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131.
Sawalha MF Sengupta MK Ohira S Idowu AD Gill TE Rojo L Barnes M Dasgupta PK 《Talanta》2008,77(1):372-379
A gas phase chemiluminescence (GPCL)-based method for trace measurement of arsenic has been recently described for the measurement of arsenic in water. The principle is based on the reduction of inorganic As to AsH3 at a controlled pH (the choice of pH governs whether only As(III) or all inorganic As is converted) and the reaction of AsH3 with O3 to produce chemiluminescence (Idowu et al., Anal. Chem. 78 (2006) 7088-7097). The same general principle has also been used in postcolumn reaction detection of As, where As species are separated chromatographically, then converted into inorganic As by passing through a UV photochemical reactor followed by AsH3 generation and CL reaction with ozone (Idowu and Dasgupta, Anal. Chem. 79 (2007) 9197-9204). In the present paper we describe the measurement of As in different soil and dust samples by serial extraction with water, citric acid, sulfuric acid and nitric acid. We also compare parallel measurements for total As by induction coupled plasma mass spectrometry (ICP-MS). As(V) was the only species found in our samples. Because of chloride interference of isobaric ArCl+ ICP-MS analyses could only be carried out by standard addition; these results were highly correlated with direct GPCL and LC-GPCL results (r2 = 0.9935 and 1.0000, respectively). The limit of detection (LOD) in the extracts was 0.36 μg/L by direct GPCL compared to 0.1 μg/L by ICP-MS. In sulfuric acid-based extracts, the LC-GPCL method provided LODs inferior to those previously observed for water-based standards and were 2.6, 1.3, 6.7, and 6.4 μg/L for As(III), As(V), dimethylarsinic acid (DMA) and monomethylarsonic acid (MMA), respectively. 相似文献
132.
Hydrothermal reaction of [MnCl2(terpy)] with elemental As and Se at 150 °C in 1:2:4 and 1:4:8 molar ratios in the presence of Cs2CO3 affords the complexes [{Mn(terpy)}2 (As2Se5)]2 ( 1 ) and [{Mn(terpy)}2 (As4Se8)] ( 2 ), respectively. 1 contains dipyramidal [As2Se5]4? ligands that bridge three MnII atoms in a tetradentate μ3‐1κ2Se1,Se2:2κSe4:3κSe5 manner. The tetranuclear complex is centrosymmetric and exhibits a central 8‐membered (MnSeAsSe)2 ring. Cyclic [As4Se8]4? ligands are present in the centrosymmetric dinuclear complex 2 and chelate the Mn(II) atoms through adjacent terminal Se atoms. Both 1 and 2 are linked into infinite chains through weak Mn···Se interactions. [{Mn(terpy)}2(As4S8)] ( 3 ) and ( 4 ) can be obtained by hydrothermal reaction of [MnCl2(terpy)] with As2S3 at respectively 150 °C and 190 °C. Whereas 3 exhibits an identical connectivity pattern to that of 2 , the coordination polymer 4 contains vierer chains that coordinate {(terpy)Mn}2+ fragments in a bidentate manner through terminal S atoms. The complex ( 5 ) contains double chains and results from the analogous hydrothermal reaction of [MnCl2(tren)] with As2S3 at 150 °C. 相似文献
133.
Synthesis and Coordination Behaviour of (Ph3SnO)3As. The Crystal Structures of (Ph3SnO)3As and [{(Ph3SnO)3As}Fe(CO)4] (Ph3SnO)3As ( 1 ) was obtained from the reaction of Ph3SnOH with As2O3 in a dichloromethane/water mixture as solvent. Upon recrystallization from DMF 1 forms orthorhombic crystals, space group P212121, with a = 977.3(2), b = 1903.5(3) and c = 2600.9(5) pm (at 220 K). In 1 the As atom is bound to three OSnPh3 groups with As–O distances of 171.9(3)–174.9(3) pm. Reaction of 1 with Fe2(CO)9 gives [{(Ph3SnO)3As}Fe(CO)4] ( 2 ). 2 crystallizes monoclinic, space group P21/n with a = 2242.3(5), b = 1112.6(2), c = 2353.0(5) pm and β = 111,46(2)° (at 220 K). In 2 the iron atom exhibits a trigonal bipyramidal coordination with the (Ph3SnO)3As ligand in an axial position. The Fe–As bond length is 230.5(1) pm. 相似文献
134.
