Chasing quantitative biases in neutron imaging with scintillator-camera detectors: a practical method with black body grids.

We propose a method for improving the quantification of neutron imaging measurements with scintillator-camera based detectors by correcting for systematic biases introduced by scattered neutrons and other sources such as light reflections in the detector system. This method is fully experimental, using reference measurements with a grid of small black bodies (BB) to measure the bias contributions directly. Using two test samples, one made of lead alloy and having a moderate (20%) neutron transmission and one made of stainless-steel and having a very low (1%) transmission, we evaluated the improvement brought by this method in reducing both the average quantification bias and the uncertainty around this average bias after tomographic reconstruction. The results show that a reduction of the quantification bias of up to one order of magnitude can be obtained. For moderately transparent samples, little sensitivity is observed to the parameters used for the correction. For the more challenging sample with very low transmission, a correct placement of the BB grid is of utmost importance for a successful correction.

On the needle clogging of staked-in-needle pre-filled syringes: Mechanism of liquid entering the needle and solidification process.

Staked-in-needle prefilled syringes (SIN-PFS) are widely used for the parenteral administration of drug product solutions. During stability studies, clogging of the injection needle was observed in syringes filled with concentrated antibody solution. A prerequisite for this phenomenon is that liquid has entered the needle. In this study, we characterized the mechanism causing the entry and movement of liquid in the needle using neutron imaging without manipulating the container closure integrity of the syringe. The gas pressure difference between inside and outside of the syringe was identified as the major cause of liquid movement. The influence of external factors, such as temperature fluctuation and physical pressure on the stopper, were tested and were confirmed to have a relevant impact on the processes of liquid entering and moving inside the injection needle. In a second step, the solidification process of the liquid segments inside the needle via solvent evaporation was further investigated, and the process was found to be dependent on storage time, environmental climate and interaction between the drug product solution and the needle surface. The presence of air/liquid segments was identified as a further factor for the stochastic behavior of needle clogging. For the first time, this fundamental mechanism behind the needle clogging issue was investigated in depth and the results will help to reduce the defect rate for clogged SIN-PFS products.

A Monte Carlo approach for scattering correction towards quantitative neutron imaging of polycrystals.

The development of neutron imaging from a qualitative inspection tool towards a quantitative technique in materials science has increased the requirements for accuracy significantly. Quantifying the thickness or the density of polycrystalline samples with high accuracy using neutron imaging has two main problems: (i) the scattering from the sample creates artefacts on the image and (ii) there is a lack of specific reference attenuation coefficients. This work presents experimental and simulation results to explain and approach these problems. Firstly, a series of neutron radiography and tomography experiments of iron, copper and vanadium are performed and serve as a reference. These materials were selected because they attenuate neutrons mainly through coherent (Fe and Cu) and incoherent (V) scattering. Secondly, an ad hoc Monte Carlo model was developed, based on beamline, sample and detector parameters, in order to simulate experiments, understand the physics involved and interpret the experimental data. The model, developed in the McStas framework, uses a priori information about the sample geometry and crystalline structure, as well as beamline settings, such as spectrum, geometry and detector type. The validity of the simulations is then verified with experimental results for the two problems that motivated this work: (i) the scattering distribution in transmission imaging and (ii) the calculated attenuation coefficients.

Water distribution in a sorption enhanced methanation reactor by time resolved neutron imaging.

Water adsorption enhanced catalysis has been recently shown to greatly increase the conversion yield of CO2 methanation. However, the joint catalysis and adsorption process requires new reactor concepts. We measured the spatial water distribution in a model fixed bed reactor using time resolved neutron imaging. Due to the high neutron attenuation coefficient of hydrogen, the absorbed water in the sorption catalyst gives a high contrast allowing us to follow its formation and map its distribution. At the same time, the product gas was analysed by FTIR-gas analysis. The measurements provided crucial insights into the future design of sorption reactors: during the sorption enhanced reaction, a reaction front runs through the reactor. Once the extension of the reaction front reaches the exhaust, the conversion rate of sorption enhanced methanation decreases. The existence of a reaction front running through the reactor is prerequisite for a high conversion rate. We give a simple model of the experimental results, in particular the conditions, under which a reaction front is established. In particular the latter effect must be taken into account for the dimensions of a large scale reactor.

Dual spectrum neutron radiography: identification of phase transitions between frozen and liquid water.

In this Letter, a new approach to distinguish liquid water and ice based on dual spectrum neutron radiography is presented. The distinction is based on arising differences between the cross section of water and ice in the cold energy range. As a significant portion of the energy spectrum of the ICON beam line at Paul Scherrer Institut is in the thermal energy range, no differences can be observed with the entire beam. Introducing a polycrystalline neutron filter (beryllium) inside the beam, neutrons above its cutoff energy are filtered out and the cold energy region is emphasized. Finally, a contrast of about 1.6% is obtained with our imaging setup between liquid water and ice. Based on this measurement concept, the temporal evolution of the aggregate state of water can be investigated without any prior knowledge of its thickness. Using this technique, we could unambiguously prove the production of supercooled water inside fuel cells with a direct measurement method.

Using 2H labeling with neutron radiography for the study of solid polymer electrolyte water transport properties.

A method combining (2)H labeling of different sources of H atoms (hydrogen, water vapor) with neutron imaging for the analysis of transport parameters in the bulk and at the interfaces of Nafion polymer electrolyte membranes is proposed. The use of different isotope compositions in the steady state allows evaluation of the relation between bulk and interface transport parameters, but relies on literature data for evaluating absolute values. By using transients of isotope composition, absolute values of these parameters including the self-diffusion coefficient of H can be extracted, making this method an attractive alternative to self-diffusion measurements using nuclear magnetic resonance (NMR), allowing measurements in precisely controlled conditions in real fuel cell structures. First measurements were realized on samples with and without electrodes and we report values of the self-diffusion coefficient of the same order of magnitude as values measured using NMR, although with slightly higher numbers. In our particular case, lower interfacial exchange rates for water transport were observed for samples with an electrode.