would inhibit methanogenesis and generate more toxic inorganic arsenic compounds during anaerobic digestion, implying the limitation of anaerobic digestion for ASA- contaminated animal manure. However, the co-existence of ASA and Cu2+ could mitigate the inhibition. These results could provide useful information for the management of anaerobic digestion of pig manure containing ASA and Cu2+.
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the performance of activated sludge exposed to Arsanilic Acid and amprolium hydrochloride in sequencing batch reactors
International Biodeterioration & Biodegradation, 2017Co-Authors: Kui Chen, Shoujun Yuan, Wentao Hao, Wei WangAbstract:Abstract Arsanilic Acid (ASA) and amprolium hydrochloride (AMP) are widely used as feed additives to control coccidial intestinal parasites and improve feed efficiency, but due to low metabolism most of the drugs are excreted by the animals unchanged and eventually end up in wastewaters. Little is known about the impacts of AMP and ASA on the performance of activate sludge in sequencing batch reactors (SBRs) as well as about their fate in wastewater treatment. In this study, the long-term performance of activated sludge in SBRs exposed to ASA and AMP was investigated. The COD removal and nitrification were not affected when the concentration of ASA or AMP was lower than 20 mg L −1 , but were markedly inhibited at 100 mg L −1 of ASA or AMP. The inhibition to of COD removal was reversible whereas the inhibition to nitrification was irreversible. Phosphate removal was not affected by the continuous exposure to ASA or AMP. ASA and AMP were very resistant to be degraded by the activated sludge in SBRs, and only a small quantity of ASA was degraded to inorganic arsenic (no more than 300 μg L −1 ) in the form of As (III) and As (V).
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effect of Arsanilic Acid on anaerobic methanogenic process kinetics inhibition and biotransformation analysis
Biochemical Engineering Journal, 2014Co-Authors: Hailong Wang, Zilin Tong, Wei Wang, Shoujun YuanAbstract:Abstract Arsanilic Acid (4-aminophenylarsonic Acid) is widely used in the poultry and animal industries as a feed additive in the diets. Nearly all the added Arsanilic Acid is excreted unchanged in manure resulting in the risk of arsenic contamination. In this study, the effects of Arsanilic Acid on the kinetics, inhibition of methanogenic process and its biotransformation were investigated. The methane yield was not affected by Arsanilic Acid loading at concentration 50 of Arsanilic Acid in this study was 0.47 mM. After 115 days of incubation, 37–59% of the added Arsanilic Acid was degraded. The species analysis indicated that at lower initial Arsanilic Acid concentration, the soluble inorganic arsenic mainly existed in the species of arsenate (As(V)), while at higher initial Arsanilic Acid concentration (>0.460 mM), the soluble inorganic arsenic mainly existed in the species of arsenite (As(III)), which explains why higher Arsanilic Acid concentration has severe inhibition to methanogens.
Wei Zhang - One of the best experts on this subject based on the ideXlab platform.
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simultaneous adsorption and oxidation of para Arsanilic Acid by a highly efficient nanostructured fe ti mn composite oxide
Chemical Engineering Journal, 2021Co-Authors: Wei Zhang, Wei Liu, Jianguo Song, Qixia YangAbstract:Abstract The para Arsanilic Acid (p-ASA) used as feed additive in the poultry and swine industries tends to transform into more toxic inorganic arsenic (As(V) and As(III)), leading to a greater risk to human health and environmental system. In this study, simultaneous adsorption and oxidation of p-ASA was achieved by a synthesized highly efficient nanostructured Fe-Ti-Mn composite oxide (FTMO), with a high specific surface area of 424.7 m2/g. The maximum adsorption capacity for p-ASA could be as high as 45.6 mg/g, meanwhile the combined oxidation/photo-oxidation processes led to the formation of intermediate containing hydrazine group, however, without release of toxic inorganic As(III) and As(V). The p-ASA adsorption by FTMO was verified as the chemisorption process with the formation of inner-sphere complexes at the solid/water interface, which was prominently influenced by solution pH, coexisting ions and humic Acid, however relatively insensitive to ionic strength. The systematic characterization by FTIR, XPS, EPR and XANES revealed that Fe phase of FTMO played the dominant role for p-ASA adsorption, while Mn and Ti phases were responsible for the oxidation and photo-oxidation of p-ASA, respectively.
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highly efficient removal of p Arsanilic Acid with fe ii peroxydisulfate under near neutral conditions
Water Research, 2020Co-Authors: Panxin Wang, Wei Zhang, Jin Jiang, Zhuangsong Huang, Haijun Cheng, Suyan Pang, Yang Zhou, Xuedong ZhaiAbstract:Abstract As a common animal feed additive, p-Arsanilic Acid (p-AsA) is thought to be excreted with little uptake and unchanged chemical structure, threatening the environment by potentially releasing more toxic inorganic arsenic. We herein investigated the removal of arsenic by in situ formed ferric (oxyhydr)oxides with the promotion of p-AsA degradation in Fe(II)/peroxydisulfate (PDS) system. Results showed that under Acid conditions, p-AsA degraded very quickly and over 99% of p-AsA (5 μM) was degraded within 10 min at the optimal dosage of Fe(II) (100 μM) and PDS (150 μM) at pH 3, while less than 66.4% of arsenic was removed at pH 3–5. Higher pH (3–7) would inhibit the degradation of p-AsA but promote the arsenic removal. At pH 6–7, over 98.5% of total arsenic was removed, while the degradation efficiency of p-AsA was lower than 52.4%. HPLC-ICP-MS results indicated that the arsenic group was cleaved from p-AsA in the form of As(III) and then rapidly oxidized to As(V). FTIR and XPS analysis indicated that both As(V) products and residual p-AsA were bonded to ferric (oxyhydr)oxides via hydroxyl groups. Common cations (e.g., Na+, Ca2+, Mg2+) and anions such as Cl−, SO42−, CO32− had no significant influence on arsenic removal, while SiO32−, PO43− and HA inhibited the removal of total arsenic, mainly by affecting the zeta potential of iron particles. In summary, the Fe(II)/PDS process, as an efficient method for partial oxidation and simultaneous adsorption of p-AsA under near-neutral conditions, is expected to control the potential environmental risks of p-AsA.