Hg(II) ions

  • 文章类型: Journal Article
    为了有效去除水体中的重金属Hg(II),设计了一种新型的MgAl层状双氢氧化物(LDH)吸附剂,并用席夫碱进行了功能化。吸附剂(MgAl-LDH@SiO2-AG)的表征结果表明,席夫碱聚合物成功地包覆在具有六方结构的MgAl-LDH的外表面上。在pH7和298K时,对Hg(II)的理论最大吸附容量为228.46mg/g。研究了从pH2到8的不同pH溶液,MgAl-LDH@SiO2-AG对Hg(II)的最佳容量在pH=7.2,T=36.8°C时达到268.7mg/g,C0=32.1mg/L,剂量=0.083g/L在现实中,该吸附剂不仅能有效去除各种水体中的Hg(II),包括湖水,河水,污水处理厂的废水,而且对含有不同重金属离子的电镀废水也有很好的选择性。现实废水中低含量的TN和TP对Hg(Ⅱ)的去除影响较小。此外,制备的吸附剂具有良好的可重用性和稳定性。反应机理主要涉及与含氮/氧基团的螯合以及氮原子在席夫碱官能团中的主要参与。汞(II)的去除依赖于伪二级动力学和Langmuir模型,是吸热和自发的化学反应。本工作提供了一种实用的方法,可以用LDH复合材料制备高效的吸附材料,并处理水体中的重金属Hg(II)。
    To effectively remove heavy metal Hg(II) from water bodies, a novel adsorbent of MgAl-layered double hydroxide (LDH) was designed and functionalized with Schiff base. The characterization results of the adsorbent (MgAl-LDH@SiO2-AG) show that the Schiff base polymer was successfully coated onto the outside surface of MgAl-LDH with hexagonal structure. The theoretical maximum adsorption capacity to Hg(II) is 228.46 mg/g at pH 7 and 298 K. The different pH solutions were investigated from pH 2 to 8, and the optimal capacity of MgAl-LDH@SiO2-AG toward Hg(II) achieves 268.7 mg/g at pH = 7.2, T = 36.8 °C, C0 = 32.1 mg/L and dosage = 0.083 g/L. In reality, the adsorbent not only exhibits efficient removal of Hg(II) in various water bodies, including lake water, river water, effluent from sewage treatment plant, but also has an excellent selectivity in electroplating wastewater containing different heavy metal ions. Low contents of TN and TP in real wastewater have less effect on the removal of Hg(II). Moreover, the prepared adsorbent had a good reusability and stability. The reaction mechanism mainly involves chelation with nitrogen/oxygen-containing groups and the predominant participation of nitrogen atoms in the Schiff base functional group. The removal of Hg(II) relies on the pseudo-second-order kinetics and Langmuir model, and is an endothermic and spontaneous chemical reaction. The present work offers a practical method for preparing highly effective adsorptive materials with the LDH composites and for the treatment of heavy metal Hg(II) from water bodies.
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  • 文章类型: Journal Article
    水污染已经成为一个严重的问题,汞(II)离子(Hg(II))即使在低浓度下也具有剧毒。因此,应严格监测Hg(II)浓度。这项研究评估了吡唑啉化合物作为用于Hg(II)检测的荧光化学传感器剂。这些化合物是由香草醛通过醚化制备的,Claisen-Schmidt,和环缩合反应,得到苯并噻唑-吡唑啉-苯乙烯杂化化合物。以97.70%的产率成功合成了不含苯乙烯的杂化化合物,检测限(LoD)和定量限(LoQ)值为323.5和1078μM,分别。相反,杂合化合物以97.29%的产率产生,LoD和LoQ值为8.94和29.79nM,分别。进一步的光谱研究表明,Hg(II)离子可以与吡啶的三个氮螯合,吡唑啉,和苯并噻唑结构或两个氧的香草醛和苯乙烯。此外,该杂化化合物已成功应用于自来水和地下水样品中Hg(II)离子的直接定量,有效期分别为91.63%和86.08%,分别,与汞分析仪测量相比。通过加入乙二胺四乙酸溶液也容易实现吡唑啉的再生。这些发现表明,苯并噻唑-吡唑啉-苯乙烯杂化化合物在实际环境样品中的Hg(II)监测中具有广阔的应用前景。
    Water pollution has become a serious issue, and mercury(II) ion (Hg(II)) is highly toxic even at low concentrations. Therefore, Hg(II) concentration should be strictly monitored. This study evaluated pyrazoline compounds as fluorescence chemosensor agents for Hg(II) detection. These compounds were prepared from vanillin via etherification, Claisen-Schmidt, and cyclocondensation reactions, to yield benzothiazole-pyrazoline-styrene hybrid compounds. The hybrid compound without styrene was successfully synthesized in 97.70% yield with limit of detection (LoD) and limit of quantification (LoQ) values of 323.5 and 1078 μM, respectively. Conversely, the hybrid compound was produced in 97.29% yield with the LoD and LoQ values of 8.94 and 29.79 nM, respectively. Further spectroscopic investigations revealed that Hg(II) ions can either chelate with three nitrogen of pyridine, pyrazoline, and benzothiazole structures or two oxygen of vanillin and styrene. Furthermore, the hybrid compound was successfully applied in the direct quantification of Hg(II) ions in tap and underground water samples with a validity of 91.63% and 86.08%, respectively, compared with mercury analyzer measurement. The regeneration of pyrazoline was also easily achieved via the addition of an ethylenediaminetetraacetic acid solution. These findings show the promising application of the benzothiazole-pyrazoline-styrene hybrid compound for Hg(II) monitoring in real environmental samples.
