arXiv subjects

Z. D. Harris

Publications and source records attributed to Z. D. Harris.

3 recordsLinked to original sources

arXiv2026

High-sensitivity hydrogen gas permeation: system development, sample preparation, and influence of testing variables

There is a need to develop quantitative, high-resolution hydrogen gas (H2) permeation techniques to provide a better understanding of hydrogen-material interactions. This study aims to develop and validate a high-sensitivity H2 permeation system, which is then leveraged to systematically quantify the influence of surface condition and key testing variables (surface oxides, residual gas impurities, pressure, and temperature) on hydrogen permeation. A gas permeation system capable of operating at pressures up to 50 bar and temperatures up to 250 C was developed, incorporating high-sensitivity mass spectrometric detection and controlled surface preparation protocols. Permeation transients were analysed in a model material (annealed pure Fe) to determine hydrogen diffusivity and permeability under systematically varied surface states, oxygen contents, pressures and temperatures. Surface oxides are shown to play a dominant role in controlling hydrogen permeation at room temperature. The presence of oxide layers can severely hinder or completely suppress hydrogen uptake, with measurable permeation requiring oxide removal via pickling and Pd coating on both surfaces, or activation through hydrogen-assisted reduction at elevated temperature. Residual oxygen present prior to hydrogen exposure further reduces permeability by modifying surface boundary conditions, indicating strongly surface-controlled kinetics. Under optimised surface conditions, hydrogen transport follows bulk diffusion-controlled behaviour, with steady-state flux obeying Sieverts' law at 25 C (1-5 bar) and diffusivity and permeability exhibiting Arrhenius behaviour between 25 and 150 C at 5 bar, indicating bulk diffusion-controlled transport. The developed system resolves hydrogen fluxes as low as 1.98x10-9 mol(m2 s) and provides a robust platform for investigating surface, mechanical and environmental effects on H2 permeation.

physics.chem-ph↗

arXiv2025

New insights into hydrogen-assisted intergranular cracking in nickel

We characterize the grain boundary (GB) susceptibility to hydrogen-assisted intergranular cracking in pure nickel as a function of coincident site lattice value ($Σ$-n), over a wide range of hydrogen concentrations (4 to 14 wppm). Cracks on the surface and within the bulk material were identified across the entire gauge region of the specimens. The susceptibility of GBs to crack initiation and propagation was evaluated by separating cracks containing single GB or multiple GBs. A larger loss in fracture strain, a smaller reduction in area, and an increase in the percentage of intergranular fracture indicated a higher degree of embrittlement at elevated hydrogen concentrations. The number of cracks was significantly higher on the surface than in the bulk for the most severe hydrogen charging conditions ($\geq$ 8 wppm), while a similar number was observed for lower concentrations. The propensity for hydrogen-assisted intergranular cracking at different types of GBs on the surface and in the bulk material was consistent, indicating that while cathodic charging can promote surface cracks, it does not significantly impact the GBs relative susceptibility. The $Σ$-3 boundaries were the most resistant to cracking, as evidenced by the considerably lower fraction of these GBs exhibiting intergranular cracking at all hydrogen concentrations considered. This contrasts literature findings for Ni alloys and can be explained by the segregation energies and reductions in the cohesive strength with hydrogen, with less favorable trapping at the $Σ$-3 boundaries. No evidence of plasticity-mediated cracking initiation was observed.

cond-mat.mtrl-sci↗

arXiv2024

TDS Simulator: A MATLAB App to model temperature-programmed hydrogen desorption

We present TDS Simulator, a new software tool aimed at modelling thermal desorption spectroscopy (TDS) experiments. TDS is a widely used technique for quantifying key characteristics of hydrogen-material interactions, such as diffusivity and trapping. However, interpreting the output of TDS experiments is non-trivial and requires appropriate post-processing tools. This work introduces the first software tool capable of simulating TDS curves for arbitrary choices of material parameters and hydrogen trap characteristics, using the primary hydrogen diffusion and trapping models (Oriani, McNabb-Foster). Moreover, TDS Simulator contains a specific functionality for loading experimental TDS data and conducting the inverse calibration of a selected transport model, providing automatic estimates of the density and binding energy of each hydrogen trap type in the material. In its first version, TDS Simulator is provided as a MATLAB App, which is made freely available to the community and provides a simple graphical user interface (GUI) to make use of TDS Simulator straightforward. As reported in the present manuscript, the outputs of TDS Simulator have been extensively validated against literature data. Demonstrations of automatic determination of trap characteristics from experimental data through the optimisation tool are also provided. The present work enables an efficient and straightforward characterisation of hydrogen-material characteristics relevant to multiple applications, from nuclear fusion to the development of hydrogen-compatible materials for the hydrogen economy. TDS Simulator can be downloaded from https://mechmat.web.ox.ac.uk/codes.

cs.CE↗