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The mass storage of hydrogen is a challenge considering large industrial applications and continuous distribution, e.g., for domestic use as a future energy carrier that respects the environment. For a long time, molecular hydrogen was stored and distributed, either as a gas (pressurized up to 75 MPa) or as a cryogenic liquid (20.4 K). Furthermore, the atomic storage of hydrogen in the solid-state form via metallic or covalent compounds is still the subject of intense research and limited to a small scale for some practical developments. In addition, other type H chemical storage routes are being tested, such as ammonia and LOHC (Liquid Organic Hydrogen Carrier), etc. In any case, the main constraint remains security. However, Hydrogen Solid State Storage (HSSS) using MgH2 bodies has been shown to be feasible in terms of process and safety. Furthermore, its intrinsic volumetric densification was proven to be much better performing with 106:70:45 kgH2/m3 for solid (RT):LH (20.4 K):gas (75 MPa), respectively. Very early on, fairly reactive MgH2-based pellets were produced (for max. ~27 tons/year) at McPhy Energy using a series of unique and self-built installations. Thus, the design of large instrumented reservoirs was undertaken thanks to fundamental research first carried out at the CNRS. So, prototypes of storage units from 100 to ~5500 kWh have been produced. However, McPhy took other routes a few years ago (smelting and refueling stations) because the HSSS market was not merging at that time. Today, a new operator, Jomi–Leman, therefore, decided to try the challenge again focusing on applications with on-site production and mass HSSS.

Fast forging of compacts made up of Mg and Ni powders is shown to be an effective method to induce severe plastic deformation with improved H2 sorption properties. Here, using such processed samples, a comprehensive analysis of the sorption properties reveals that the first hydrogenation sequence significantly depends on the forging temperature, through different microstructures. More in detail, no phase transformation occurs upon cold forging, while solid-state reaction leads to the formation of the Mg2Ni intermetallic compound upon forging above 400 °C. Forging below the brittle-to-ductile transition (225–250 °C) leads to faster H2 uptake upon first absorption owing to a more textured fiber along the c-axis and internal strains which promote hydrogen diffusion through the bulk material. Desorption kinetics remain slower with low-temperature forging, despite Ni recombining to form Mg2Ni during the first desorption. After several cycles, a two-step behavior is observed with a fast absorption step occurring up to about 3 wt.%. Despite this limited uptake performance, the forging process can be considered as a straightforward, safe, and cost-efficient process to produce large amounts of Mg-based alloys for hydrogen storage. In particular, such severe plastic deformation processes can be considered as reliable substitutes for ball-milling, which is highly efficient but energy- and time-consuming.

Both numerical simulation and hardness measurements were used to determine the mechanical and microstructural behavior of AZ31 bulk samples when submitted to the Equal Channel Angular Pressing (ECAP) technique. Billets of this representative of Mg-rich alloys were submitted to different numbers of passes for various ECAP modes (anisotropic A, isotropic BC). The strain distribution, the grain size refinement, and the micro-hardness were used as indicators to quantify the effectiveness of the different processing routes. Structural characterizations at different scales were achieved using Scanning Electron Microscopy (SEM), micro-analysis, metallography, Small Angle Neutron Scattering SANS, X-Ray Diffraction (XRD), and texture determination. The grain and crystallite size distribution and orientation as well as defect impacts were determined. Anelastic Spectroscopy (AS) on mechanically deformed samples have shown that the temperature of ECAP differentiate the fragile to ductile regime. MgH2 consolidated powders were checked for using AS to detect potential hydrogen motions and interaction with host metal atoms. After further optimization, the different mechanically-treated samples were submitted to hydrogenation/dehydrogenation (H/D) cycles, which shows that, for a few passes, the BC mode is better than the A one, as supported by theoretical and experimental microstructure analyses. Accordingly, the hydrogen uptake and (H/D) reactions were correlated with the optimized microstructure peculiarities and interpreted in terms of Johnson-Avrami- Mehl-Kolmogorov (JAMK) and Jander models, successively.

Magnetic and magnetocaloric effect (MCE) of the Er(Fe0.8−xMn0.2−yCox+y)2 Laves phase-type compounds have been investigated. X-ray diffraction (XRD) analysis has revealed that these compounds crystallize with the C15 type Laves phase structure (Space Group Fd-3m). The magnetization curves indicate a ferri-magnetic-ordering resulting of the antiparallel coupling between the moments of the heavy rare earth Er and the transition metal (TM). The partial substitution of Fe/Mn by Co increases the Curie temperature from 355 K for Er(Fe0.8Mn0.2)2 to 475, 550, and 555 K for Er(Fe0.7Mn0.2Co0.1)2, Er(Fe0.8Mn0.1Co0.1)2, and Er(Fe0.7Mn0.1Co0.2)2, respectively. According to the nature of the TM elements, arguments were presented forwards either Molecular Field or Spin Fluctuation Theory, even Stoner type pictures should be considered for. MCE was calculated according to the Maxwell relation based on isotherm magnetization measurements. The magnetic entropy change (−∆SM) observed on a 300–400 K temperature range can be understood in terms of a Spin Fluctuation Theory picture supported by both the different magnetic polarization levels that were shared by the TM elements and the related interatomic exchange forces.

