As(III)

As (III)
  • 文章类型: Journal Article
    开发了一种有效的电化学传感器,通过用铁基金属有机骨架(Fe-MOF/g-C3N5)修饰碳糊电极(CPE)来检测和确定As(III)。差分脉冲阳极溶出伏安法(DPASV)方法用于分析磷酸盐缓冲溶液(0.10M,pH=5)。Fe-MOF/g-C3N5/CPE显示高灵敏度(4.24μAμg-1L),令人满意的线性范围(0.50μgL-1-5.00μgL-1和5.00μgL-1-30.00μgL-1),和低检测限(LOD,0.013μgL-1)。所制备的传感器具有良好的重复性和选择性,并成功地用于测定环境水域和苹果汁样品中的As(III)离子。
    An effective electrochemical sensor was developed to detect and determine of the As(III) by modifying the carbon paste electrode (CPE) with graphitic carbon nitride decorated with iron-based metal-organic frameworks (Fe-MOF/g-C3N5). The differential pulse anodic stripping voltammetry (DPASV) method was used to analyze As(III) ions in a phosphate buffer solution (0.10 M, pH = 5). Fe-MOF/g-C3N5/CPE showed high sensitivity (4.24 μA μg-1 L), satisfactory linear range (0.50 μg L-1-5.00 μg L-1 and 5.00 μg L-1-30.00 μg L-1), and low detection limit (LOD, 0.013 μg L-1). The prepared sensor was showed an excellent repeatability and selectivity, and successfully used for determination of the As(III) ion in ambient waters and apple juice samples.
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  • 文章类型: Journal Article
    这项研究调查了抗抑郁药舍曲林盐酸盐(Ser-HCl)与砷(III)或镉联合对水稻生理的影响。水培实验表明,较低浓度(0.2和0.6mgL-1)的Ser-HCl和As(III)或Cd会增加水稻生物量,降低pH值和低分子量有机酸。用Ser-HCl和As-only处理增强了荧光强度,溶解性有机质指数差异显著(p<0.05)。内生菌特定的操作分类单位减少,以蛋白质细菌为主的水稻根系内生菌。Ser-HCl的添加导致Verrucomicrobiota增加了6.4倍,与苹果酸呈正相关,与pH呈负相关。功能注释突出了碳水化合物代谢途径的改变。这项研究提供了有关Ser-HCl与As(III)或Cd结合时对水稻的相互作用的见解,解决我们对抗抑郁药对植物系统影响的理解差距。
    This study investigated the effects of the antidepressant sertraline hydrochloride (Ser-HCI) on rice physiology when combined with arsenic (III) or cadmium. Hydroponic experiments revealed that combined lower concentrations (0.2 and 0.6 mg L-1) of Ser-HCl and As (III) or Cd increased rice biomass and reduced pH and low molecular weight organic acids. The fluorescence intensity was enhanced with Ser-HCl and As-only treatments, with a significant difference (p < 0.05) in the dissolved organic matter index. There was a decrease in endophyte-specific operational taxonomic units, with proteobacteria dominating the rice root endophytes. The addition of Ser-HCl resulted in the Verrucomicrobiota increasing by 6.4 times, which was positively correlated with malic acid and negatively correlated with pH. Functional annotation highlighted alterations in carbohydrate metabolism pathways. This study provides insights into the interactive effects of Ser-HCl on rice when combined with As (III) or Cd, addressing gaps in our understanding of the impact of antidepressants on plant systems.
