Chelating Materials Immobilizing Carboxymethylated Pentaethylenehexamine and Polyethyleneimine as Ligands

Kagaya, Shigehiro; Inoue, Yasuhiro

doi:10.2116/analsci.30.35

Cited by 21 publications

(6 citation statements)

References 101 publications

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“…The seaFAST-pico TM system buffers acidified seawater inline before loading onto a column, containing a high-affinity resin with carboxymethylated polyethylenimine as the chelating ligand to retain transition metals while allowing the bulk seawater major ion matrix to pass through. Concentrated samples are eluted into clean collection vials (Kagaya and Inoue, 2014) and trace metal concentrations are determined in the eluent by triple quadrupole ICP-MS/MS (Jackson et al, 2018). Procedural blank solution was prepared fresh for each batch of samples following Lagerström et al (2013).…”

Section: Dissolved Copper Complexationmentioning

confidence: 99%

Seasonal dissolved copper speciation in the Strait of Georgia, British Columbia, Canada

et al. 2022

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The Strait of Georgia (SoG) is a semi-enclosed, urban basin with seasonally dependent estuarine water circulation, dominantly influenced by Northeast Pacific waters and the Fraser River. To establish a baseline and understand the fate and potential toxicity of Cu in the SoG, we determined seasonal and spatial depth profiles of dissolved Cu (dCu) speciation, leading to estimates of the free hydrated copper (Cu2+) concentrations, as a proxy for Cu toxicity. The concentration of dCu was largely controlled by conservative mixing of the ocean and freshwater endmembers in the SoG. In all samples, ligand concentrations exceeded dCu, by a ratio greater than 1.5, resulting in the complexation of 99.98% of the dCu by strong binding organic ligands. The concentrations of Cu2+ were less than 10-13.2 M, significantly lower than the well-established Cu toxicity threshold (10-12 M Cu2+) for microorganisms. Our results indicate that ambient Cu-binding ligands effectively buffer Cu2+ concentrations within the Strait of Georgia, posing no threat to marine life. In almost 90% of the samples, the ligands were best classified as a single ligand class, with a logKCuL,Cu2+cond between 12.5 and 14.1. The concentrations of these single class ligands were greatest in warm, low salinity, nutrient depleted waters, suggesting that either terrestrially sourced ligands dominate dCu speciation in the SoG, or freshwater sources in the SoG establish the conditions that promote the production of Cu binding ligands in its surface waters. The remaining 10% of the samples were from the euphotic zone, where we detected a stronger ligand class, L1, of logKCuL1,Cu2+cond between 13.5 and 14.3, and a weaker ligand class, L2, of logKCuL2,Cu2+cond between 11.5 and 12.3. In these surface samples, logKCuL1,Cu2+cond and logKCuL2,Cu2+cond were positively correlated with temperature, while L2 concentrations were positively correlated with chromophoric dissolved organic matter of terrestrial origin. This study is the first to perform hierarchal clustering of a trace metal speciation dataset and enabled the distinction of 6 clusters across season, depth, and region of the SoG, highlighting the influence of freshwater and open ocean ligand sources, conservative mixing dynamics, and particulate Cu concentrations on dCu speciation within estuarine basins.

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Section: Dissolved Copper Complexationmentioning

confidence: 99%

Seasonal dissolved copper speciation in the Strait of Georgia, British Columbia, Canada

et al. 2022

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“…Depending on the way of its synthesis, PEI can be linear, branched, or even dendritic . Branched forms are mostly synthesized by the acid-catalyzed ring-opening polymerization of aziridine, while the linear variant is made from poly(2-ethyl-2-oxazoline) by acidic hydrolysis. , Besides being mostly used in its raw form, PEI is a valuable starting material due to its easily substitutable hydrogen atoms. , …”

Section: Introductionmentioning

confidence: 99%

Synthesis and Characterization of Carboxymethylated Polyethylenimines

Novák,

Miklósi,

Nyul

et al. 2023

ACS Appl. Polym. Mater.

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As potential paramagnetic metal ion complexing macromolecular ligands, carboxymethylated polyethylenimines (CM-PEIs) were successfully prepared from polyethylenimine (PEI) with 2-chloroacetic acid (CA) in an alkaline medium. SEC, pH-potentiometry, DLS, and multinuclear and multidimensional NMR techniques were used to determine the degree of functionalization, size, and possible structure of the modified polymers. By varying the amount of CA, functionalization degrees of 7–67% relative to the theoretical maximum were achieved. Diffusometry shows that the PEI and CM-PEIs are highly hydrated. The CM-PEIs are larger molecules than the parent PEI, although their hydrodynamic size decreases with higher degrees of functionalization. CM-PEIs are isostable except for the most highly substituted derivative. CM-PEIs form complexes with Cu(II) and efficiently decrease the rate of the copper-mediated oxidation of ascorbic acid. The good affinity toward cations of CM-PEI functionalized at 67% is further demonstrated by its capacity to bind even sodium ions. These properties show that CM-PEIs are promising metal-chelating polymers for diagnostic or theranostic purposes.

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“…Recently, it has been found that a chelating resin immobilizing carboxymethylated polyethyleneimine (CM-PEI), which is classified as an aminocarboxylic acid group, is a material capable of achieving selective extraction of some trace elements. [24][25][26][27][28][29][30] The CM-PEI resin is prepared by immobilizing PEI on a methacrylate resin and then carboxymethylating the PEI on the resin with sodium monochloroacetate. The carboxymethylation (CM) rate, which is defined as the ratio of the amount of the carboxylic acid group to that of the amino group in the PEI, can be controlled by the amount of monochloroacetate used for the carboxymethylation process.…”

Section: Introductionmentioning

confidence: 99%

Phosphomethylated Polyethyleneimine-immobilized Chelating Resin: Role of Phosphomethylation Rate on Solid-Phase Extraction of Trace Elements

et al. 2019

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Chelating resins immobilizing phosphomethylated polyethyleneimine (PM-PEI) with different phosphomethylation (PM) rates were prepared by using different amounts of both phosphonic acid and paraformaldehyde in the phosphomethylation of PEI immobilized on a methacrylate resin as a base resin. The extraction of many elements improved with increasing PM rate; REEs, Be, Fe, Mo, Ti, and V were quantitatively extracted at pH 2. The elution of the elements tended to become difficult with increasing PM rate. When a PM-PEI resin with a PM rate of 0.26 was used, REEs and Be could be eluted using 0.2 mol L -1 EDTA solution adjusted to a pH of 7 and 3 mol L -1 nitric acid, respectively, although the elution of Fe, Mo, Ti, and V was insufficient. The PM-PEI resin could be reused at least 10 times to recover REEs and Be without the influence of any other elements. The PM-PEI resin could be applied to a recovery test using artificial seawater spiked with REEs, except for Sc, Tm, Yb, and Lu, and the separation of the REEs in NIST SRM 1515 Apple Leaves.

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Chelating Materials Immobilizing Carboxymethylated Pentaethylenehexamine and Polyethyleneimine as Ligands

Cited by 21 publications

References 101 publications

Seasonal dissolved copper speciation in the Strait of Georgia, British Columbia, Canada

Seasonal dissolved copper speciation in the Strait of Georgia, British Columbia, Canada

Synthesis and Characterization of Carboxymethylated Polyethylenimines

Phosphomethylated Polyethyleneimine-immobilized Chelating Resin: Role of Phosphomethylation Rate on Solid-Phase Extraction of Trace Elements

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