To achieve the shift to renewable energies, efficient energy storage is of the upmost importance. Hydrogen as a chemical energy storage represents a promising technology due to its high gravimetric energy density. However, the most efficient form of hydrogen storage still remains an open question. Absorption-based storage of hydrogen in metal hydrides offers high volumetric energy densities as well as safety advantages. In this work technical, economic and environmental aspects of different metal hydride materials are investigated. An overview of the material properties, production methods as well as possibilities for enhancement of properties are presented. Furthermore, impacts on material costs, abundance of raw materials and dependency on imports are discussed. Advantages and disadvantages of selected materials are derived and may serve as a decision basis for material selection based on application. Further research on enhancement of material properties as well as on the system level is required for widespread application of metal hydrides. 

A review on metal hydride materials for hydrogen storage

Magnesium hydride (MgH2) is the mostly used material for solid-state hydrogen storage. However, their slow kinetics and highly unfavorable thermodynamics make them unsuitable for the practical applications. The current study describes the unusual catalytic action of a new class of catalyst, a high-entropy alloy (HEA) of Al20Cr16Mn16Fe16Co16Ni16 and its leached version, on the de/re-hydrogenation properties of MgH2. The onset desorption temperature of MgH2 was reduced significantly from 360 °C (for ball-milled MgH2) to 338 °C when it was catalyzed with a leached HEA-based catalyst. On the other hand, a fast de/re-hydrogenation kinetics of MgH2 was observed during the addition of leached HEA-based catalyst. It absorbed ∼6.1 wt% of hydrogen in just 2 min at a temperature of 300 °C under 10 atm hydrogen pressure and desorbed ∼5.4 wt% within 40 min. At moderate temperatures and low pressure, the HEA-based catalyst reduced desorption temperatures and improved re-hydrogenation kinetics. Even after 25 cycles of de/re-hydrogenation, the storage capacity of MgH2 catalyzed with the leached version of HEA degrades negligibly. 

Superior catalytic action of high-entropy alloy on hydrogen sorption properties of MgH2

While magnesium hydride (MgH2) has drawn considerable attention as a promising hydrogen storage material, it suffers from sluggish kinetics and high desorption temperature, hindering potential applications. Herein, we show that the hydrogen desorption kinetics of MgH2 can be significantly improved using bimetallic oxide MnV2O6 as the catalyst. A MgH2-MnV2O6 composite was prepared by a high-energy ball milling method. The results showed that the MgH2-MnV2O6 composite can release 5.57 wt % hydrogen within 10 min under 250 °C. The dehydrogenated MgH2-MnV2O6 sample can absorb 3.09 wt % hydrogen within 10 min under 50 °C. Notably, the reversible hydrogen storage property did not degrade at least within 100 cycles, showing excellent cycle stability. X-ray diffraction and transmittance electron microscopy measurements revealed that MnV alloy and V2O3 phases were formed during the ball milling process, leading to the synergistic catalytic effect. We argue that the bimetallic MnV alloy plays key catalytic roles in this system because MnV alloy can promote the fracture of the H-H and Mg-H bonds, significantly improving the hydrogen storage kinetics and low-temperature reversible hydrogen storage performance of MgH2.

Synergistic Effect of a Facilely Synthesized MnV2O6 Catalyst on Improving the Low-Temperature Kinetic Properties of MgH2.

The development of materials has coincided with the development of human civilization. In recent years, high-entropy alloys (HEAs) have been extensively applied to structural and functional materials owing to their unique physical and chemical properties. Therefore, HEAs have emerged as a promising materials. This review summarizes recent research progress on HEAs for hydrogen storage. First, the history and basic concepts of HEAs are systematically introduced. Furthermore, recent developments in the field of HEA-based hydrogen storage are reviewed and discussed. The preparation process, design methods, microstructures, and hydrogen-storage performance of HEAs are systematically compared and summarized. Other hydrogen-related applications are also presented. Finally, the shortcomings of the HEAs currently used in hydrogen-storage applications are highlighted, and future development directions are outlined. 

High-entropy alloys for solid hydrogen storage: a review

Hydrogen-based energy systems offer potential solutions for replacing fossil fuels in the future. However, the practical utilization of hydrogen energy depends partly on safe and efficient hydrogen storage techniques. The development of hydrogen storage materials has attracted extensive interest for decades. Solid-state hydrogen storage systems based on metal hydride materials provide great promises for many applications. Recently, interest has been revived in TiFe alloys as a prime candidate for stationary hydrogen storage material. The advantages of TiFe alloys over some of the other solid metal hydrides include that it can hydrogenate and dehydrogenate at near room temperature under near atmospheric pressures and that it is a low-cost material because there are abundant supplies of Fe and Ti on the earth's crust. However, the TiFe alloy must be activated at relatively high temperatures (400–450 °C) and high pressure of hydrogen (65 bar) before it can be hydrogenated, which is a hindrance to the industrial-scale application of TiFe alloys. The materials science community on hydrogen storage materials has conducted and reported considerable amounts of studies on TiFe-based alloys. In this work, we provided a comprehensive review of TiFe-based alloys. The fundamentals and synthesis approaches of TiFe-based alloys were summarized. The activation properties of TiFe-based alloys including the understanding of the activation mechanisms and the methods for improving the activation kinetics were reviewed. Moreover, the cycle stability and anti-poisoning ability were discussed. Finally, the potential applications and the perspective of TiFe-based alloys were introduced. 

An overview of TiFe alloys for hydrogen storage: Structure, processes, properties, and applications

The superior catalytic activity of TiVNb-based high entropy alloys enhanced the reversible hydrogen storage and low-temperature hydrogenation properties of MgH2.

TiVNb-based high entropy alloys as catalysts for enhanced hydrogen storage in nanostructured MgH2

Nano-engineering is of particular interest in tailoring the hydrogen storage properties of magnesium hydride (MgH2). This work demonstrates in situ formation of nanocrystalline MgH2 by hydrogenation at room temperature. We investigated the effects of hydrogenation variables on the MgH2 nanostructure. The results showed a large amount of MgH2 nanocrystallites with sizes of 4–10 nm in the hydrogenated samples. The sample recharged at 298 K under 0.1 bar hydrogen showed MgH2 nanocrystallites with a mean size of 5.2 nm. The dehydrogenation kinetics of the sample hydrogenated at lower pressure are improved over samples hydrogenated at higher pressures. The in situ formation of nanocrystalline MgH2 can be achieved by deliberately engineering the nucleation and growth rate of MgH2. Hydrogenation pressure, temperature, and the defect density of the material are the critical parameters affecting the nucleation rate of MgH2. In addition to low temperature, hydrogenation under lower pressure can significantly slow the growth rate of MgH2 during hydrogenation. These findings provide a different strategy enabling in-process control over the nanostructure of MgH2. 

In situ Formation of Nanocrystalline MgH2 through Room Temperature Hydrogenation

The Role of Oxide in Hydrogen Absorption and Desorption Kinetics of MgH2-based Material

The mechanistic role of Ti4Fe2O1- phases in the activation of TiFe alloys for hydrogen storage

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