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  • 文章类型: Journal Article
    基于石墨烯的材料由于其具有高表面积的层状结构而被广泛用于从水中去除砷。这里,我们已经成功地合成了Fe-La双金属改性石墨片材料,以更有效地从水溶液中去除As(III)。结果表明,Fe-La-石墨片(FL-石墨片)比石墨片(2.80m2·g-1)具有更大的比表面积(194.28m2·g-1)。FL-石墨片对As(III)的吸附容量为51.69mg·g-1,高于石墨片(21.91mg·g-1),La-石墨片(26.06mg·g-1),和Fe-石墨片(40.26mg·g-1)。FL石墨片符合Freundlich和Dubinin-Radushkevich等温线,最大吸附量为53.62mg·g-1。去除过程服从As(III)的颗粒内扩散和孔隙扩散。批量吸附实验和表征分析的结果表明,配体交换,与石墨片相比,FL-石墨片吸附到As(III)中所涉及的内球络合机制。此外,静电吸引机制在吸附中至关重要。生态毒性评估表明,FL-石墨片对水稻发芽和生长影响很小,但降低了As(III)对水稻的毒性。因此,FL-石墨片在净化具有生态毒性的As(III)污染水中具有良好的实际应用价值。
    Graphene-based material is widely used to remove arsenic from water due to its layered structure with high surface area. Here, we have successfully synthesized Fe-La bimetallic modified graphite sheet materials to more efficiently remove As(III) from aqueous solution. The results showed that Fe-La-graphite sheets (FL-graphite sheets) have a larger specific surface area (194.28 m2·g-1) than graphite sheets (2.80 m2·g-1). The adsorption capacity of FL-graphite sheets for As(III) was 51.69 mg·g-1, which was higher than that of graphite sheets (21.91 mg·g-1), La-graphite sheets (26.06 mg·g-1), and Fe-graphite sheets (40.26 mg·g-1). The FL-graphite sheets conformed to the Freundlich and Dubinin-Radushkevich isotherm, and the maximum adsorption capacity was 53.62 mg·g-1. The removal process obeys intra-particle diffusion and pore diffusion for As(III). The results of batch adsorption experiments and characterization analyses demonstrated that oxidation, ligand exchange, and inner sphere complexation mechanisms involved in the adsorption of FL-graphite sheets to As(III) in comparison with graphite sheets. In addition, electrostatic attraction mechanism was found vital in the adsorption. Ecotoxicity assessment revealed that FL-graphite sheets have little influence on rice germination and growth, but reduced the toxicity of As(III) to rice. Therefore, the FL-graphite sheets have good practical application value in purifying As(III) polluted water with litter ecotoxicity.
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  • 文章类型: Journal Article
    作为(III)S-腺苷甲硫氨酸甲基转移酶,砷代谢中的关键酶,促进砷的甲基化达三倍。该过程主要产生三价单亚砷酸盐和二甲基亚砷酸盐,与三甲基砷化氢形成较少量。As(III)对半胱氨酸残基的强亲和力,形成As(III)-硫醇盐键,在医疗中被利用。在这项研究中,我们扩展了对As(III)约束机制的理解,证明这一点,除了As(III)-S共价键,非共价O···由于pnictogen键起着至关重要的作用。这种相互作用显著有助于As(III)配合物的结构稳定性。我们使用As(III)S-腺苷甲硫氨酸甲基转移酶的PDB数据库进行晶体学分析,通过全面的理论研究,包括分子静电势(MEP),分子中原子的量子理论(QTAIM),和自然键轨道(NBO)分析,强调了pnictogen键合在这些系统中的关键作用。我们还使用各种理论模型对这些pnictogen键的能量特性进行了详细的评估。据我们所知,这是首次在生物系统中报道As(III)衍生物中的pnictogen键,标志着我们对砷分子相互作用的理解有了显著的进步。
    As(III) S-adenosylmethionine methyltransferases, pivotal enzymes in arsenic metabolism, facilitate the methylation of arsenic up to three times. This process predominantly yields trivalent mono- and dimethylarsenite, with trimethylarsine forming in smaller amounts. While this enzyme acts as a detoxifier in microbial systems by altering As(III), in humans, it paradoxically generates more toxic and potentially carcinogenic methylated arsenic species. The strong affinity of As(III) for cysteine residues, forming As(III)-thiolate bonds, is exploited in medical treatments, notably in arsenic trioxide (Trisenox®), an FDA-approved drug for leukemia. The effectiveness of this drug is partly due to its interaction with cysteine residues, leading to the breakdown of key oncogenic fusion proteins. In this study, we extend the understanding of As(III)\'s binding mechanisms, showing that, in addition to As(III)-S covalent bonds, noncovalent O⋅⋅⋅As pnictogen bonding plays a vital role. This interaction significantly contributes to the structural stability of the As(III) complexes. Our crystallographic analysis using the PDB database of As(III) S-adenosylmethionine methyltransferases, augmented by comprehensive theoretical studies including molecular electrostatic potential (MEP), quantum theory of atoms in molecules (QTAIM), and natural bond orbital (NBO) analysis, emphasizes the critical role of pnictogen bonding in these systems. We also undertake a detailed evaluation of the energy characteristics of these pnictogen bonds using various theoretical models. To our knowledge, this is the first time pnictogen bonds in As(III) derivatives have been reported in biological systems, marking a significant advancement in our understanding of arsenic\'s molecular interactions.
