Magnetocaloric cooling offers the potential to improve the efficiency of refrigeration devices and hence cut the significant CO2 emissions associated with cooling processes. A critical issue in deployment of this technology is the mechanical degradation of the magnetocaloric material during processing and operation, leading to limited service-life. The mechanical properties of hydrogenated La(Fe,Mn,Si)13-based magnetocaloric material are studied using macroscale bending tests of polycrystalline specimens and in situ micropillar compression tests of single crystal specimens. The impact of hydrogenation on the mechanical properties are quantified. Understanding of the deformation/failure mechanisms is aided by characterization with transmission electron microscopy and atom probe tomography to reveal the arrangement of hydrogen atoms in the crystal lattice. Results indicate that the intrinsic strength of this material is ~3-6 GPa and is dependent on the crystal orientation. Single crystals under compressive load exhibit shearing along specific crystallographic planes. Hydrogen deteriorates the strength of La(Fe,Mn,Si)13 through promotion of transgranular fracture. The weakening effect of hydrogen on single crystals is anisotropic; it is significant upon shearing parallel to the {111} crystallographic planes but is negligible when the shear plane is {001}-oriented. APT analysis suggests that this is associated with the close arrangement of hydrogen atoms on {222} planes.
The processing of promising magnetocaloric materials into spheres is one of the important issues on developing high-performance magnetic refrigeration systems. In the present study, we achieved in producing spherical particles of a giant magnetocaloric compound HoB2 by a crucible-free gas atomization process, despite its high melting point of 2350 C. The particle size distribution ranges from 100 to 710 micrometers centered at 212-355 micrometers with the highest yield of 14-20wt% of total melted electrode, which is suitable for magnetic refrigeration systems. The majority of the resulting par…
We are witnessing a great transition towards a society powered by renewable energies to meet the ever-stringent climate target. Hydrogen, as an energy carrier, will play a key role in building a climate-neutral society. Although liquid hydrogen is essential for hydrogen storage and transportation, liquefying hydrogen is costly with the conventional methods based on Joule-Thomas effect. As an emerging technology which is potentially more efficient, magnetocaloric hydrogen liquefaction is a "game-changer". In this work, we have investigated the rare-earth-based Laves phases ${\rm R}Al_2$ and ${\…
We report on the impact of magnetoelastic coupling on the magnetocaloric properties of LaFe$_{11.4}$Si$_{1.6}$H$_{1.6}$ in terms of the vibrational density of states, which we determined with $^{57}$Fe nuclear resonant inelastic X-ray scattering measurements and with density-functional-theory based first-principles calculations in the ferromagnetic low-temperature and paramagnetic high-temperature phase. In experiments and calculations, we observe pronounced differences in the shape of the Fe-partial VDOS between non-hydrogenated and hydrogenated samples. This shows that hydrogen does not only…
National Institute for Materials Science（国立材料科学研究所）；University of Tsukuba（筑波大学）；Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences（中国科学院福建物质结构研究所）
Magnetic refrigeration exploits the magnetocaloric effect which is the entropy change upon application and removal of magnetic fields in materials, providing an alternate path for refrigeration other than the conventional gas cycles. While intensive research has uncovered a vast number of magnetic materials which exhibits large magnetocaloric effect, these properties for a large number of compounds still remain unknown. To explore new functional materials in this unknown space, machine learning is used as a guide for selecting materials which could exhibit large magnetocaloric effect. By this …
Processing magnetocaloric materials into magnetic refrigerant particles is an essential issue in developing high-performance magnetic refrigerators. Here, we succeed in stably producing magnetocaloric particles of the promising material HoAl2 by a newly devised method based on electrode induction melting gas atomization process. The particle size range is on the order of submillimeter, which is suitable for practical refrigeration systems. The resulting particles with less contamination have good morphological, magnetic, and magnetocaloric properties: (i) almost spherical shapes with few inter…
Two-dimensional magnets could potentially revolutionize information technology, but their potential application to cooling technology and magnetocaloric effect (MCE) in a material down to the monolayer limit remain unexplored. Herein, we reveal through multiscale calculations the existence of giant MCE and its strain tunability in monolayer magnets such as CrX$_3$ (X=F, Cl, Br, I), CrAX (A=O, S, Se; X=F, Cl, Br, I), and Fe$_3$GeTe$_2$. The maximum adiabatic temperature change ($ΔT_\text{ad}^\text{max}$), maximum isothermal magnetic entropy change, and specific cooling power in monolayer CrF$_3…