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  • 文章类型: Journal Article
    在这里,有效和潜在的螯合α-氨基膦酸酯基吸附剂(AP-)衍生自三种不同的胺来源(苯胺/邻氨基苯甲酸/邻苯二胺)以形成AP-H,作为AP-H的羧化和胺化增强的氨基膦酸酯,AP-COOH,和AP-NH2通过简单的方法合成。使用不同的技术阐明了合成吸附剂的结构;元素分析(CHNP/O),FT-IR,NMR(1H-,13C和31PNMR),TGA和BET。利用制造的吸附剂通过吸附性能从水溶液中去除Hg(II)。由Langmuir方程拟合的等温线:最佳pH5.5和T:25±1°C时的最大吸附容量,发现AP-COOH为1.33、1.23和1.15mmolHgg-1,AP-NH2,AP-H,分别,这大致与活性位点密度和吸附剂反应基团的硬/软特性相关。根据硬酸和软酸和碱(HSAB)理论,金属-配体结合亲和力在质量上是合理的。与参考材料(AP-H)相比,Hg(II)(软)对AP-COOH的相互作用比AP-NH2(硬)具有更强的亲和力,可以认为是更软的碱。根据空间效应调节和比表面积,该序列结果显示了相反的趋势,与它们的倒数性质一致。ΔH°绝对值的热力学分析,ΔS°和ΔG°提供了对Hg(II)吸附的选择性,其顺序如下:AP-COOH>AP-NH2>AP-H。通过HCl溶液进行洗脱和再生,并循环至少五个循环。吸附和解吸效率大于91%。这种吸附剂表现出良好的耐久性,汞(II)去除的稳定性和有希望的潜力。最后,一种新的建模技术,用于定量非线性描述和比较扩展关系的3D空间中的等效地理位置。使用建议的Floatotherm(包括Van\'tHoff参数模型)观察到放热和自发行为。
    Herein, efficient and potential chelating α-aminophosphonate based sorbents (AP-) derived from three different amine origins (aniline/anthranilic acid/O-phenylenediamine) to form AP-H, carboxylated and aminated enhanced aminophosphonate as AP-H, AP-COOH, and AP-NH2 were synthesized via a facile method. The structure of the synthesized sorbents was elucidated using different techniques; elemental analysis (CHNP/O), FT-IR, NMR (1H-, 13C and 31P NMR), TGA and BET. The fabricated sorbents were exploited for Hg(II) removal from aqueous solution via sorption properties. Isotherm fitted by Langmuir equation: the maximum sorption capacities at optimum pH 5.5, and T:25 ± 1 °C, were found to be 1.33, 1.23, and 1.15 mmol Hg g-1 for AP-COOH, AP-NH2, AP-H, respectively, which is roughly correlated with the active sites density and the hard/soft characteristics of adsorbents\' reactive groups. Metal-ligand binding affinities are qualitatively rationalized in terms of hard and soft acids and bases (HSAB) theory. The interaction of Hg(II) (soft) has a stronger affinity to AP-COOH can be considered a softer base compared with reference material (AP-H) over than AP-NH2 (hard). This sequence result showed opposite trends consistent with their reciprocal properties according to the steric effect modulates and the specific surface area. Thermodynamics analysis for absolute values of ΔH°, ΔS° and ΔG° afford the selectivity towards Hg(II) sorption with the following order: AP-COOH > AP-NH2 >AP-H. Elution and regeneration was carried out by HCl solution and recycled for a minimum of five cycles, the sorption and desorption efficiencies are greater than 91%. Such sorbents exhibit good durability, stability and promising potential for Hg(II) removal. Finally, a new modelling technique for quantitative non-linear description and comparison of equivalent geographical positions in 3D space of extended relationships. Exothermic and spontaneous behavior were observed using a proposed Floatotherm that included the Van\'t Hoff parameters model.