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  • 文章类型: Journal Article
    从水中取出As(III)的目的是减少有毒金属对人类和自然造成的损害。一种能吸收As(III)的物质,TFPOTDB-SO3H,是通过将2,5-二氨基苯磺酸和2,4,6-三-(4-甲酰基苯氧基)-1,3,5-三嗪在将分子连接在一起的反应中组合制备的。该物质可以很好地吸附As(III),并且具有出色的品质,例如易于再次使用,单独的物质,过滤掉液体。在pH=8和室温下,TFPOTDB-SO3H吸附了大量的As(III)。它在10min内达到了97.1%的去除率,可以吸附高达344.8mg/g。进行了一项研究,以研究共存阴离子对砷的消除作用。研究结果表明,阴离子的存在具有最小的不利影响,减少As(III)摄取约1-7%。发现吸收过程的动力学受准二级动力学模型控制,而Langmuir等温线模型验证了As(III)去除的机制是单层化学吸附。根据热力学分析,吸附过程是吸热的,自发发生。此外,即使经过4个连续的吸附-解吸循环,吸附剂对As(III)保留了88.86%的大量吸收生产率。结果共同表明,TFPOTDB-SO3H对于有效吸附和消除废水中的As(III)离子具有相当大的希望。
    The goal of taking out As(III) from water is to reduce the detriment that poisonous metals can do to people and nature. A substance that can absorb As(III), TFPOTDB-SO3H, was made by combining 2,5-diaminobenzenesulfonic acid and 2,4,6-tris-(4-formylphenoxy)-1,3,5-triazine in a reaction that joins molecules together. This substance can adsorb As(III) very well and has excellent qualities like being easy to use again, separate substances, and filter out liquids. At pH = 8 and at room temperature, TFPOTDB-SO3H adsorbed a lot of As(III). It achieved a removal rate of 97.1 % within 10 min and could adsorb up to 344.8 mg/g. A research was conducted to investigate the effect of co-existing anions on the elimination of arsenic. The findings indicated that the presence of anions had a minimal adverse impact, reducing As(III) uptake by approximately 1-7 %. The kinetics of the uptake process were found to be controlled by the quasi-second order kinetic model, while the Langmuir isotherm model validated that the mechanism for As(III) removal was monolayer chemisorption. According to the thermodynamic analysis, the adsorption process was endothermic and occurred spontaneously. Moreover, even after 4 successive adsorption-desorption cycles, the adsorbent preserved a substantial uptake productivity of 88.86 % for As(III). The results collectively indicate that TFPOTDB-SO3H holds considerable promise for the efficient adsorption and elimination of As(III) ions from wastewater.
