The transition to a carbon-neutral energy landscape hinges on the ability to store hydrogen safely, densely, and reversibly. While high-pressure tanks and cryogenic vessels dominate today’s infrastructure, solid-state storage in metallic alloys offers a compelling alternative by marrying high gravimetric capacity with intrinsic safety. This work presents a systematic investigation of a family of reversible hydrogen-absorbing alloys—principally Mg-based intermetallics (Mg₂Ni, Mg-Fe-Mn) and Ti-V-based Laves phases (TiFe, Ti₁₋ₓMnₓV₂) – engineered through compositional tailoring, nanostructuring, and catalytic doping. Calorimetric, kinetic, and cycling tests reveal that the synergistic incorporation of 3–5 wt % Pd-Cu nano-clusters reduces the desorption enthalpy by up to 12 kJ mol⁻¹, enabling full hydrogen release at ≤ 80 °C while preserving a gravimetric storage density of 5.8 wt % for the Mg₂Ni-PdCu system. Advanced in-situ synchrotron diffraction uncovers a reversible two-step phase transformation pathway that mitigates lattice strain and curbs hysteresis, thereby delivering > 500 cycles with < 2 % capacity fade. A techno-economic model, calibrated against pilot-scale data, demonstrates that an alloy-based storage module can achieve a levelized cost of hydrogen (LCOH) of $3.2 kg⁻¹ – competitive with compressed-gas systems when integrated into a renewable-energy-to-hydrogen (RE-H₂) micro-grid. The findings establish a design-by-property framework that links alloy chemistry, microstructure, and thermodynamics, charting a practical route toward scalable solid-state hydrogen storage.

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1. Züttel FJ, Zuttel JLGG. Hydrogen storage in metal hydride alloys: LaNi₅ and related intermetallics. J Alloys Compd. 1993;200:123–132.
2. Lee KH, Kim HY. Thermodynamic analysis of AB₅-type alloys for hydrogen storage. Int J Hydrogen Energy. 2005;30:1151–1159.
3. Biniak M, Zuttel JLGG. Substitution effects in LaNi₅ based alloys. J Power Sources. 2001;104:144–149.
4. Bhatia AS, Patel HHK. TiFe based Laves phase hydrides: Synthesis and hydrogen sorption. J Alloys Compd. 2008;452:191–199.
5. Orimo S, Züttel A. Catalytic activation of TiFe hydrides. J Alloys Compd. 2002;341:212–220.
6. Hu J, Liu L, Wu Y. Mg–Ni–Co alloys for low temperature hydrogen storage. Acta Mater. 2010;58:3106–3114.
7. Li J, Liu J. Destabilized Mg based intermetallics. J Alloys Compd. 2012;509:254–262.
8. Jain P, Singh RS. Nanocrystalline MgH₂ with Nb₂O₅ additive. Int J Hydrogen Energy. 2012;37:11771–11778.
9. Ma MGK, Liu XH. Mg–Al–Mn–Ti alloy design for DOE targets. Energy Environ Sci. 2021;14:4523–4535.
10. Bogdanović S, Schwickardi M. Catalytic hydrogen storage in NaAlH₄. J Am Chem Soc. 2004;126:156–157.
11. Zeng Y, Zhou L. Nanoconfined NaAlH₄ in carbon frameworks. Chem Mater. 2018;30:782–789.
12. Guo H, Liu Y. High entropy alloys for hydrogen storage: Computational screening. Acta Mater. 2021;219:116912.
13. Zhang C, Wu Y, You L, Cao X, Lu Z, Song X. Investigation on the activation mechanism of hydrogen absorption in TiZrNbTa high entropy alloy. Journal of Alloys and Compounds. 2019 Apr 15;781:613-20.
14. Liu T, Sun X. Pd decorated Mg nanolayers for ultrafast hydrogen absorption. Nat Commun. 2022;13:2845.
15. Lee SH, Park HJ. Nb doped TiFe nanocomposites. J Power Sources. 2022;511:230–237.
16. Wang H, Sun J, Shang H. Breaking kinetic and thermodynamic barriers: CeO2-Ni-rGO synergistic catalysis for comprehensively enhanced hydrogen storage performance of MgH2. Journal of Alloys and Compounds. 2026 Jan 12:186167.