Slejkovec Z Falnoga I Goessler W van Elteren JT Raml R Podgornik H Cernelc P 《Analytica chimica acta》2008,607(1):83-91
Urine and blood samples of cancer patients, treated with high doses of arsenic trioxide were analysed for arsenic species using HPLC-HGAFS and, in some cases, HPLC-ICPMS. Total arsenic was determined with either flow injection-HGAFS in urine or radiochemical neutron activation analysis in blood fractions (in serum/plasma, blood cells). The total arsenic concentrations (during prolonged, daily/weekly arsenic trioxide therapy) were in the μg mL−1 range for urine and in the ng g−1 range for blood fractions. The main arsenic species found in urine were As(III), MA and DMA and in blood As(V), MA and DMA.With proper sample preparation and storage of urine (no preservation agents/storage in liquid nitrogen) no analytical artefacts were observed and absence of significant amounts of alleged trivalent metabolites was proven. On the contrary, in blood samples a certain amount of arsenic can get lost in the speciation procedure what was especially noticeable for the blood cells although also plasma/serum gave rise to some disappearance of arsenic. The latter losses may be attributed to precipitation of As(III)-containing proteins/peptides during the methanol/water extraction procedure whereas the former losses were due to loss of specific As(III)-complexing proteins/peptides (e.g. cysteine, metallothionein, reduced GSH, ferritin) on the column (Hamilton PRP-X100) during the separation procedure. Contemporary analytical protocols are not able to completely avoid artefacts due to losses from the sampling to the detection stage so that it is recommended to be careful with the explanation of results, particularly regarding metabolic and pharmacokinetic interpretations, and always aim to compare the sum of species with the total arsenic concentration determined independently. 相似文献
135.
《Arabian Journal of Chemistry》2023,16(2):104501
This study investigates the simultaneous removal of low concentrations of arsenic and mercury ions from synthetic produced water via hollow fiber supported liquid membrane (HFSLM). Results show that HFSLM can remove both arsenic and mercury ions from synthetic produced water to less than 0.02 and 0.001 mg·L-1, respectively. These final concentrations comply with the wastewater standard of Thailand. Percentages of extraction for arsenic and mercury ions proved to be about 100 %. Those of recovery for arsenic and mercury ions reached 70 % and 75 %, respectively. A quantum model based on density functional theory (DFT) is introduced to analyze the forming and breaking of supramolecular complex species in the processes of extraction and recovery, respectively. Furthermore, the concept of Generating Function is applied to construct a mathematical model for forecasting the potential of removing metal ions via HFSLM. The mathematical model conforms to the experimental data, having an average relative deviation of 5 %. The results of this study provide a better understanding of the transport mechanisms of arsenic and mercury ions. 相似文献
136.
M. S. Podder 《Composite Interfaces》2016,23(4):327-372
The granular activated carbon/MnFe2O4 composite with a mass ratio of 2:1 was synthesized using a simple chemical coprecipitation procedure and used for the removal of As(III) and As(V) from synthetically prepared wastewater. Physicochemical analysis of the composite was carried out through Brunauer, Emmett and Teller surface area and total pore volume, Fourier Transform Infrared Spectroscopy (FT-IR) and Scanning Electron Micrograph and Energy-Dispersive X-Ray Spectroscopy (SEM-EDX). The impact of various adsorption parameters such as the initial pH, adsorbent dose, contact time, temperature and initial arsenic concentration were systematically investigated to evaluate the optimum operating conditions. Nonlinear regression analysis was employed to identify the best-fit isotherm on the basis of three correlation coefficients and three error functions and also to predict the parameters involved in one one-parameter, six two-parameter, nineteen three-parameter, three four-parameter and one five-parameter isotherms. The maximum adsorption capacities estimated using the Langmuir model were 1253 mg/g for As(III) and 1314 mg/g for As(V) at 30 °C temperature and 70 min contact time. The results showed that As(III) and As(V) removal was strongly pH-dependent with an optimum pH value of 7.0 and 4.0, respectively. The mean adsorption energy (E) calculated from the D–R model indicated the nature of adsorption being ion exchange type. 相似文献
137.