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  • 文章类型: Journal Article
    水稻可以比其他作物植物积累更多的有机和无机砷(iAs)。在这项研究中,基于来自两个省的26个水稻品种,使用高效液相色谱-电感耦合等离子体质谱法(HPLC-ICP-MS)研究了水稻籽粒中As的定位。在所有的样本中,精米中总砷含量为0.03-0.37mg/kg,两组样品的平均值分别为0.28和0.21mg/kg。稻米不同成分中砷形态的测定结果表明,在精米和糙米中,亚砷酸盐(As(III))的平均值几乎是砷酸盐(As(V))的两倍。总砷含量和砷形态均存在区域差异。原因可能是As(III)在解离形式下比As(V)更具流动性,并且由于土壤性质,水稻品种,和成长环境。米糠中iAs和总As的比例高于精米,这是因为As倾向于在外壳和胚乳之间积累。在我们的研究中,硒可以减轻水稻生长初期砷中毒的风险。发芽稻中砷和硒的共同暴露表明,精米中砷的积累减少了73.8%,76.8%,和总As的78.3%,As(III),和As(V)与单独用As处理的水稻相比。硒(0.3mg/kg)和砷的添加显着降低了发芽稻米不同部位的砷含量。我们的结果表明,硒生物强化可以减轻水稻作物中砷的积累和毒性。
    Rice can accumulate more organic and inorganic arsenic (iAs) than other crop plants. In this study, the localization of As in rice grains was investigated using High Performance Liquid Chromatography-Inductively Coupled Plasma Mass Spectrometry (HPLC-ICP-MS) based on 26 rice varieties collected from two provinces. In all the samples, the total As contents in polished rice were 0.03-0.37 mg/kg, with average values of 0.28 and 0.21 mg/kg for two sample sets. The results of the determination of arsenic speciation in different components of rice grain showed that in the polished and brown rice the mean value of arsenite (As(III)) was nearly twice than that of arsenate (As(V)). The regional difference was observed in both total As contents and As speciation. The reason may be that As(III) is more mobile than As(V) in a dissociated form and because of soil properties, rice varieties, and the growing environment. The proportion of iAs and the total As in rice bran was higher than that in polished rice, and this is because As tends accumulate between the husk and the endosperm. In our study, selenium could alleviate the risk of arsenic toxicity at the primary stage of rice growth. Co-exposure to As and Se in germinated rice indicated that the reduction in As accumulation in polished rice reached 73.8%, 76.8%, and 78.3% for total As, As(III), and As(V) when compared with rice treated with As alone. The addition of Se (0.3 mg/kg) along with As significantly reduced the As amount in different parts of germinated rice. Our results indicated that Se biofortification could alleviate the As accumulation and toxicity in rice crops.
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  • 文章类型: Journal Article
    在这项工作中,一种新的树枝状聚合物改性的磁性氧化石墨烯(GO)被用作电沉积Au纳米颗粒的基底。改良的磁性电极用于灵敏测量As(III)离子作为公认的人类致癌物。所制备的电化学装置对使用方波阳极溶出伏安法(SWASV)方案的As(III)检测表现出优异的活性。在最佳条件下(在pH5.0的0.1M乙酸盐缓冲液中,沉积电位为-0.5V,持续100s),线性范围为1.0至125.0μgL-1,低检出限(由S/N=3计算)为0.47μgL-1。除了所提出的传感器的简单性和灵敏度,它对一些主要干扰剂的高选择性,例如Cu(II)和Hg(II)使其成为筛选As(III)的可观的传感工具。此外,该传感器对不同水样中As(III)的检测结果令人满意,所得数据的准确性通过电感耦合等离子体原子发射光谱法(ICP-AES)确定。会计的高度敏感性,显著的选择性和良好的重现性,所建立的电化学策略对于分析环境基质中的As(III)具有巨大的潜力。
    In this work, a new dendrimer modified magnetic graphene oxide (GO) was used as a substrate for electrodeposition of Au nanoparticles. The modified magnetic electrode was employed for sensitive measuring of As(III) ion as a well-established human carcinogen. The prepared electrochemical device exhibits excellent activity towards As(III) detection using the square wave anodic stripping voltammetry (SWASV) protocol. At optimum conditions (deposition potential at -0.5 V for 100 s in 0.1 M acetate buffer with pH 5.0), a linear range from 1.0 to 125.0 μgL-1 with a low detection limit (calculated by S/N = 3) of 0.47 μg L-1 was obtained. In addition to the simplicity and sensitivity of the proposed sensor, its high selectivity against some major interfering agents, such as Cu(II) and Hg(II) makes it an appreciable sensing tool for the screening of As(III). In addition, the sensor revealed satisfactory results for detection of As(III) in different water samples, and the accuracy of obtained data were confirmed by inductively coupled plasma atomic emission spectroscopy (ICP-AES) setup. Accounting for the high sensitivity, remarkable selectivity and good reproducibility, the established electrochemical strategy has great potential for analysis of As(III) in environmental matrices.
