Dataset Information

Triethylenetetramine-Based Semiconducting Fe(III) Metallogel: Effective Catalyst for Aryl-S Coupling.

ABSTRACT: A fascinating way to originate a mechanically stable metallogel of ferric ions with metal-coordinating organic ligand triethylenetetramine through direct mixing of their water solutions in a stoichiometric ratio is achieved under ambient conditions. The rheological study established the mechanical property of the Fe(III) metallogel. A cashew-shaped microstructure of the metallogel was observed by FESEM analysis. The electrical property of the Fe(III) metallogel was also carefully scrutinized. The semiconducting features like the Schottky barrier diode property of the Fe(III) metallogel were explored. The catalytic role of the Fe(III) metallogel was also critically explored. The Fe(III) metallogel shows an excellent catalytic property toward the synthesis of aryl thioethers via a C-S coupling reaction under mild reaction conditions without the use of any organic solvent.

SUBMITTER: Dhibar S

PROVIDER: S-EPMC7033679 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Triethylenetetramine-Based Semiconducting Fe(III) Metallogel: Effective Catalyst for Aryl-S Coupling.

Dhibar Subhendu S Dey Arka A Ghosh Debasish D Majumdar Santanu S Dey Amiya A Ray Partha Pratim PP Dey Biswajit B

ACS omega 20200210 6

A fascinating way to originate a mechanically stable metallogel of ferric ions with metal-coordinating organic ligand triethylenetetramine through direct mixing of their water solutions in a stoichiometric ratio is achieved under ambient conditions. The rheological study established the mechanical property of the Fe(III) metallogel. A cashew-shaped microstructure of the metallogel was observed by FESEM analysis. The electrical property of the Fe(III) metallogel was also carefully scrutinized. Th ...[more]

PMID: 32095691

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Project description:To evaluate the microbial populations involved in the reduction of Fe(III) in an acidic, iron-rich sediment, the anaerobic flow of supplemental carbon and reductant was evaluated in sediment microcosms at the in situ temperature of 12 degrees C. Supplemental glucose and cellobiose stimulated the formation of Fe(II); 42 and 21% of the reducing equivalents that were theoretically obtained from glucose and cellobiose, respectively, were recovered in Fe(II). Likewise, supplemental H(2) was consumed by acidic sediments and yielded additional amounts of Fe(II) in a ratio of approximately 1:2. In contrast, supplemental lactate did not stimulate the formation of Fe(II). Supplemental acetate was not consumed and inhibited the formation of Fe(II). Most-probable-number estimates demonstrated that glucose-utilizing acidophilic Fe(III)-reducing bacteria approximated to 1% of the total direct counts of 4', 6-diamidino-2-phenylindole-stained bacteria. From the highest growth-positive dilution of the most-probable-number series at pH 2. 3 supplemented with glucose, an isolate, JF-5, that could dissimilate Fe(III) was obtained. JF-5 was an acidophilic, gram-negative, facultative anaerobe that completely oxidized the following substrates via the dissimilation of Fe(III): glucose, fructose, xylose, ethanol, glycerol, malate, glutamate, fumarate, citrate, succinate, and H(2). Growth and the reduction of Fe(III) did not occur in the presence of acetate. Cells of JF-5 grown under Fe(III)-reducing conditions formed blebs, i.e., protrusions that were still in contact with the cytoplasmic membrane. Analysis of the 16S rRNA gene sequence of JF-5 demonstrated that it was closely related to an Australian isolate of Acidiphilium cryptum (99.6% sequence similarity), an organism not previously shown to couple the complete oxidation of sugars to the reduction of Fe(III). These collective results indicate that the in situ reduction of Fe(III) in acidic sediments can be mediated by heterotrophic Acidiphilium species that are capable of coupling the reduction of Fe(III) to the complete oxidation of a large variety of substrates including glucose and H(2).

Project description:Whole-genome DNA microarray analysis of Geobacter sulfurreducens cells grown on Fe(III)-oxide or Mn(IV)-oxide versus cells grown on soluble Fe(III) citrate indicated that there were significant differences in transcription patterns during growth on the insoluble metal oxides compared to growth on soluble Fe(III). Many of the genes that appeared to be up-regulated during growth on the metal hydroxides were involved in electron transport. The most highly up-regulated genes for both conditions were omcS and omcT, which encode co-transcribed c-type cytochromes exposed on the outer surface of the cell that are known to be required for Fe(III) and Mn(IV)-oxide reduction. Other electron transport genes that were up-regulated on both insoluble metals included the gene coding for the outer membrane c-type cytochrome, OmcG, genes for the outer membrane proteins, OmpB and OmpC, and the gene that codes for the structural protein of electrically conductive pili, PilA. Genes that were up-regulated in cells grown on Fe(III)-oxide but not Mn(IV)-oxide, included outer membrane c-type cytochromes including OmcE, a putative DMSO reductase protein, and proteins from the cytochrome bc1 complex. Electron transport genes that were only up-regulated in Mn(IV)-oxide grown cells included the genes that code for the outer membrane c-type cytochromes, OmcZ and OmcB, the periplasmic c-type cytochrome, MacA, and fumarate reductase. Genetic studies indicated that the c-type cytochrome proteins, PpcH, OmcJ, OmcM, OmcV, MacA, OmcF, OmcI, and OmcQ, and the iron sulfur subunit of the cytochrome b/b6 complex, QcrA, are important for reduction of insoluble Fe(III)-oxides but do not appear to be important for Mn(IV) reduction. These results demonstrate that the physiology of Fe(III) reducing bacteria differ significantly during growth on insoluble electron and soluble electron acceptors and emphasizes the importance of c-type cytochromes in extracellular electron transfer in G. sulfurreducens. Geobacter sulfurreducens cells were grown with acetate (5 mM) provided as the electron donor and either Fe(III) oxide or Fe(III) citrate provided as the electron acceptor. Cells were harvested at mid-log and total RNA was extracted. Total RNA (0.5 μg) was amplified using the MessageAmp II-Bacteria Kit (Ambion, Foster City, CA) according to the manufacturers instructions. Ten micrograms of amplified RNA (aRNA) was chemically labeled with Cy3 (for the control or soluble electron acceptor condition) or Cy5 (for the experimental or insoluble electron acceptor condition) dye using the MicroMax ASAP RNA Labeling Kit (Perkin Elmer, Wellesley, MA) according to the manufacturer’s instructions.

Dataset Information

Triethylenetetramine-Based Semiconducting Fe(III) Metallogel: Effective Catalyst for Aryl-S Coupling.

Publications

Triethylenetetramine-Based Semiconducting Fe(III) Metallogel: Effective Catalyst for Aryl-S Coupling.

Similar Datasets

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