← Iliya Angelov Radulov Lab Research
Magnetocaloric Materials

Cooling by magnetic field, not gas compression

Solid-state refrigeration built on the magnetocaloric effect (MCE): align magnetic moments with a field and the material heats; remove the field and it cools below where it started. My work develops the alloys, processing routes, and diagnostic tools that turn this effect into usable technology — from room-temperature cooling to hydrogen liquefaction.

+35%energy efficiency vs. vapor-compression cooling
23%efficiency of conventional Joule-Thomson H₂ liquefaction
>60%theoretical efficiency of magnetocaloric H₂ liquefaction
200 KCurie temperature of pure La(Fe,Si)₁₃ — needs tuning to room temp
01

The material system

A central focus of my work is La(Fe,Si)₁₃-based alloys — recognized for their giant magnetocaloric effect, high magnetization, and low cost, which makes them strong candidates for real magnetic refrigeration devices.

The scientific challenge is twofold: tuning the Curie temperature up from the pure compound's ~200 K to near room temperature, and taming the thermal hysteresis that comes with the alloy's first-order phase transition. I've approached both problems through systematic chemical substitution — Mn, Co, Ni, and Cr — and through hydrogenation of the material.

Magnetic refrigeration trades gaseous refrigerants and compressors for a solid alloy and a magnet — quieter, and built on water instead of gas.
02

Why it matters beyond the lab

Liquid hydrogen is central to a carbon-neutral energy system, but making it is inefficient. Conventional Joule-Thomson expansion liquefaction runs at only about 23% efficiency — too costly for large-scale use.

Magnetocaloric liquefaction changes that math: theoretical models put its efficiency above 60%, which is what makes affordable liquid hydrogen production plausible at scale. The catch is materials — this needs alloys with large magnetic entropy and adiabatic temperature change across the 77 K (nitrogen) to 20 K (hydrogen) range, under magnetic fields that are practical to generate commercially.

03

The materials dilemma

Materials selection for magnetocaloric hydrogen liquefaction runs into a hard trade-off between performance and resource criticality.

⬤ High performance

Gd · Tb · Dy · Ho · Er · Tm

Heavy rare-earth intermetallics deliver superior magnetocaloric performance — but these elements are highly critical in terms of resource availability.

◯ High availability

La · Ce · Pr · Nd

Light rare earths are relatively abundant and far less critical — but their alloys generally show weaker magnetocaloric properties.

This performance-versus-criticality trade-off is central to scaling magnetocaloric technology for widespread adoption — and it's the throughline across the contributions below.

04

Key contributions

Faster, better sample processing

Combining induction melting with suction casting shortened the annealing time of La(Fe,Si)₁₃ compounds by an order of magnitude — improving processing efficiency and widening the range of obtainable NaZn₁₃-type structures. This became the foundation for the systematic substitution studies that followed.

Ni substitution: tuning the transition order

Ni addition raises the transition temperature and, more importantly, converts the phase transition from first-order to second-order. DFT calculations showed Ni atoms preferentially occupy 96i sites without materially changing the total magnetic moment — giving a theoretical basis for the experimental result.

Cr substitution: a counterintuitive result

La(Fe,Cr,Si)₁₃ compounds retain both the magnetocaloric response and the first-order character of the transition despite a significant drop in magnetic moment — challenging the assumption that magnetocaloric performance and moment size must track together.

Mn doping: atomic-scale structure

Using XMCD, EXAFS, and DFT together, this work resolved how Mn doping reshapes the local magnetic and geometric structure of La(Fe,Si)₁₃ — atomic-scale insight into a macroscopic property.

A sharper criterion for transition order

Co-developed a quantitative criterion for classifying magnetic phase transition order from the magnetocaloric effect itself — more accurate than the conventional Banerjee criterion, especially for compositions sitting near the critical point where the transition order is ambiguous.

Mastering hysteresis

Co-authored a comprehensive review on reducing thermal and magnetic hysteresis in first-order magnetocaloric materials — one of the main obstacles between lab-grade material and a device that can cycle reliably.

Composites that survive a real device

Most room-temperature magnetocaloric materials are brittle and corrosion-prone — hard to put directly into a cooling machine. I developed polymer-bonded and metal-bonded composites of La(Fe,Mn,Si)₁₃Hₓ for active magnetic regenerators, systematically mapping how powder particle size, adhesive type and concentration, and compaction pressure affect performance — and introduced a low-melting Field's-metal binder to solve the fatigue issues polymer binders suffer from the material's large magnetovolume effect.

Multi-property probing of the transition

Contributed to simultaneous multi-property probing techniques that combine element-specific and macroscopic hysteresis characterization during magneto-structural phase transitions — giving a more complete picture of what happens inside the material as it switches.

Beyond magnetic field: pressure and multicaloric effects

Ongoing work on the pressure dependence of the MCE and on multicaloric effects — stimulating the material with more than one field at once. In FeRh, exploiting thermal hysteresis across multi-stimuli cycles that combine pulsed magnetic fields with uniaxial load points toward devices that need a smaller, cheaper magnetic field to do the same job.

