Day: September 6, 2021

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Soluble amyloid-beta oligomer (AbetaO) is believed to be a reliable molecular biomarker for the diagnosis of Alzheimer’s disease (AD) because of its high toxicity for neuronal synapse and higher concentration level in cerebrospinal fluid sample from AD patient than from control individual. At present, it is critical to develop a simple method for AbetaO detection with low cost as well as high sensitivity and selectivity. In this work, we reported an antibody-free electrochemical method for the detection of AbetaO based on the specific interaction between AbetaO and PrP(95-110) peptide, a segment of cellular prion protein. Specifically, cysteine-containing PrP(95-110) peptide was first immobilized on a gold electrode for the capture of AbetaO. Then, alkaline phosphatase-conjugated PrP(95-110) was used for the recognition of the captured AbetaO and the generation of electroactive species. Furthermore, an “outer-sphere to inner-sphere” electrochemical-chemical-chemical (ECC) redox cycling using ferrocene methanol as the redox mediator was employed to enhance the detection sensitivity. As a result, a detection limit of 3 pM for equivalent monomer was achieved. The amenability of this method to AbetaO analysis in a biological matrix was demonstrated by assays of AbetaO in serum samples.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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This paper describes the electrochemical reduction of nitrite ion in neutral aqueous solution mediated by tetraruthenated metalloporphyrins (Co(II), Ni(II) and Zn(II)) electrostatically assembled onto a Nafion film previously adsorbed on glassy carbon or ITO electrodes. Scanning electron microscope (SEM-EDX) and transmission electron microscopy (TEM) results have shown that on ITO electrodes the macrocycles forms multiple layers with a disordered stacking orientation over the Nafion film occupying hydrophobic and hydrophilic sites in the polyelectrolyte. Atomic force microscopy (AFM) results demonstrated that the Nafion film is 35 nm thick and tetraruthenated metalloporphyrins layers 190 nm thick presenting a thin but compacted morphology. Scanning electrochemical microscopy (SECM) images shows that the Co(II) tetraruthenated porphyrins/Nf/GC modified electrode is more electrochemically active than their Ni and Zn analogues. These modified electrodes are able to reduce nitrite at -660 mV showing enhanced reduction current and a decrease in the required overpotential compared to bare glassy carbon electrode. Controlled potential electrolysis experiments verify the production of ammonia, hydrazine and hydroxylamine at potentials where reduction of solvent is plausible demonstrating some selectivity toward the nitrite ion. Rotating disc electrode voltammetry shows that the factor that governs the kinetics of nitrite reduction is the charge propagation in the film.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

Chemical engineers work across a number of sectors, processes differ within each of these areas, but chemistry and chemical engineering roles are found throughout, creation and manufacturing process of chemical products and materials. Recommanded Product: 1273-86-5. Catalysts allow a reaction to proceed via a pathway that has a lower activation energy than the uncatalyzed reaction. Introducing a new discovery about 1273-86-5, Name is Ferrocenemethanol

