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Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes.

ABSTRACT: Discerning the influence of electrochemical reactions on the electrode microenvironment is an unavoidable topic for electrochemical reactions that involve the production of OH^- and the consumption of water. That is particularly true for the carbon dioxide reduction reaction (CO₂ RR), which together with the competing hydrogen evolution reaction (HER) exert changes in the local OH^- and H₂ O activity that in turn can possibly affect activity, stability, and selectivity of the CO₂ RR. We determine the local OH^- and H₂ O activity in close proximity to a CO₂ -converting Ag-based gas diffusion electrode (GDE) with product analysis using gas chromatography. A Pt nanosensor is positioned in the vicinity of the working GDE using shear-force-based scanning electrochemical microscopy (SECM) approach curves, which allows monitoring changes invoked by reactions proceeding within an otherwise inaccessible porous GDE by potentiodynamic measurements at the Pt-tip nanosensor. We show that high turnover HER/CO₂ RR at a GDE lead to modulations of the alkalinity of the local electrolyte, that resemble a 16 m KOH solution, variations that are in turn linked to the reaction selectivity.

SUBMITTER: Dieckhofer S

PROVIDER: S-EPMC8048634 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Combining Nanoconfinement in Ag Core/Porous Cu Shell Nanoparticles with Gas Diffusion Electrodes for Improved Electrocatalytic Carbon Dioxide Reduction

Project description:Abstract Bimetallic silver‐copper electrocatalysts are promising materials for electrochemical CO2 reduction reaction (CO2RR) to fuels and multi‐carbon molecules. Here, we combine Ag core/porous Cu shell particles, which entrap reaction intermediates and thus facilitate the formation of C2+ products at low overpotentials, with gas diffusion electrodes (GDE). Mass transport plays a crucial role in the product selectivity in CO2RR. Conventional H‐cell configurations suffer from limited CO2 diffusion to the reaction zone, thus decreasing the rate of the CO2RR. In contrast, in the case of GDE‐based cells, the CO2RR takes place under enhanced mass transport conditions. Hence, investigation of the Ag core/porous Cu shell particles at the same potentials under different mass transport regimes reveals: (i) a variation of product distribution including C3 products, and (ii) a significant change in the local OH‐ activity under operation. Direct comparison of the impact of the CO2 mass transport on the performance of Ag core/porous Cu shell nanoparticles for CO2 reduction between a conventional H‐cell and a gas‐diffusion electrode cell provides the basis for a decrease of the competing hydrogen evolution and boosting the formation of C2 and C3 products.

| S-EPMC9303450 | biostudies-literature

Probing the local activity of CO<sub>2</sub> reduction on gold gas diffusion electrodes: effect of the catalyst loading and CO<sub>2</sub> pressure.

Project description:Large scale CO2 electrolysis can be achieved using gas diffusion electrodes (GDEs), and is an essential step towards broader implementation of carbon capture and utilization strategies. Different variables are known to affect the performance of GDEs. Especially regarding the catalyst loading, there are diverging trends reported in terms of activity and selectivity, e.g. for CO2 reduction to CO. We have used shear-force based Au nanoelectrode positioning and scanning electrochemical microscopy (SECM) in the surface-generation tip collection mode to evaluate the activity of Au GDEs for CO2 reduction as a function of catalyst loading and CO2 back pressure. Using a Au nanoelectrode, we have locally measured the amount of CO produced along a catalyst loading gradient under operando conditions. We observed that an optimum local loading of catalyst is necessary to achieve high activities. However, this optimum is directly dependent on the CO2 back pressure. Our work does not only present a tool to evaluate the activity of GDEs locally, it also allows drawing a more precise picture regarding the effect of catalyst loading and CO2 back pressure on their performance.

| S-EPMC8654039 | biostudies-literature

Gas Diffusion Electrodes on the Electrosynthesis of Controllable Iron Oxide Nanoparticles.

Project description:The electrosynthesis of iron oxide nanoparticles offers a green route, with significant energy and environmental advantages. Yet, this is mostly restricted by the oxygen solubility in the electrolyte. Gas-diffusion electrodes (GDEs) can be used to overcome that limitation, but so far they not been explored for nanoparticle synthesis. Here, we develop a fast, environmentally-friendly, room temperature electrosynthesis route for iron oxide nanocrystals, which we term gas-diffusion electrocrystallization (GDEx). A GDE is used to generate oxidants and hydroxide in-situ, enabling the oxidative synthesis of a single iron salt (e.g., FeCl2) into nanoparticles. Oxygen is reduced to reactive oxygen species, triggering the controlled oxidation of Fe2+ to Fe3+, forming Fe3-xO4-x (0 ≤ x ≤ 1). The stoichiometry and lattice parameter of the resulting oxides can be controlled and predictively modelled, resulting in highly-defective, strain-heavy nanoparticles. The size of the nanocrystals can be tuned from 5 nm to 20 nm, with a large saturation magnetization range (23 to 73 A m2 kg-1), as well as minimal coercivity (~1 kA m-1). Using only air, NaCl, and FeCl2, a biocompatible approach is achieved, besides a remarkable level of control over key parameters, with a view on minimizing the addition of chemicals for enhanced production and applications.

| S-EPMC6814830 | biostudies-literature

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment.

