Browse
Submit Data
Databases
API
Help

Dataset Information

15 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Electrocatalytic Volleyball: Rapid Nanoconfined Nicotinamide Cycling for Organic Synthesis in Electrode Pores.

ABSTRACT: In living cells, redox chains rely on nanoconfinement using tiny enclosures, such as the mitochondrial matrix or chloroplast stroma, to concentrate enzymes and limit distances that nicotinamide cofactors and other metabolites must diffuse. In a chemical analogue exploiting this principle, nicotinamide adenine dinucleotide phosphate (NADPH) and NADP⁺ are cycled rapidly between ferredoxin-NADP⁺ reductase and a second enzyme-the pairs being juxtaposed within the 5-100 nm scale pores of an indium tin oxide electrode. The resulting electrode material, denoted (FNR+E2)@ITO/support, can drive and exploit a potentially large number of enzyme-catalysed reactions.

SUBMITTER: Megarity CF

PROVIDER: S-EPMC6491978 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Progress in Scaling up and Streamlining a Nanoconfined, Enzyme-Catalyzed Electrochemical Nicotinamide Recycling System for Biocatalytic Synthesis.

Project description:An electrochemically driven nicotinamide recycling system, referred to as the 'electrochemical leaf' has unique attributes that may suit it to the small-scale industrial synthesis of high-value chemicals. A complete enzyme cascade can be immobilized within the channels of a nanoporous electrode, allowing complex reactions to be energized, controlled and monitored continuously in real time. The electrode is easily prepared by depositing commercially available indium tin oxide (ITO) nanoparticles on a Ti support, resulting in a network of nanopores into which enzymes enter and bind. One of the enzymes is the photosynthetic flavoenzyme, ferredoxin NADP+ reductase (FNR), which catalyzes the quasi-reversible electrochemical recycling of NADP(H) and serves as the transducer. The second enzyme is any NADP(H)-dependent dehydrogenase of choice, and further enzymes can be added to build elaborate cascades that are driven in either oxidation or reduction directions through the rapid recycling of NADP(H) within the pores. In this Article, we describe the measurement of key enzyme/cofactor parameters and an essentially linear scale-up from an analytical scale 4 mL reactor with a 14 cm2 electrode to a 500 mL reactor with a 500 cm2 electrode. We discuss the advantages (energization, continuous monitoring that can be linked to a computer, natural enzyme immobilization, low costs of electrodes and low cofactor requirements) and challenges to be addressed (optimizing minimal use of enzyme applied to the electrode).

| S-EPMC7756331 | biostudies-literature

Flexible 2D Cu Metal: Organic Framework@MXene Film Electrode with Excellent Durability for Highly Selective Electrocatalytic NH<sub>3</sub> Synthesis.

Project description:Electrocatalytic nitrate reduction to ammonia (ENRA) is an effective strategy to resolve environmental and energy crisis, but there are still great challenges to achieve high activity and stability synergistically for practical application in a fluid environment. The flexible film electrode may solve the abovementioned problem of practical catalytic application owing to the advantages of low cost, light weight, eco-friendliness, simple and scalable fabrication, extensive structural stability, and electrocatalytic reliability. Herein, 2D hybridization copper 1,4-benzenedi-carboxylate (CuBDC) has been grown on electronegative MXene nanosheets (Ti3C2Tx) seamlessly to prepare a 2D flexible CuBDC@Ti3C2Tx electrode for ENRA. The flexible electrode simultaneously exhibits high Faradaic efficiency (86.5%) and excellent stability for NH3 synthesis, which are comparable to previously reported nanomaterials toward ENRA. Especially, the flexible electrode maintains outstanding FE NH3 toward ENRA after the bending, twisting, folding, and crumpling tests, indicating excellent electroconductibility, high stability, and durability. This work not only provides mild permeation-mediated strategy to fabricate a flexible electrode but also explores the practical applications of the electrode with effectively environmental adaptability in solving global environmental contamination and energy crisis by effective ENRA.

| S-EPMC9175116 | biostudies-literature

Rapid Synthesis and Correlative Measurements of Electrocatalytic Nickel/Iron Oxide Nanoparticles.

