Font Size: a A A

Uptake and Release of Hydrogen from Palladium

Posted on:2012-07-25Degree:Ph.DType:Thesis
University:Carnegie Mellon UniversityCandidate:Michalak, William DFull Text:PDF
GTID:2451390011457233Subject:Chemistry
Abstract/Summary:PDF Full Text Request
Understanding H2's interactions on the surface and within the subsurface regions of Pd is critical to development of advanced energy technologies for H2 storage and separations, as well as a variety of catalytic processes including (de)hydrogenation reactions. While many of the physical, chemical, and electronic properties of the H2-Pd system are known, the kinetics and thermodynamics during absorption into the bulk, transport back to the Pd surface, and desorption at low temperature remain uncertain. No studies have measured the uptake and release kinetics of H2 over a range of conditions and prepared a model that can predict the experimental results. In this thesis, H2 release kinetics from Pd are measured over a range of exposure pressures and temperatures. To simulate the observed kinetic behaviors, a continuum-based model is extended from other previously published work to include activation barriers for desorption and transport that change with concentration. This addition improves the model's ability to predict the experimental trends. Further analysis of the system is performed with the model to understand what processes are rate-controlling and how they influence H2 release. A variant of the degree of rate control method for transient systems is developed and used to identify the processes that control H2 uptake and release with Pd.;Metal nanoparticles on structured supports are used in many technological applications such as biosensing, energy harvesting, and electronics. In every case, the functions and properties of the metallic nanostructures depend on their composition, structure, size, shape, and spatial distribution. A challenge for using metal nanoparticles in these applications is the inability to create controlled distributions of the particles with well-defined structural properties. In this thesis, a method is shown to create metal nanostructures over a range of particle sizes, shapes, and spatial distributions. The metal structures are created via spinodal dewetting of precursor thin films. A new approach to induce spinodal dewetting is shown, which makes the technique suitable for high-throughput creation and analysis of metal nanostructures. The results are especially promising for future scientific discovery and accelerated optimization for a diversity of technological applications.
Keywords/Search Tags:Uptake and release, Metal
PDF Full Text Request
Related items