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  • 文章类型: Journal Article
    基于聚集诱导发射(AIE)机制,合成了一种新的荧光探针TPE-GHK,其中包含四苯乙烯(TPE)衍生物作为荧光团和经典三肽(Gly-His-Lys-NH2)作为受体。TPE-GHK在其他竞争性金属离子中显示出高选择性和对Hg2的快速荧光“开启”响应。通过荧光滴定法验证了TPE-GHK对Hg2+的2:1复合物结合机制,作业的情节,和ESI-HRMS光谱。荧光发射在0-1.0μM范围内显示出良好的线性响应,低检测限为28.6nM。同时,TPE-GHK表现出优异的生物相容性和低毒性,并成功地用于监测活CAKI2细胞中的Hg2。证明了其在环境和生物科学中的潜在应用。更重要的是,TPE-GHK可用于检测两个真实水样中的Hg2,并成功设计为测试条。
    A new fluorescent probe TPE-GHK was synthesized containing a tetrastyrene (TPE) derivative as fluorophore and classical tripeptide (Gly-His-Lys-NH2) as a receptor based on the aggregation-induced emission (AIE) mechanism. TPE-GHK displayed high selectivity and rapid fluorescent \"turn-on\" response to Hg2+ among other competitive metal ions. The 2:1 complex binding mechanism of TPE-GHK toward Hg2+ was verified by fluorometric titration, Job\'s plots, and ESI-HRMS spectra. The fluorescent emission showed a good linear response in the range of 0-1.0 μM with the low detection limit of 28.6 nM. Meanwhile, TPE-GHK exhibited the excellent biocompatibility and low toxicity and was successfully applied in monitoring Hg2+ in living CAKI 2 cells, which demonstrated its potential application in environment and biological science. More importantly, TPE-GHK could be used to detect Hg2+ in two real water samples and also was successfully designed as test strips.
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  • 文章类型: Journal Article
    In the field of nanotechnology, nanoadsorbents have emerged as a powerful tool for the purification of contaminated aqueous environments. Among the variety of nanoadsorbents developed so far, magnetite (Fe3O4) nanoparticles have drawn particular interest because of their quick separation, low cost, flexibility, reproducibility, and environmentally benign nature. Herein, we describe a new strategy for the synthesis of Fe3O4 nanoclusters, which is based on the use of naturally available edible mushrooms (Pleurotus eryngii) and environmentally benign propylene glycol as a solvent medium. By tuning the temperature, we successfully convert Fe3O4 nanoparticles into Fe3O4 nanoclusters via hydrothermal treatment, as evidenced by transmission electron microscopy. The Fe3O4 nanoclusters are functionalized with an organic molecule linker (dihydrolipoic acid, DHLA) to remove hazardous Hg(II) ions selectively. Batch adsorption experiments demonstrate that Hg(II) ions are strongly adsorbed on the material surface, and X-ray photoelectron and Fourier transform infrared spectroscopy techniques reveal the Hg(II) removal mechanism. The DHLA@Fe3O4 nanoclusters show a high removal efficiency of 99.2 % with a maximum Hg(II) removal capacity of 140.84 mg g-1. A kinetic study shows that the adsorption equilibrium is rapidly reached within 60 min and follows a pseudo second-order kinetic model. The adsorption and separation system can be readily recycled using an external magnet when the separation occurs within 10 s. We have studied the effect of various factors on the adsorption process, including pH, concentration, dosage, and temperature. The newly synthesized superparamagnetic DHLA@Fe3O4 nanoclusters open a new path for further development of the medical, catalysis, and environmental fields.
