The present study showcases the importance of temperature and potential window for evaluation of Pt-based supported electrocatalyst stability. A platinum based commercial material with an average size of Pt nanoparticles between 2-3 nm (Pt/C) and its thermally annealed analogue with an average particle size of ∼5 nm (Pt/C-HT) are considered. X-ray diffraction (XRD), ex situ transmission electron microscopy (TEM) imaging and thin film rotating disc electrode (TF-RDE) along with proprietary hightemperature disc electrode (HT-DE) are used for electrocatalysts inspection. The study shows a clear dependence between the electrochemical surface area (ECSA) loss and the temperature increase during the potentiodynamic accelerated degradation test (ADT). Additionally it is demonstrated that selection of the lower and upper potential limits in ADT protocol plays an important role in ECSA loss. Comparing various results obtained on Pt/C and Pt/C-HT, we show that varying ADT conditions of temperature and different potential windows is crucial for adequate evaluation and stability interpretation of potentially promising novel electrocatalysts and that relatively mild ADT conditions (i.e. 0.4-1.0 V RHE , RT) can be potentially misleading.
We present a model and web-based tool for rapid and efficient prediction and rationalization of chemical membrane degradation in PEMFCs including protection mechanisms.
An exact solution is presented for the time-dependent wavefunction of a
Kramers doublet which propagates around a quantum ring with tuneable Rashba
spin-orbit interaction. By propagating in segments it is shown that
Kramers-doublet qubits may be defined for which transformations on the Bloch
sphere may be performed for an integral number of revolutions around the ring.
The conditions for full coverage of the Bloch sphere are determined and
explained in terms of sequential qubit rotations due to electron motion along
the segments, with change of rotation axes between segments due to adiabatic
changes in the Rashba spin-orbit interaction. Prospects and challenges for
possible realizations are discussed for which rings based on InAs quantum wires
are promising candidates
The degradation of the catalyst layer represents one of the main limiting factors in a wider adoption of fuel cells. The identification of the contributions of different mechanisms of catalyst degradation, namely the Ostwald ripening and particle agglomeration, is an important step in the development of mitigation strategies for increasing fuel cell reliability and prolonging its life time.
In this paper, the degradation phenomena in high temperature polymer electrolyte membrane fuel cell (HT‐PEMFC) are analyzed using a physically‐based model of fuel cell operation and catalyst degradation, describing carbon corrosion, platinum dissolution and consequent growth of catalyst particles. The model results indicate significantly different time dependence of catalyst particle growth resulting from different mechanisms: linear growth in the case of particle agglomeration and root‐like time dependence for the Ostwald ripening.
Based on these results, a new analytic method is proposed, performed by the fitting of a test root‐function to the time profile of the particle size growth and using best‐fit parameters to identify the prevailing growth mechanism. Using this method on a particle growth time trace deduced from in situ cyclic voltammetry measurement during HT‐PEMFC degradation, we are able to identify the agglomeration as the main mechanism of catalyst particle grow.
The limited durability of hydrogen fuel cells is one of the main obstacles in their wider adoption as a clean alternative technology for small scale electricity production. The Ostwald ripening of catalyst material is recognized as one of the main unavoidable degradation processes deteriorating the fuel cell performance and shortening its lifetime. The paper systematically studies how the modeling approach towards the electrochemically driven Ostwald ripening in the fuel cell catalyst differs from the classical diffusion driven models and highlights how these differences affect the resulting evolution of particle size distribution. At moderately low electric potential, root-law growth of mean particle size is observed with linear relation between mean particle size and standard deviation of particle size distribution, similar to Lifshitz-Slyozov-Wagner theory, but with broader and less skewed distribution. In case of high electric potential, rapid particle growth regime is observed and qualitatively described by redeposition of platinum from a highly oversaturated solution, revealing the deficiencies of the existing platinum degradation models at describing the Ostwald ripening in the fuel cells at high electric potentials. Several improvements to the established models of platinum degradation in fuel cell catalysts are proposed, aimed at better description of the diffusion processes involved in particle growth due to Ostwald ripening.
An exact solution for single electron states on mezoscopic rings with the Rashba coupling and in the presence of external magnetic and electric fields is derived by means of a unitary transformation. The transformation maps the model to a bare ring, which gives the possibility of a very simple formulation of single or many electron problems. As an example some exact results for spin and energy levels are presented.
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