Collisional activation (CA) mass spectrometry has been employed to show that C6H6Fe+ ions formed upon electron impact of dicarbonyl-(eta5-2,4-cyclopentadienyl)-methyliron consist of a 1:1 mixture of fulvene-iron and benzene-iron structures.Analysis of daughter-ion spectra of the deuterium-labelled analogue shows that there exist two independent fragmentation routes leading to the different ion structures.These routes differ in the sequence in the sequence in which the CO ligands and H2 are lost from the molecular ion.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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Alkene-based self-assembled monolayers grafted on oxidized Pt surfaces were used as a scaffold to covalently immobilize oxidase enzymes, with the aim to develop an amperometric biosensor platform. NH2-terminated organic layers were functionalized with either aldehyde (CHO) or N-hydroxysuccinimide (NHS) ester-derived groups, to provide anchoring points for enzyme immobilization. The functionalized Pt surfaces were characterized by X-ray photoelectron spectroscopy (XPS), static water contact angle (CA), infrared reflection absorption spectroscopy (IRRAS) and atomic force microscopy (AFM). Glucose oxidase (GOX) was covalently attached to the functionalized Pt electrodes, either with or without additional glutaraldehyde crosslinking. The responses of the acquired sensors to glucose concentrations ranging from 0.5 to 100 mM were monitored by chronoamperometry. Furthermore, lactate oxidase (LOX) and human hydroxyacid oxidase (HAOX) were successfully immobilized onto the PtOx surface platform. The performance of the resulting lactate sensors was investigated for lactate concentrations ranging from 0.05 to 20 mM. The successful attachment of active enzymes (GOX, LOX and HAOX) on Pt electrodes demonstrates that covalently functionalized PtOx surfaces provide a universal platform for the development of oxidase enzyme-based sensors.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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An effective mild procedure for the reductive deoxygenation of alpha-ferrocenyl aldehydes, ketones, and alcohols into the corresponding alkylferrocenes is described using a combination of zinc borohydride and zinc chloride. This is the first example of such reactivity of zinc borohydride. The present method allows the synthesis of alkylferrocenes bearing terminally functionalized pendant chains.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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The sol-gel polycondensation of tetramethoxysilane has been followed for the first time by functionalization of the oligomeric silane species with a redox active ferrocene. Recording the decrease of the average diffusion coefficient of the mobile species brings information on the sol or gel state, as well as an easy insight of the polycondensation kinetics.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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Microorganisms exploit extracellular electron transfer (EET) with external minerals during their growth. This process is accompanied by the conversion of chemical energy. Direct electron transfer (DET) from the microorganisms to solid electron acceptors via membrane-bound cytochrome c enzymes or conductive nanowires/pili has been reported. In previous studies, mediated electron transfer (MET) has also been demonstrated to occur through electrochemically active metabolites acting as redox mediators. The microorganisms with EET capabilities have been harnessed for bioelectrochemical systems (BESs) in the bioremediation of environmental contaminants and the production of biofuels and nanomaterials. Electron transfer at the electrode biofilm/solution interface is one of the core phenomena occurring in BESs. The study of the redox reactions occurring in the microenvironment of the biofilm should elucidate the mechanism of microbial EET, which will then help improve the electron transfer efficiency of BESs. The composition of a biofilm is complex and contains many redox secreta and extracellular polymeric substances. Therefore, the specific current generated from the DET or MET pathways cannot be solely detected using classic electrochemical methods. In the present study, the interfacial electron transfer of Shewanella oneidensis MR-1 on an ITO surface was investigated. Cyclic voltammetry (CV) was first applied to study the redox properties of Shewanella and its interaction with ferrocenylmethanol (FcMeOH), which served as an exogenous electron mediator. The cyclic voltammograms showed that the oxidation current of S. oneidensis MR-1 was dramatically enhanced in the presence of 0.01 mmol·L-1 FcMeOH compared to a control, i.e. bacterium-free ITO. This can be explained by the ability of S. oneidensis MR-1 to reduce FcMeOH+ during the positive scan. These results also showed that FcMeOH was a good redox mediator and capable of transferring electrons between the electrode and the bacterial cells. In addition, using the penetration mode in scanning electrochemical microscopy, the current generated from the MET by FcMeOH was collected using a microelectrode. Examination of the approaching curve showed that the current started to increase when the tip was approaching the solution/biofilm interface, providing positive feedback for the FcMeOH-mediated electron transfer between the microelectrode and the bacterial cells. The electrode biofilm/solution microenvironment was also detected, showing the thickness of the solution/biofilm to be 500 mum and the thickness of the biofilm to be 1100 mum. This study indicates that scanning electrochemical microscopy can be used in studying microbial MET. It also provides insight into the electron transfer mechanism of the microbial metabolism from a physical chemistry perspective.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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A generic amperometric bioassay based on the enzymatic oxidation catalysed by the stable NADH oxidase (NAox) from Thermus thermophilus has been developed for NADH measurements. The NAox uses O2 as its natural electron acceptor and produces H2O2 in a two-electron process. Electrochemical and spectrophotometric experiments showed that the NAox used in this work, presents a very good activity towards its substrate and, in contrary to previously mentioned NADH oxidases, does not require the addition of any exogenous flavin cofactor neither to promote nor to maintain its activity. In addition, the NAox used also works with artificial electron acceptors like ferrocene derivatives. O2 was successfully replaced by redox mediators such as hydroxymethyl ferrocene (FcCH2OH) for the regeneration of the active enzyme. Combining the NAox with the mediator and the horseradish peroxidase we developed an original, high sensitive “redox-flexible” NADH amperometric bioassay working in a large window of applied potentials in both oxidation and reduction modes. The biosensor has a continuous and complementary linearity range permitting to measure NADH concentrations starting from 5 × 10-6 M in reduction until 2 × 103 M in oxidation. This redox-flexibility allows choosing the applied potential in order to avoid electrochemical interferences. The association of the “redox-flexible” concept with NADH dependent enzymes opens a novel strategy for dehydrogenases based bioassays and biosensors. The great number of dehydrogenases available makes the concept applicable for numerous substrates to analyse. Moreover it allows the development of a wide range of biosensors on the basis of a generic platform. This gives several advantages over the previous manufacturing techniques and offers a general and flexible scheme for the fabrication of biosensors presenting high sensitivities, wide calibration ranges and less affected by electrochemical interferences.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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Autooxidation of ethoxymethylferrocene at 30-50C promoted by the participation of strong and weak carboxylic acids HX is studied. The radical chain mechanism of the process is established, its kinetics characteristics are determined as well as the composition of the products among which other derivatives of ferrocene have been found. Based on the results of the present study and the earlier obtained data on oxidation of hydroxymethylferrocene a mechanism of initiation of the chains general for both metallocomplexes is suggested. It includes the formation of the intermediate CH2OR (R = H, C2H5) and its subsequent oxidative transformations leading to the formation of the peroxide radical C5H 4Fe+?C5H4-CH2O 2 ? and ROH. The role of the approaching and orientation effect in transformations of this intermediate is discussed as well as the mechanism of the investigated reaction in general.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion

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The design and synthesis of two new receptors, C20H 19O3BFe and C20H21O3BFe and their anion sensing properties through multiple channels are reported. Both the receptors, having chelating boronic ester Lewis acidic centre as the sole binding site, selectively bind fluoride ion in micromolar concentration. The binding constant of C20H19O3BFe with the fluoride ion has been found to be quite high [K = 106 M -1], whereas it displays a negligible affinity towards other effective competitors, for example acetate and cyanide (K = 10 M-1) and no sensitivity towards other halide ions. Upon selective recognition of F- in acetonitrile, the redox potential of C20H 19O3BFe shifted by DeltaE = 200 mV and the fluorescence emission was quenched drastically. The considerable changes in their absorption spectra are accompanied by the appearance of a new low energy (LE) peak at 566 nm and by a strong colour change from yellow to deep green which allows the prospective for “naked eye” detection of F- anion.

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Reference：
Iron Catalysis in Organic Synthesis | Chemical Reviews,
Iron Catalysis in Organic Synthesis: A Critical Assessment of What It Takes To Make This Base Metal a Multitasking Champion