Project description:Electrocatalytic core-shell nanoparticles, such as nickel/iron oxides for the oxygen evolution reaction (OER) in alkaline electrolytes, require rapid synthesis and measurement for practical use. To meet this challenge, we investigated a novel process of adding Ni(II) species to Fe nanoparticles immediately after synthesis, which we expected to yield Ni-rich shells around Fe-rich cores. Cyclic voltammetry showed that the overpotential decreased as the molar ratio of Ni to Fe in the synthesis vessel increased from 0.2?mol Ni:1?mol Fe to 1.5?mol Ni:1?mol Fe, consistent with an increase of Ni composition. Unexpectedly, the overpotential increased abruptly at 2.0?mol Ni:1?mol Fe. X-ray photoelectron spectroscopy revealed that this synthesis ratio resulted in less Ni at the nanoparticle surfaces than lower synthesis ratios. These results demonstrate the sensitivity of rapid electrochemical measurements to surface composition, and the limits of Ni(II) adsorption and reduction to rapidly form Ni-rich shells around Fe-rich cores. Cyclic voltammetry also showed that the onset of the methanol oxidation reaction (MOR) correlates with the oxidation of Ni(OH)2 to NiOOH. Therefore, tuning materials to improve performance as OER catalysts also improves their performance as MOR catalysts.

| S-EPMC5854608 | biostudies-literature

On the complex structural diffusion of proton holes in nanoconfined alkaline solutions within slit pores.

Project description:The hydroxide anion OH(-)(aq) in homogeneous bulk water, that is, the solvated proton hole, is known to feature peculiar properties compared with excess protons solvated therein. In this work, it is disclosed that nanoconfinement of such alkaline aqueous solutions strongly affects the key structural and dynamical properties of OH(-)(aq) compared with the bulk limit. The combined effect of the preferred hypercoordinated solvation pattern of OH(-)(aq), its preferred perpendicular orientation relative to the confining surfaces, the pronounced layering of nanoconfined water and the topology of the hydrogen bond network required for proton hole transfer lead to major changes of the charge transport mechanism, in such a way that the proton hole migration mechanism depends exquisitely on the width of the confined space that hosts the water film. Moreover, the anionic Zundel complex, which is of transient nature in homogeneous bulk solutions, can be dynamically trapped as a shallow intermediate species by suitable nanoconfinement conditions.

| S-EPMC4996981 | biostudies-literature

Rapid Cycling and Exceptional Yield in a Metal-Organic Framework Water Harvester.

Project description:Sorbent-assisted water harvesting from air represents an attractive way to address water scarcity in arid climates. Hitherto, sorbents developed for this technology have exclusively been designed to perform one water harvesting cycle (WHC) per day, but the productivities attained with this approach cannot reasonably meet the rising demand for drinking water. This work shows that a microporous aluminum-based metal-organic framework, MOF-303, can perform an adsorption-desorption cycle within minutes under a mild temperature swing, which opens the way for high-productivity water harvesting through rapid, continuous WHCs. Additionally, the favorable dynamic water sorption properties of MOF-303 allow it to outperform other commercial sorbents displaying excellent steady-state characteristics under similar experimental conditions. Finally, these findings are implemented in a new water harvester capable of generating 1.3 L kgMOF -1 day-1 in an indoor arid environment (32% relative humidity, 27 °C) and 0.7 L kgMOF -1 day-1 in the Mojave Desert (in conditions as extreme as 10% RH, 27 °C), representing an improvement by 1 order of magnitude over previously reported devices. This study demonstrates that creating sorbents capable of rapid water sorption dynamics, rather than merely focusing on high water capacities, is crucial to reach water production on a scale matching human consumption.

| S-EPMC6813556 | biostudies-literature

Electrocatalytic carboxylation of halogenated compounds with mesoporous silver electrode materials.