Project description:Electroreduction of carbon dioxide (CO2) over copper-based catalysts provides an attractive approach for sustainable fuel production. While efforts are focused on developing catalytic materials, it is also critical to understand and control the microenvironment around catalytic sites, which can mediate the transport of reaction species and influence reaction pathways. Here, we show that a hydrophobic microenvironment can significantly enhance CO2 gas-diffusion electrolysis. For proof-of-concept, we use commercial copper nanoparticles and disperse hydrophobic polytetrafluoroethylene (PTFE) nanoparticles inside the catalyst layer. Consequently, the PTFE-added electrode achieves a greatly improved activity and Faradaic efficiency for CO2 reduction, with a partial current density >250 mA cm-2 and a single-pass conversion of 14% at moderate potentials, which are around twice that of a regular electrode without added PTFE. The improvement is attributed to a balanced gas/liquid microenvironment that reduces the diffusion layer thickness, accelerates CO2 mass transport, and increases CO2 local concentration for the electrolysis.

| S-EPMC7794506 | biostudies-literature

Introductory Guide to Assembling and Operating Gas Diffusion Electrodes for Electrochemical CO2 Reduction.

Project description: Not available

| S-EPMC6413482 | 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

Probing lung microstructure with hyperpolarized noble gas diffusion MRI: theoretical models and experimental results.

Project description:The introduction of hyperpolarized gases ((3)He and (129)Xe) has opened the door to applications for which gaseous agents are uniquely suited-lung MRI. One of the pulmonary applications, diffusion MRI, relies on measuring Brownian motion of inhaled hyperpolarized gas atoms diffusing in lung airspaces. In this article we provide an overview of the theoretical ideas behind hyperpolarized gas diffusion MRI and the results obtained over the decade-long research. We describe a simple technique based on measuring gas apparent diffusion coefficient (ADC) and an advanced technique, in vivo lung morphometry, that quantifies lung microstructure both in terms of Weibel parameters (acinar airways radii and alveolar depth) and standard metrics (mean linear intercept, surface-to-volume ratio, and alveolar density) that are widely used by lung researchers but were previously available only from invasive lung biopsy. This technique has the ability to provide unique three-dimensional tomographic information on lung microstructure from a less than 15 s MRI scan with results that are in good agreement with direct histological measurements. These safe and sensitive diffusion measurements improve our understanding of lung structure and functioning in health and disease, providing a platform for monitoring the efficacy of therapeutic interventions in clinical trials.

| S-EPMC6366858 | biostudies-literature

Corrosion Resistance of the CpTi G2 Cellular Lattice with TPMS Architecture for Gas Diffusion Electrodes.

Project description:The corrosion of materials used in the design of metal-air batteries may shorten their cycle life. Therefore, metal-based materials with enhanced electrochemical stability have attracted much attention. The purpose of this work was to determine the corrosion resistance of commercially pure titanium Grade 2 (CpTi G2) cellular lattice with the triply periodic minimal surfaces (TPMS) architecture of G80, D80, I-2Y80 in 0.1 M KOH solution saturated with oxygen at 25 °C. To produce CpTi G2 cellular lattices, selective laser melting technology was used which allowed us to obtain 3D cellular lattice structures with a controlled total porosity of 80%. For comparison, the bulk electrode was also investigated. SEM examination and statistical analysis of the surface topography maps of the CpTi G2 cellular lattices with the TPMS architecture revealed much more complex surface morphology compared to the bulk CpTi SLM. Corrosion resistance tests of the obtained materials were conducted using open circuit potential method, Tafel curves, anodic polarization curves, and electrochemical impedance spectroscopy. The highest corrosion resistance and the lowest material consumption per year were revealed for the CpTi G2 cellular lattice with TPMS architecture of G80, which can be proposed as promising material with increased corrosion resistance for gas diffusion in alkaline metal-air batteries.

| S-EPMC7795527 | biostudies-literature

In Situ Regeneration of Copper-Coated Gas Diffusion Electrodes for Electroreduction of CO2 to Ethylene.

Project description:A key challenge for carbon dioxide reduction on Cu-based catalysts is its low faradic efficiency (FE) and selectivity towards higher-value products, e.g., ethylene. The main factor limiting the possibilities of long-term applications of Cu-based gas diffusion electrodes (GDE) is a relatively fast drop in the catalytic activity of copper layers. One of the solutions to the catalyst stability problem may be an in situ reconstruction of the catalyst during the process. It was observed that the addition of a small amount of copper lactate to the electrolyte results in increased Faradaic efficiency for ethylene formation. Moreover, the addition of copper lactate increases the lifetime of the catalytic layer ca. two times and stabilizes the Faradaic efficiency of the electroreduction of CO2 to ethylene at ca. 30%. It can be concluded that in situ deposition of copper through reduction of copper lactate complexes present in the electrolyte provides new, stable, and selective active sites, promoting the reduction of CO2 to ethylene.

| S-EPMC8228262 | biostudies-literature

Tropical tree cover in a heterogeneous environment: A reaction-diffusion model.

Project description:Observed bimodal tree cover distributions at particular environmental conditions and theoretical models indicate that some areas in the tropics can be in either of the alternative stable vegetation states forest or savanna. However, when including spatial interaction in nonspatial differential equation models of a bistable quantity, only the state with the lowest potential energy remains stable. Our recent reaction-diffusion model of Amazonian tree cover confirmed this and was able to reproduce the observed spatial distribution of forest versus savanna satisfactorily when forced by heterogeneous environmental and anthropogenic variables, even though bistability was underestimated. These conclusions were solely based on simulation results for one set of parameters. Here, we perform an analytical and numerical analysis of the model. We derive the Maxwell point (MP) of the homogeneous reaction-diffusion equation without savanna trees as a function of rainfall and human impact and show that the front between forest and nonforest settles at this point as long as savanna tree cover near the front remains sufficiently low. For parameters resulting in higher savanna tree cover near the front, we also find irregular forest-savanna cycles and woodland-savanna bistability, which can both explain the remaining observed bimodality.

| S-EPMC6597153 | biostudies-literature

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