An alternative route for metal hydrogenation has been investigated: cold plasma hydrogen implantation on polyol-made transition metal nanoparticles. This treatment applied to a challenging system, Ni–H, induces a re-ordering of the metal lattice, and superstructure lines have been observed by both Bragg–Brentano and grazing incidence X-ray diffraction. The resulting intermetallic structure is similar to those obtained by very high-pressure hydrogenation of nickel and prompt us to suggest that plasma-based hydrogen implantation in nanometals is likely to generate unusual metal hydride, opening new opportunities in chemisorption hydrogen storage. Typically, almost isotropic in shape and about 30 nm sized hexagonal-packed Ni2H single crystals were produced starting from similarly sized cubic face-centred Ni polycrystals.

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Hydrogen storage in metal hydride tanks (MHT) is a very promising solution. Several experimental tanks, studied by different teams, have already proved the feasibility and the interesting performances of this solution. However, in much cases, an optimization of tank geometry is still needed in order to perform fast hydrogen loading. The development of efficient numerical tools is a key issue for MHT design and optimization. We propose a simple model representing a metal hydride tank exchanging its heat of reaction with a thermal fluid flow. In this model, the radial and axial discretisations have been decoupled by using Matlab® one-dimensional tools. Calculations are compared to experimental results obtained in a previous study. A good agreement is found for the loading case. The discharging case shows some discrepancies, which are discussed in this paper.

The series of Mn2−xFexP1−ySiy types of compounds form one of the most promising families of magnetocaloric materials in term of performances and availability of the elemental components. Potential for large scale application needs to optimize the synthesis process, and an easy and rather fast process here described is based on the use of two main type of precursors, providing the Fe-P and Mn-Si proportions. The series of Mn2−xFexP1−ySiy compounds were synthesized and carefully investigated for their crystal structure versus temperature and compared interestingly with earlier results. A strong magnetoelastic effect accompanying the 1st order magnetic transition—as well as the parent phosphide–arsenides—was related to the relative stability of both the Fe magnetic polarization and the Fe–Fe exchange couplings. In order to better understand this effect, we propose a local distortion index of the non-metal tetrahedron hosting Fe atoms. Besides, from Mn-rich (Si-rich) to Fe-rich (P-rich) compositions, it is shown that the magnetocaloric phenomenon can be established on demand below and above room temperature. Excellent performance compounds were realized in terms of magnetic entropy ΔSm and adiabatic temperature ΔTad variations. Since from literature it was seen that the magnetic performances are very sensitive to the synthesis process, correspondingly here a new effective process is proposed. Mössbauer spectroscopy analysis was performed on Mn-rich, equi-atomic Mn-Fe, and Fe-rich compounds, allowing determination of the distribution of hyperfine fields setting on Fe in the tetrahedral and pyramidal sites, respectively. Electronic structure calculations confirmed the scheme of metal and non-metal preferential ordering, respectively. Moreover, the local magnetic moments were derived, in fair agreement with both the experimental magnetization and the Fe contributions, as determined by Mössbauer spectroscopy.

The mass storage of hydrogen is a challenge considering large industrial applications and continuous distribution, e.g., for domestic use as a future energy carrier that respects the environment. For a long time, molecular hydrogen was stored and distributed, either as a gas (pressurized up to 75 MPa) or as a cryogenic liquid (20.4 K). Furthermore, the atomic storage of hydrogen in the solid-state form via metallic or covalent compounds is still the subject of intense research and limited to a small scale for some practical developments. In addition, other type H chemical storage routes are being tested, such as ammonia and LOHC (Liquid Organic Hydrogen Carrier), etc. In any case, the main constraint remains security. However, Hydrogen Solid State Storage (HSSS) using MgH[sub.2] bodies has been shown to be feasible in terms of process and safety. Furthermore, its intrinsic volumetric densification was proven to be much better performing with 106:70:45 kgH[sub.2]/m[sup.3] for solid (RT):LH (20.4 K):gas (75 MPa), respectively. Very early on, fairly reactive MgH[sub.2]-based pellets were produced (for max. ~27 tons/year) at McPhy Energy using a series of unique and self-built installations. Thus, the design of large instrumented reservoirs was undertaken thanks to fundamental research first carried out at the CNRS. So, prototypes of storage units from 100 to ~5500 kWh have been produced. However, McPhy took other routes a few years ago (smelting and refueling stations) because the HSSS market was not merging at that time. Today, a new operator, Jomi–Leman, therefore, decided to try the challenge again focusing on applications with on-site production and mass HSSS.