Project description:Mesoporous silver materials are used as electrocatalysts for halogenated compounds. The mesoporous silver materials have uniform mesoporous size (8 nm), large specific surface area (12 m2 g-1), high pore volume (0.07 cm3 g-1), and a good 3D network structure of the metallic silver skeleton. The results show that the prepared materials exhibit high performance in electrocatalytic carboxylation of halogenated compounds to acid (78%).

| S-EPMC9034108 | biostudies-literature

Li<sup>+</sup> Dynamics of Liquid Electrolytes Nanoconfined in Metal-Organic Frameworks.

Project description:Metal-organic frameworks (MOFs) are excellent platforms to design hybrid electrolytes for Li batteries with liquid-like transport and stability against lithium dendrites. We report on Li+ dynamics in quasi-solid electrolytes consisting in Mg-MOF-74 soaked with LiClO4-propylene carbonate (PC) and LiClO4-ethylene carbonate (EC)/dimethyl carbonate (DMC) solutions by combining studies of ion conductivity, nuclear magnetic resonance (NMR) characterization, and spin relaxometry. We investigate nanoconfinement of liquid inside MOFs to characterize the adsorption/solvation mechanism at the basis of Li+ migration in these materials. NMR supports that the liquid is nanoconfined in framework micropores, strongly interacting with their walls and that the nature of the solvent affects Li+ migration in MOFs. Contrary to the "free'' liquid electrolytes, faster ion dynamics and higher Li+ mobility take place in LiClO4-PC electrolytes when nanoconfined in MOFs demonstrating superionic conductor behavior (conductivity σrt > 0.1 mS cm-1, transport number tLi+ > 0.7). Such properties, including a more stable Li electrodeposition, make MOF-hybrid electrolytes promising for high-power and safer lithium-ion batteries.

| S-EPMC8603352 | biostudies-literature

Electrocatalytic oxidation of water at a polyoxometalate nanoparticle modified gold electrode.

Project description:Spherical polyoxometalate nanoparticles, [HPMo]NPs, were synthesized from a very well known Keggin-type polyoxometalate [H3PMo12O40] in the presence of sodium dodecyl sulphate (SDS) and polyvinyl pyrrolidine (PVP) in aqueous medium and characterized by UV-Vis spectroscopy and Transmission Electron Microscopy (TEM). The [HPMo]NPs were used to modify a gold working electrode and they were characterized by SEM, EDX, elemental mapping, cyclic voltammetry and electrochemical impedance spectroscopy and applied for the electrocatalytic oxidation of water in a phosphate buffer solution at neutral pH. The modified electrode showed excellent electrocatalytic activity towards oxidation of water at an impressively low overpotential ∼350 mV with a high current density of around 1.7 mA cm-2, good stability under exhaustive electrolysis conditions and also showed long term stability.

| S-EPMC9076066 | biostudies-literature

Investigating the Cycling Stability of Fe2WO6 Pseudocapacitive Electrode Materials.

Project description:The stability upon cycling of Fe2WO6 used as a negative electrode material for electrochemical capacitors was investigated. The material was synthesized using low temperature conditions for the first time (220 °C). The electrochemical study of Fe2WO6 in a 5 M LiNO3 aqueous electrolyte led to a specific and volumetric capacitance of 38 F g-1 and 240 F cm-3 when cycled at 2 mV·s-1, respectively, associated with a minor capacitance loss after 10,000 cycles. In order to investigate this very good cycling stability, both surface and bulk characterization techniques (such as Transmission Electron Microscopy, Mössbauer spectroscopy, and magnetization measurements) were used. Only a slight disordering of the Fe3+ cations was observed in the structure, explaining the good stability of the Fe2WO6 upon cycling. This study adds another pseudocapacitive material to the short list of compounds that exhibit such a behavior up to now.

| S-EPMC8230245 | biostudies-literature

Integrated electrocatalytic synthesis of ammonium nitrate from dilute NO gas on metal organic frameworks-modified gas diffusion electrodes

Project description: Not available

| S-EPMC11341735 | biostudies-literature