Hydrogen enhanced cracking is one of the many failure mechanisms in metals depending on the corrosive environment. In the presented work, a multiscale constitutive model has been presented for hydrogen enhanced intergranular cracking in metals. The proposed constitutive model takes into account one of the many micromechanisms, i.e. Slip based micromechanisms active in the grain interior using crystal plasticity theory while sensitized grain boundary zone has been modelled by proposing a phenomenological constitutive model motivated from cohesive zone modelling approach. Model has been assessed…
Recently, a massive magnetocaloric effect near the liquefaction temperature of hydrogen has been reported in the ferromagnetic material HoB$_{2}$. Here we investigate the effects of Dy substitution in the magnetocaloric properties of Ho$_{1-x}$Dy$_{x}$B$_{2}$ alloys ($\textit{x}$ = 0, 0.3, 0.5, 0.7, 1.0). We find that the Curie temperature ($\textit{T}$$_{C}$) gradually increases upon Dy substitution, while the magnitude of the magnetic entropy change |$Δ\textit{S}_{M}$| at $\textit{T}$ = $\textit{T}_{C}$ decreases from 0.35 to 0.15 J cm$^{-3}$ K$^{-1}$ for a field change of 5 T. Due to the pr…
La(Fe,Mn,Si)13 alloys are a promising material family for magnetic refrigeration. Challenges associated with their structural integrity during device assembly and operation requires deep understanding of the mechanical properties. Here we developed a workflow to quantitatively study the fracture properties of La(Fe,Mn,Si)13 plates used in magnetic cooling devices. We employed microstructural characterisation, optical examination of defects, and four-point bending tests of samples with known defect sizes to evaluate their mechanical performance. We established the residual strength curve which …
Solid state-refrigerants have generated worldwide interest owing to their growing potential for use in efficient and green cooling devices. Caloric effects could be obtained by manipulating their degrees of freedom such as magnetization, electric polarization and volume using a variable external field. In conventional magnetocaloric refrigeration systems, the magnetocaloric effect is exploited by moving the active material in and out of the magnetic field source. Here we demonstrate that a giant and reversible magnetocaloric effect can be generated simply by rotating the multiferroic TbMn2O5 s…
It is known that the Zircon-type orthovanadates RVO4 show promise in many different applications as catalysts and optical materials. In this work, we demonstrate that the TbVO4 compound can be also used as magnetic refrigerant in efficient and ecofriendly cryocoolers due to its strong magnetocaloric effect at low temperature regime. The application of a relatively low magnetic field of 2 T along the easy magnetization axis (a) gives rise to a maximum entropy change of about 20 J/kg K at 4 K. More interestingly, under sufficiently high magnetic fields, the isothermal entropy change -ΔST remains…
This short paper presents the potential of using machine learning to predict materials behaviour in the context of hydrogen interaction with steel. Effort has been made to understand the quality, and amount of data needed to get improved predictions. An approach known as physics informed machine learning has been adapted in a simplified way through data classification to show the improvement in predictions. Proposed model eliminates the requirement to solve complex materials constitutive models and can work for any length scale, in the present case it is used for single crystalline steel inter…
Based on the in-detail tracking of the movements of atoms in a large number of molecular dynamics simulation boxes, we find that the diffusion of H and He atoms in single-crystal W is composed of non-Markovian jumps. The waiting time distribution of the triggering of jumps is not the usually recognized exponential distribution, but a temperature-dependent power-law distribution. The power-law distribution of the waiting time may lead to clear ergodicity-breaking diffusion, a phenomenon that has formerly been reported to only occur in complex systems such as living biological cells or soft matt…
Building a physics-aware AI ecosystem for solid-state hydrogen storage materials
Tohoku University（东北大学）；National University of Singapore（新加坡国立大学）；University at Buffalo（布法罗纽约州立大学）；The University of Tokyo（东京大学）；Washington University in St. Louis（华盛顿大学圣路易斯分校）；Utrecht University（乌得勒支大学）；University of Turin（都灵大学）
Spin-orbit interaction is an important vehicle for spin relaxation. At finite temperature lattice vibrations modulate the spin-orbit interaction and thus generate a mechanism for spin-phonon coupling, which needs to be incorporated in any quantitative analysis of spin transport. Starting from a density functional theory \textit{ab initio} electronic structure, we calculate spin-phonon matrix elements over the basis of maximally localized Wannier functions. Such coupling terms form an effective Hamiltonian to be used to extract thermodynamic quantities, within a multiscale approach particularly…