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  • 文章类型: Journal Article
    在这项研究中,制备了一种新型单宁酸交联纤维素/聚乙烯亚胺功能化磁性复合材料(MCP)作为Hg(II)离子的生物质吸附剂。用FT-IR对MCP的形貌和结构进行了表征,TG,XRD,SEM和TEM。pH等不同因素的影响,接触时间,初始Hg(II)离子浓度,研究了吸附温度对吸附行为的影响。结果表明,MCP具有良好的选择性和再利用率,去除率快,和非常高的吸附能力。当pH值达到99.00%和247.51mg/g时,吸附时间,在293K时,Hg(II)离子浓度分别为5、180分钟和100mg/L。动力学遵循伪二级,表明MCP对Hg(Ⅱ)离子的吸附行为属于化学吸附过程和外扩散过程。热力学研究表明,吸附过程是一个自发的放热过程。经过第五次吸附-解吸实验,仍具有较好的吸附性能和再利用率。总而言之,MCP具有高度稳定和高效,以及出色的可重用性将成为汞(II)离子废水的工业级应用的候选人。
    In this study, a new tannic acid cross-linking cellulose/polyethyleneimine functionalized magnetic composite (MCP) as a biomass adsorbent of Hg(II) ions was prepared. The morphology and structure of MCP were characterized with FT-IR, TG, XRD, SEM and TEM. The effect of the different factors such as pH, contact time, initial Hg(II) ion concentration, and adsorption temperature on the adsorption behavior was investigated. The results showed that MCP exhibited an excellent selectivity and reutilization, fast removal rate, and very high adsorption capacity. The corresponding adsorption capacity and removal rate of could reach 99.00% and 247.51 mg/g when the pH value, adsorption time, Hg(II) ion concentration were 5, 180 min and 100 mg/L at 293 K. The kinetics followed the pseudo-second-order, which indicated that the adsorption behavior of MCP for Hg(II) ion belonged to the chemical adsorption process and external diffusion. The thermodynamic study showed that the adsorption process was a spontaneous and exothermic process. After the fifth adsorption-desorption experiment, it still had better adsorption performance and reutilization. All in all, MCP with highly stable and efficient, as well as excellent reusability will be a candidate for industry-level applications from wastewater with Hg(II) ions.
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  • 文章类型: Journal Article
    Carbon dots and gold nanoclusters co-encapsulated by zeolitic imidazolate framework-8 (CDs/AuNCs@ZIF-8) have been obtained at room temperature. The composite has been applied to the ratiometric fluorescence determination of mercury(II). The composite shows fluorescence emission maxima at 440 and 640 nm under 360 nm excitation, due to the CDs and AuNCs, respectively (associated quantum yields were 18% and 17%, respectively). In the presence of Hg2+, the fluorescence at about 640 nm is quenched, while the fluorescence at about 440 nm is unaffected. The CDs/AuNCs@ZIF-8 composite allows the sensitive detection of Hg2+, with the fluorescence intensity ratio (I640/I440) decreasing linearly with Hg2+ concentration over the range 3-30 nM. The fluorescence emission of the composite changes color from red to blue with increasing Hg2+ under UV excitation, which can easily be discerned visually. This visual detection of Hg2+ is due to the high fluorescence quantum yields of the CDs and AuNCs and the ~ 200 nm separation between the two emission maxima. Graphical abstract (A) Schematic diagram showing the operating principle of the determination for Hg(II). (B) Digital graph of the solutions in absence and presence of 30 nM Hg(II) under a portable UV lamp.
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  • 文章类型: Journal Article
    In the current work, Cu(I)1.28Cu(II)0.36Se nanoparticles were synthesized via a simple procedure and were applied for the first time for recognition, adsorption, enrichment, and detection of Hg(II) ions. The experimental results show that 99.9% Hg(II) could be adsorbed by Cu(I)1.28Cu(II)0.36Se nanoparticles within just 30 s, and the Hg(II) concentration could be lowered down to a super-low level of 0.01 ppb. Cu(I)1.28Cu(II)0.36Se nanoparticles also demonstrate high selectivity to Hg(II) and Ag(I) among nine representative metal ions. The enrichment experiments show that Hg(II) of ultratrace concentration could be enriched significantly by Cu(I)1.28Cu(II)0.36Se nanoparticles, and thus, the detection limit of Hg(II) based on inductively coupled plasma emission spectroscopy-mass spectrometry would be pushed down by 2 orders of magnitude. These outstanding features of Cu(I)1.28Cu(II)0.36Se nanoparticles could be well accounted for in terms of the solubility product principle and the high affinity between selenium and mercury. Cu(I)1.28Cu(II)0.36Se nanoparticles were also found to have peroxidase-like activity, which could be inhibited by Hg(II) but not by Ag(I). This unique characteristic coupled with the solubility product principle successfully allows recognition and detection of Hg(II) even in the presence of Ag(I), which has a similar pKsp to Hg(II). As a result, the qualitative and quantitative analyses of Hg(II) could be performed by the naked eye and UV-visible spectroscopy, respectively. The current results indicate that Cu(I)1.28Cu(II)0.36Se nanoparticles not only have great potential in various aspects of dealing with Hg(II) pollution but would also shed light on discovering new nanomaterials to address other heavy metal ions.