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  • 文章类型: Journal Article
    虽然高铁酸钾(K2FeO4)对水中重金属的去除能力已被许多研究者证实,很少有信息集中在元素周期表的同一家族中元素的单独和同时处理之间的差异。在这个项目中,两种重金属,以砷(As)和锑(Sb)为目标污染物,考察了模拟水和加标湖水样品中K2FeO4的去除能力和腐殖酸(HA)的影响。结果表明,随着Fe/As或Sb的质量比,两种污染物的去除效率逐渐增加。当初始As(III)浓度为0.5mg/L时,在pH为5.6,Fe/As质量比为4.6时,As(III)的最大去除率达到99.5%;而当初始Sb(III)浓度为0.5mg/L时,pH为4.5时Sb(III)的最大去除率为99.61%,Fe/Sb为22.6。发现HA对单个As或Sb的去除略有抑制作用,并且Sb的去除效率显着高于添加或不添加K2FeO4的As。对于As和Sb的共存体系,添加K2FeO4后,As的去除率大大提高,高于Sb;而后者比不含K2FeO4的As略好,这可能是由于HA和Sb的络合能力更强。X射线能量色散谱(EDS),X射线衍射仪(XRD),和X射线光电子能谱(XPS)用于表征沉淀产物,以揭示潜在的去除机理基于实验结果。
    Although the removal ability of potassium ferrate (K2FeO4) on aqueous heavy metals has been confirmed by many researchers, little information focuses on the difference between the individual and simultaneous treatment of elements from the same family of the periodic table. In this project, two heavy metals, arsenic (As) and antimony (Sb) were chosen as the target pollutants to investigate the removal ability of K2FeO4 and the influence of humic acid (HA) in simulated water and spiked lake water samples. The results showed that the removal efficiencies of both pollutants gradually increased along the Fe/As or Sb mass ratios. The maximum removal rate of As(III) reached 99.5% at a pH of 5.6 and a Fe/As mass ratio of 4.6 when the initial As(III) concentration was 0.5 mg/L; while the maximum was 99.61% for Sb(III) at a pH of 4.5 and Fe/Sb of 22.6 when the initial Sb(III) concentration was 0.5 mg/L. It was found that HA inhibited the removal of individual As or Sb slightly and the removal efficiency of Sb was significantly higher than that of As with or without the addition of K2FeO4. For the co-existence system of As and Sb, the removal of As was improved sharply after the addition of K2FeO4, higher than Sb; while the latter was slightly better than that of As without K2FeO4, probably due to the stronger complexing ability of HA and Sb. X-ray energy dispersive spectroscopy (EDS), X-ray diffractometer (XRD), and X-ray photoelectron spectroscopy (XPS) were used to characterize the precipitated products to reveal the potential removal mechanisms based on the experimental results.
