Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userNafion-induced reduction of manganese and its impact on the electrocatalytic properties of a highly active MnFeNi oxide for bifunctional oxygen conversion
79
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
Electrocatalysts for bifunctional oxygen reduction (ORR) and oxygen evolution reaction (OER) are commonly studied under hydrodynamic conditions, rendering the use of binders necessary to ensure the mechanical stability of the electrode films. The presence of a binder, however, may influence the properties of the materials under examination to an unknown extent. Herein, we investigate the impact of Nafion on a highly active ORR/OER catalyst consisting of MnFeNi oxide nanoparticles supported on multi-walled carbon nanotubes. Electrochemical studies revealed that, in addition to enhancing the mechanical stability and particle connectivity, Nafion poses a major impact on the ORR selectivity, which correlates with a decrease in the valence state of Mn according to X-ray absorption spectroscopy. These findings call for awareness regarding the use of electrode additives, since in some cases the extent of their impact on the properties of electrode films cannot be regarded as negligible.
rate research
Read More
Active, selective and stable catalysts are imperative for sustainable energy conversion, and engineering materials with such properties are highly desired. High-entropy alloys (HEAs) offer a vast compositional space for tuning such properties. Too vast, however, to traverse without the proper tools. Here, we report the use of Bayesian optimization on a model based on density functional theory (DFT) to predict the most active compositions for the electrochemical oxygen reduction reaction (ORR) with the least possible number of sampled compositions for the two HEAs Ag-Ir-Pd-Pt-Ru and Ir-Pd-Pt-Rh-Ru. The discovered optima are then scrutinized with DFT and subjected to experimental validation where optimal catalytic activities are verified for Ag-Pd, Ir-Pt, and Pd-Ru binary systems. This study offers insight into the number of experiments needed for exploring the vast compositional space of multimetallic alloys which has been determined to be on the order of 50 for ORR on these HEAs.
The four-electron oxygen reduction reaction on Pt catalyst in alkaline solution undergoes proton transfer via tunneling mechanism. The hydrogen/deuterium kinetic isotopic rate constant ratio (kH/kD ) = 32 in a low overpotential region, indicating the importance of the quantum-proton-tunneling at the rate-determining step (RDS). However, kH/kD goes down to 3 in a high overpotential region, suggesting the classical proton-transfer (PT) scheme. Therefore, there is a quantum-to-classical transition of PT process as a function of potential, which is confirmed by theoretical study.
Graphene oxide can be used as a precursor to graphene but the quality of graphene flakes is highly heterogeneous. Scanning-Raman-Microscopy (SRM) is used to characterize films of graphene derived from flakes of graphene oxide with an almost intact carbon framework (ai-GO). The defect density of these flakes is visualized in detail by analyzing the intensity and full-width at half-maximum of the most pronounced Raman peaks. In addition, we superimpose the SRM results with AFM images and correlate the spectroscopic results with the morphology. Furthermore, we use SRM technique to display the amount of defects in a film of graphene. Thus, an area of 250 x 250 {my}m2 of graphene is probed with a step-size increment of 1 {mu}m. We are able to visualize the position of graphene flakes, edges and the substrate. Finally, we alter parameters of measurement to analyze the quality of graphene fast and reliable. The described method can be used to probe and visualize the quality of graphene films.
MXenes with versatile chemistry and superior electrical conductivity are prevalent candidate materials for energy storage and catalysts. Inspired by recent experiments of hybridizing MXenes with carbon materials, here we theoretically design a series of heterostructures of N-doped graphene supported by MXene monolayers as bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Our first-principles calculations show that the graphitic sheet on V2C and Mo2C MXenes are highly active with an ORR overpotential down to 0.36 V and reaction free energies for the HER approaching zero, both with low kinetic barriers. Such outstanding catalytic activities originate from the electronic coupling between the graphitic sheet and the MXene, and can be correlated with the pz band center of surface carbon atoms and the work function of the heterostructures. Our findings screen a novel form of highly active electrocatalysts by taking advantage of the fast charge transfer kinetics and strong interfacial coupling of MXenes, and illuminate a universal mechanism for modulating the catalytic properties of two-dimensional hybrid materials.
Controlled organic functionalization of silicon surfaces as integral part of semiconductor technology offers new perspectives for a wide range of applications. The high reactivity of the silicon dangling bonds, however, presents a major hindrance for the first basic reaction step of such a functionalization, i.e., the chemoselective attachment of bifunctional organic molecules on the pristine silicon surface. We overcome this problem by employing cyclooctyne as the major building block of our strategy. Functionalized cyclooctynes are shown to react on Si(001) selectively via the strained cyclooctyne triple bond while leaving the side groups intact. The achieved selectivity originates from the distinctly different adsorption dynamics of the separate functionalities: A direct adsorption pathway is demonstrated for cyclooctyne as opposed to the vast majority of other organic functional groups. The latter ones react on Si(001) via a metastable intermediate which makes them effectively unreactive in competition with the direct pathway of cyclooctynes strained triple bond.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