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  • 文章类型: Journal Article
    Mercury is one of the most hazardous pollutants, and mercury pollution is a serious hazard to our environment. Herein, we designed and synthesized a new peptide-based fluorescent chemosensor (L) based on a Fmoc-Lys (Fmoc)-OH backbone conjugated with two Serines and dansyl groups using solid phase peptide synthesis (SPPS) technology. L exhibited highly selective and excellent sensitive detection of Hg2+ ions in 100% aqueous solutions through fluorescence quenching. The chemosensor L forms a 2:1 stoichiometry with high binding constants (4.89×106M-1) and the detection limit for Hg2+ ions of the proposed assay was 7.59nM. In addition, the recovery test results of Hg2+ concentration in actual water samples showed that the quantitative detection of Hg2+ ions can be realized in two water samples. Moreover, L showed low cytotoxicity and excellent membrane permeability in HK2 cells, which has been successfully applied for monitoring Hg2+ ions in living LNCaP cells.
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  • 文章类型: Journal Article
    目前,磁性介孔二氧化硅纳米球由于其大的表面积和易于回收而被广泛用作吸附剂。在这里,功能化的磁性介孔二氧化硅/有机聚合物纳米复合材料(MMSP)是通过接枝聚(间氨基苯硫酚)嵌入基于Fe3O4磁芯的胺化磁性介孔二氧化硅纳米复合材料,它被介孔二氧化硅壳化,并进一步被(3-氨基丙基)三乙氧基硅烷改性。通过改变实验参数,系统地研究了开发的MMSP的吸附性能。结果表明,在pH4.0条件下,MMSP的吸附量和去除率仅在10min内就可以达到243.83mg/g和97.53%,共存离子对水溶液中Hg(II)离子的选择性去除没有显着影响。同时,磁体回收吸附剂经5次回收后仍表现出良好的吸附性能。此外,通过分析实验数据,Hg(II)离子的吸附过程属于自发放热吸附,并基于伪二阶模型和Langmuir模型提出了可能的吸附机理。经过吸附研究,开发了吸附汞(II)的废料作为苯乙炔转化为苯乙酮的高效催化剂,收率为97.06%。在这项研究中,我们设计了一种高效和选择性的材料来去除Hg(II)离子,并通过将废物转化为优异的催化剂来处理后吸附的汞吸附剂,降低了传统吸附技术对经济和环境的影响。
    Currently, magnetic mesoporous silica nanospheres have been employed widely as adsorbents due to their large surface area and easy recovery. Herein, the functionalized magnetic mesoporous silica/organic polymers nanocomposite (MMSP) was fabricated by the grafted poly(m-aminothiophenol) embedded the aminated magnetic mesoporous silica nanocomposite based on Fe3O4 magnetic core, which was shelled by mesoporous silica and further modified by (3-aminopropyl) triethoxysilane. The adsorption properties of as-developed MMSP were systematically explored by altering the experimental parameters. The results indicated that the adsorption capacity and removal percentage of the MMSP could reach 243.83 mg/g and 97.53% within only 10 min at pH 4.0, and the coexisting ions had no significant effect on the selective Hg(II) ions removal from aqueous solutions, meanwhile, the adsorbent recovered by a magnet still exhibited good adsorption performance after recycled 5 times. In addition, by analyzing experimental data, the adsorption process of Hg(II) ions belonged to spontaneous exothermic adsorption, and the possible adsorption mechanisms were proposed based on the pseudo-second-order model and Langmuir model. After adsorption study, the waste material adsorbed Hg(II) was developed as an efficient catalyst for transformation of phenylacetylene to acetophenone with yield of 97.06%. In this study, we designed an efficient and selective material for Hg(II) ions remove and provided a treatment of the post-adsorbed mercury adsorbent by converting the waste into an excellent catalyst, which reduced the economic and environmental impact from conventional adsorption techniques.
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