05

The supply-chain stakes

This isn't only a materials-science problem — it sits inside a real geopolitical bottleneck.

China's share of NdFeB production

85–90%

China controls this share of global NdFeB magnet production and dominates midstream rare-earth separation and metal conversion — a critical choke point for Europe and North America.

Rare earth magnet market by 2028

$17.44B

Projected market size, driven by the accelerating shift to electric vehicles, wind power, and other clean-energy technologies.

In response, the European wind industry — with the German Federal Ministry for Economic Affairs and Energy — has set a resilience roadmap targeting 30% of permanent magnets from alternative sources by 2030, rising to 50% by 2035. Research that reduces reliance on critical heavy rare earths, or reduces the field strength a device needs in the first place, feeds directly into that roadmap.

06

Literature

[1]A. Vinod, D. Arvindha Babu, M. Wuppulluri, "A Short Review on the Evolution of Magnetocaloric La(Fe,Si)13 and Its Fabrication through Melt Spinning," ACS Omega, 2024.
[2]V. Paul-Boncour, L. Bessais, "Tuning the Magnetocaloric Properties of the La(Fe,Si)13 Compounds by Chemical Substitution and Light Element Insertion," Magnetochemistry, 7(1), p.13, 2021.
[3]I.A. Radulov, K.P. Skokov, D.Y. Karpenkov, T. Gottschall, O. Gutfleisch, "On the preparation of La(Fe,Mn,Si)13Hx polymer-composites with optimized magnetocaloric properties," J. Magn. Magn. Mater., 396, 228–236, 2015.
[4]T. Gottschall, K.P. Skokov, M. Fries, A. Taubel, I. Radulov, F. Scheibel, D. Benke, S. Riegg, O. Gutfleisch, "Making a Cool Choice: The Materials Library of Magnetic Refrigeration," Adv. Energy Mater., 2019.
[5]L.M. Moreno-Ramírez, C. Romero-Muñiz, J.Y. Law, V. Franco, A. Conde, I.A. Radulov, F. Maccari, K.P. Skokov, O. Gutfleisch, "The role of Ni in modifying the order of the phase transition of La(Fe,Ni,Si)13," Acta Mater., 160, 137–146, 2018.
[6]B. Eggert, J. Lill, D. Günzing, A. Terwey, I.A. Radulov, F. Wilhelm, A. Rogalev, M. Rovezzi, K. Skokov, K. Ollefs, O. Gutfleisch, M.E. Gruner, H. Wende, "Local magnetic and geometric structure in Mn-doped La(Fe,Si)13," J. Alloys Compd., 1031, 180586, 2025.
[7]L.M. Moreno-Ramírez, C. Romero-Muñiz, J.Y. Law, V. Franco, A. Conde, I.A. Radulov, F. Maccari, K.P. Skokov, O. Gutfleisch, "Tunable first order transition in La(Fe,Cr,Si)13 compounds," Acta Mater., 175, 406–414, 2019.
[8]I.A. Radulov, D.Y. Karpenkov, K.P. Skokov, A.Y. Karpenkov, T. Braun, V. Brabänder, T. Gottschall, M. Pabst, B. Stoll, O. Gutfleisch, "Production and properties of metal-bonded La(Fe,Mn,Si)13Hx composite material," Acta Mater., 127, 389–399, 2017.
[9]I.A. Radulov, D.Y. Karpenkov, M. Specht, T. Braun, A.Y. Karpenkov, K.P. Skokov, O. Gutfleisch, "Heat Exchangers from Metal-Bonded La(Fe,Mn,Si)13Hx Powder," IEEE Trans. Magn., 53(11), 2017.
[10]A. Aubert, K. Skokov, G. Gomez, A. Chirkova, I. Radulov, F. Wilhelm, A. Rogalev, H. Wende, O. Gutfleisch, K. Ollefs, "Simultaneous Multi-Property Probing During Magneto-Structural Phase Transitions," IEEE Trans. Instrum. Meas., 71, 1–9, 2022.
[11]O. Gutfleisch, T. Gottschall, M. Fries, D. Benke, I. Radulov, K.P. Skokov, H. Wende, M. Gruner, M. Acet, P. Entel, M. Farle, "Mastering hysteresis in magnetocaloric materials," Phil. Trans. R. Soc. A, 374(2074), 2016.
[12]"Magnetic energy conversion," in Comprehensive Energy Systems, 2025.
[13]Bundesministerium für Wirtschaft und Energie, "Für mehr Versorgungssicherheit bei Permanentmagneten," Press Release, Aug. 5, 2025.
[14]E. Righetti, V. Rizos, "Understanding the barriers to recycling critical raw materials for the energy transition," Energy Reports, 12, 1673–1682, 2024.
[15]G. Li et al., "Rare earth permanent magnets for the green energy transition," Resources, Conservation and Recycling, 2024.
[16]"Rare Earth Magnet Global Market Insights 2025, Analysis and Forecast to 2030," Research and Markets Report, Nov. 2025.