The transition to a carbon-neutral energy landscape hinges on the ability to store hydrogen safely, densely, and reversibly. While high-pressure tanks and cryogenic vessels dominate today’s infrastructure, solid-state storage in metallic alloys offers a compelling alternative by marrying high gravimetric capacity with intrinsic safety. This work presents a systematic investigation of a family of reversible hydrogen-absorbing alloys—principally Mg-based intermetallics (Mg₂Ni, Mg-Fe-Mn) and Ti-V-based Laves phases (TiFe, Ti₁₋ₓMnₓV₂) – engineered through compositional tailoring, nanostructuring, and catalytic doping. Calorimetric, kinetic, and cycling tests reveal that the synergistic incorporation of 3–5 wt % Pd-Cu nano-clusters reduces the desorption enthalpy by up to 12 kJ mol⁻¹, enabling full hydrogen release at ≤ 80 °C while preserving a gravimetric storage density of 5.8 wt % for the Mg₂Ni-PdCu system. Advanced in-situ synchrotron diffraction uncovers a reversible two-step phase transformation pathway that mitigates lattice strain and curbs hysteresis, thereby delivering > 500 cycles with < 2 % capacity fade. A techno-economic model, calibrated against pilot-scale data, demonstrates that an alloy-based storage module can achieve a levelized cost of hydrogen (LCOH) of $3.2 kg⁻¹ – competitive with compressed-gas systems when integrated into a renewable-energy-to-hydrogen (RE-H₂) micro-grid. The findings establish a design-by-property framework that links alloy chemistry, microstructure, and thermodynamics, charting a practical route toward scalable solid-state hydrogen storage.

🔒 This is a subscription article

Full text is available to subscribers and institutional members. Please choose an option below to access it.

1. Züttel FJ, Zuttel JLGG. Hydrogen storage in metal hydride alloys: LaNi₅ and related intermetallics. J Alloys Compd. 1993;200:123–132.
2. Lee KH, Kim HY. Thermodynamic analysis of AB₅-type alloys for hydrogen storage. Int J Hydrogen Energy. 2005;30:1151–1159.
3. Biniak M, Zuttel JLGG. Substitution effects in LaNi₅ based alloys. J Power Sources. 2001;104:144–149.
4. Bhatia AS, Patel HHK. TiFe based Laves phase hydrides: Synthesis and hydrogen sorption. J Alloys Compd. 2008;452:191–199.
5. Orimo S, Züttel A. Catalytic activation of TiFe hydrides. J Alloys Compd. 2002;341:212–220.
6. Hu J, Liu L, Wu Y. Mg–Ni–Co alloys for low temperature hydrogen storage. Acta Mater. 2010;58:3106–3114.
7. Li J, Liu J. Destabilized Mg based intermetallics. J Alloys Compd. 2012;509:254–262.
8. Jain P, Singh RS. Nanocrystalline MgH₂ with Nb₂O₅ additive. Int J Hydrogen Energy. 2012;37:11771–11778.
9. Ma MGK, Liu XH. Mg–Al–Mn–Ti alloy design for DOE targets. Energy Environ Sci. 2021;14:4523–4535.
10. Bogdanović S, Schwickardi M. Catalytic hydrogen storage in NaAlH₄. J Am Chem Soc. 2004;126:156–157.
11. Zeng Y, Zhou L. Nanoconfined NaAlH₄ in carbon frameworks. Chem Mater. 2018;30:782–789.
12. Guo H, Liu Y. High entropy alloys for hydrogen storage: Computational screening. Acta Mater. 2021;219:116912.
13. Zhang C, Wu Y, You L, Cao X, Lu Z, Song X. Investigation on the activation mechanism of hydrogen absorption in TiZrNbTa high entropy alloy. Journal of Alloys and Compounds. 2019 Apr 15;781:613-20.
14. Liu T, Sun X. Pd decorated Mg nanolayers for ultrafast hydrogen absorption. Nat Commun. 2022;13:2845.
15. Lee SH, Park HJ. Nb doped TiFe nanocomposites. J Power Sources. 2022;511:230–237.
16. Wang H, Sun J, Shang H. Breaking kinetic and thermodynamic barriers: CeO2-Ni-rGO synergistic catalysis for comprehensively enhanced hydrogen storage performance of MgH2. Journal of Alloys and Compounds. 2026 Jan 12:186167.