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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 can be a “game-changer”. In this work, we have investigated the rare-earth-based Laves phases RAl and RNi2 for magnetocaloric hydrogen liquefaction. We have noticed an unaddressed feature that the magnetocaloric effect of second-order magnetocaloric materials can become “giant” near the hydrogen boiling point. This feature indicates strong correlations, down to the boiling point of hydrogen, among the three important quantities of the magnetocaloric effect: the maximum magnetic entropy change ΔSmaxm, the maximum adiabatic temperature change ΔTmaxad , and the Curie temperature TC. Via a comprehensive literature review, we interpret the correlations for a rare-earth intermetallic series as two trends: (1) ΔSmaxm increases with decreasing TC; (2) ΔTmaxad decreases near room temperature with decreasing TC but increases at cryogenic temperatures. Moreover, we have developed a mean-field approach to describe these two trends theoretically. The dependence of ΔSmaxm and ΔTmaxad on TC revealed in this work helps researchers quickly anticipate the magnetocaloric performance of rare-earth-based compounds, guiding material design and accelerating the discoveries of magnetocaloric materials for hydrogen liquefaction.

Hydrogen has the largest gravimetric energy density among all chemical fuels. At the same time, the density of gaseous ${\mathrm{H}}_{2}$ is extremely low, which makes its compression to high pressures, liquefaction, or solid-state storage necessary for transport purposes. Liquid hydrogen ($\mathrm{L}{\mathrm{H}}_{2}$) can be transported in a dewar under atmospheric pressure, but this requires energy-intensive cooling down to $20\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. Magnetocaloric materials have great potential to revolutionize gas liquefaction to make $\mathrm{L}{\mathrm{H}}_{2}$ more competitive as fuel. In this paper, we investigate a series of Laves-phase materials regarding their structural, magnetic, and magnetocaloric properties in high magnetic fields. The three compounds $\mathrm{Ho}{\mathrm{Al}}_{2}$, ${\mathrm{Ho}}_{0.5}{\mathrm{Dy}}_{0.5}{\mathrm{Al}}_{2}$, and $\mathrm{Dy}{\mathrm{Al}}_{2}$ are suited for building a stack for cooling from liquid-nitrogen temperature ($77\phantom{\rule{0.16em}{0ex}}\mathrm{K}$) down to the boiling point of hydrogen at $20\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. This is evident from our direct measurements of the adiabatic temperature change in pulsed magnetic fields, which we compare with calorimetric data measured in a static field. With this methodology, we are now able to study the suitability of magnetocaloric materials down to low temperatures up to the highest magnetic fields of 50 T.

The multicaloric effect is described by a temperature or entropy change of a material triggered by external stimuli applied or removed simultaneously or sequentially. The prerequisite for this is a material exhibiting multiple ferroic states. However, direct measurements of the effect are rarely reported. Now, for this reason, we built a measurement device allowing to determine the adiabatic temperature change in pulsed magnetic fields and, simultaneously, under the influence of a uniaxial load. We selected the all-𝑑-metal Heusler alloy Ni-Mn-Ti-Co for our first test because of its enhanced mechanical properties and enormous magneto- and elastocaloric effects. Ni-Mn-Ti-Co was exposed to pulsed magnetic fields up to 10 T and uniaxial stresses up to 80 MPa, and the corresponding adiabatic temperature changes were measured. With our new experimental tool, we are able to better understand multicaloric materials and determine their cross-coupling responses to different stimuli.

Natural gas is useful for the transition from traditional fossil fuels to renewable energies. The consumption of liquid natural gas has been rising, and the demand is predicted to double by 2040. In this context, magnetocaloric gas liquefaction, as an emerging and energy-saving technology, could be an alternative to the traditional gas-compression refrigeration. In this work, we report a large magnetic entropy change of 7.42 J/kg K under a magnetic field change of 2 T in Nd2In at 109 K, which is near the boiling temperature of natural gas of 112 K. The maximum adiabatic temperature change reaches 1.13 K under a magnetic field change of 1.95 T and is fully reversible. The magnetic phase transition is confirmed to be of the first-order type with the negligible thermal hysteresis. Further investigations on the thermal expansion and the magnetostriction reveal that the magnetic transition undergoes two stages with a negligible volume change. The longitudinal strain increases with magnetic fields and then decreases. These interesting properties are useful for the practical design of a magnetocaloric natural gas liquefaction system and for the fundamental understanding of the phase transitions in other RE2In intermetallics.

Natural gases have played a significant role in different sectors of the global economy. Recent analyses have shown that the world's gas consumption doubled over the last three decades; further growth of the gas consumption is predicted, rising to be 23%–28% of the total primary energy demand by 2030. Therefore, liquefaction of natural gases rapidly gains global importance. In this context, magnetic refrigeration emerges as a modern energy-saving technique, which is an alternative to the traditional gas-compression refrigeration. This paper is devoted to the study of the magnetocaloric effect in magnetic fields up to 10 T on a representative of the Laves phase alloys, GdNi2, which is considered as a perspective material for liquefaction of natural gases. For a magnetic field change of 10 T, the magnetic entropy change ΔSm ≈ −17 J/kg K and the adiabatic temperature change ΔTad ≈ 6.8 K was attained around Curie temperature TC = 70 K. The maximal value of the adiabatic temperature change measured directly in pulsed magnetic fields up to 50 T is ΔTad ≈ 15 K.