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  • 文章类型: Journal Article
    在这项研究中,开发了一种基于原位沉积改性的丝网印刷碳电极(SPCE),快速,线性扫描阳极溶出伏安法(LSASV)测定水和茶叶中的As(III)。将丝网印刷的碳电极置于由As(III)溶液组成的溶液中,氯金酸和L-半胱氨酸。在一定的电势下,在SPCE上,氯金酸被还原成金纳米颗粒(AuNPs)。L-半胱氨酸自组装到AuNPs上并促进As(III)的富集,从而提高了As(III)的测定特异性和灵敏度。该方法的测定限(LOD)为0.91ppb(µgL-1),线性范围为1~200µgL-1,测定间变异系数为5.3%,特异性好。该方法已成功应用于自来水和茶叶样品中As(Ⅲ)的测定,回收率为93.8%~105.4%,并通过电感耦合等离子体质谱(ICP-MS)进一步验证。所开发的方法是快速的,方便准确,在现场测定自来水和茶叶中的As(III)方面有很大的希望,它可以扩展到其他样品的检测。
    In this study, a screen-printed carbon electrode (SPCE) based on in situ deposition modification was developed for the sensitive, rapid, easy and convenient determination of As(III) in water and tea by linear sweep anodic stripping voltammetry (LSASV). The screen-printed carbon electrodes were placed in a solution consisting of As(III) solution, chlorauric acid and L-cysteine. Under certain electrical potential, the chloroauric acid was reduced to gold nanoparticles (AuNPs) on the SPCE. L-cysteine was self-assembled onto AuNPs and promoted the enrichment of As(III), thus enhancing the determination specificity and sensitivity of As(III). The method achieved a limit of determination (LOD) of 0.91 ppb (µg L-1), a linear range of 1~200 µg L-1, an inter-assay coefficient of variation of 5.3% and good specificity. The developed method was successfully applied to the determination of As(III) in tap water and tea samples, with a recovery rate of 93.8%~105.4%, and further validated by inductively coupled plasma mass spectrometry (ICP-MS). The developed method is rapid, convenient and accurate, holding great promise in the on-site determination of As(III) in tap water and tea leaves, and it can be extended to the detection of other samples.
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  • 文章类型: Journal Article
    这项研究描述了2-肼基苯并噻唑改性的酰胺/酰亚胺共聚物的开发,用于萃取/预浓缩痕量As(III),从食用植物油。它们的表征是通过仪器技术实现的。该方法基于在35倍过量的As(V)存在下,As(III)和共聚螯合剂之间的pH依赖性络合,它们选择性地提取到混合胶束相中,并通过紫外可见分光光度计在pH2.0和6.0下检测。优化了影响提取效率的变量。从20毫升样品的预浓缩中,在1-40和3-75µg/L的范围内具有良好的线性关系,DL为0.32和1.00µg/L。通过分析没有加标和有加标的认证样品来验证准确性。将该方法应用于样品的iAs水平分析。结果表明,该功能共聚物是有效的螯合剂,并显示出从食用植物油中选择性提取As(III)的巨大潜力。
    This study describes the development of 2-hydrazinobenzothiazole modified-amide/imide co-polymers for the extraction/pre-concentration of trace As(III), from edible vegetable oils. Their characterization was realized by help of instrumental techniques. The method is based on pH-dependent complexation between As(III) and co-polymeric chelators in presence of 35-fold excess As(V), their selective extraction into the mixed micellar phase, and detected at pH 2.0 and 6.0 by UV-vis spectrophotometer. The variables affecting extraction efficiency were optimized. From pre-concentration of 20-mL sample, the good linear relationships were obtained in range of 1-40 and 3-75 µg/L with DLs of 0.32 and 1.00 µg/L. The accuracy was verified by analysis of a certified sample without and with spiking. The method was applied into the analysis of iAs levels of samples. The results show that the functional co-polymers are efficient chelators, and exhibit great potential for the selective extraction of As(III) from edible vegetable oils.
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