Simultaneous separation and determination of six arsenic species in rice by anion‐exchange chromatography with inductively coupled plasma mass spectrometry 下载免费PDF全文
The simultaneous separation and determination of arsenite As(III), arsenate As(V), monomethylarsonic acid (MMA), dimethylarsinic acid (DMA), arsenobetaine (AsB), and arsenocholine (AsC) in rice samples have been carried out in one single anion‐exchange column run by high‐performance liquid chromatography with inductively coupled plasma mass spectrometry. To estimate the effect of variables on arsenic (As) speciation, the chromatographic conditions including type of competing anion, ionic strength, pH of elution buffer, and flow rate of mobile phase have been investigated by a univariate approach. Under the optimum chromatographic conditions, baseline separation of six As species has been achieved within 10 min by gradient elution program using 4 mM NH4HCO3 at pH 8.6 as mobile phase A and 4 mM NH4HCO3, 40 mM NH4NO3 at pH 8.6 as mobile phase B. The method detection limits for As(III), As(V), MMA, DMA, AsB, and AsC were 0.4, 0.9, 0.2, 0.4, 0.5, and 0.3 μg/kg, respectively. The proposed method has been applied to separation and quantification of As species in real rice samples collected from Hunan Province, China. The main As species detected in all samples were As(III), As(V) and DMA, with inorganic As accounting for over 80% of total As in these samples. 相似文献
138.
Determination of arsenic species in Solanum Lyratum Thunb using capillary electrophoresis with inductively coupled plasma mass spectrometry 下载免费PDF全文
Pei‐Yu Shuai Xiao‐Jun Yang Zong‐Qing Qiu Xiao‐Hui Wu Xi Zhu Ganga Raj Pokhrel Yu‐Ying Fu Hui‐Min Ye Wen‐Xiong Lin Gui‐Di Yang 《Journal of separation science》2016,39(16):3239-3245
A simple and highly efficient interface to couple capillary electrophoresis with inductively coupled plasma mass spectrometry by a microflow polyfluoroalkoxy nebulizer and a quadruple ion deflector was developed in this study. By using this interface, six arsenic species, including arsenite, arsenate, monomethylarsonic acid, dimethylarsinic acid, arsenobetaine, and arsenocholine, were baseline‐separated and determined in a single run within 11 min under the optimized separation conditions. The instrumental detection limit was in the range of 0.02–0.06 ng/mL for the six arsenic compounds. Repeatability expressed as the relative standard deviation (n = 5) of both migration time and peak area were better than 2.5 and 4.3% for six arsenic compounds. The proposed method, combined with a closed‐vessel microwave‐assisted extraction procedure, was successfully applied for the determination of arsenic species in the Solanum Lyratum Thunb samples from Anhui province in China with the relative standard deviations (n = 5) ≤4%, method detection limits of 0.2–0.6 ng As/g and a recovery of 98–104%. The experimental results showed that arsenobetaine was the main speciation of arsenic in the Solanum Lyratum Thunb samples from different provinces in China, with a concentration of 0.42–1.30 μg/g. 相似文献
139.
The major arsenosugar compounds have been reported to be hydride-generation-active, however to a lesser extent in comparison
with the inorganic arsenicals. We report here for the first time the identity and quantity of the volatile arsenicals generated
by As-sugar-SO3, As-sugar-SO4, dimethylarsinoyl acetic acid and dimethylarsinoyl ethanol. Only one major volatile compound was identified for all four
compounds studied: dimethylarsine. This means that the As–C bond to the longer carbon chain was cleaved during the hydride-generation
process. Theoretical calculations at the RHF/6-31G(d,p) ab initio level confirm that this As–C bond is much weaker than the
As–CH3 bonds. Furthermore, it was revealed that the sulphur analogue of dimethylarsinic acid (DMAS ) is hydride-generation-active
at pH 7 in contrast to dimethylarsinic acid, despite the fact that arsenic is also pentavalent. This has been substantiated
by the calculation of the change in susceptibility of the arsenic towards nucleophilic attack when oxygen is replaced by sulphur.
Hence, DMAS can easily be mistaken for a trivalent arsenic species. 相似文献
140.
A novel quartz device has been designed to trap arsine and selenium hydride and subsequently to volatilize the collected analyte
and atomize it for atomic-absorption spectrometric detection. The device is actually the multiple microflame quartz-tube atomizer
(multiatomizer) with inlet arm modified to serve as the trap and to accommodate the oxygen-delivery capillary used to combust
hydrogen during the trapping step. The effect of relevant experimental conditions (trap temperature during trapping and hydrogen
flow rate and trap temperature during volatilization) on collection and volatilization efficiency was investigated. Under
the optimum conditions collection and volatilization efficiency for arsenic and selenium were 50 and 70%, respectively.
相似文献