Artificial Intelligence and High-Throughput Computational Workflows Empowering the Fast Screening of Metal-Organic Frameworks for Hydrogen Storage.

Metal-organic frameworks (MOFs) are one of the most promising hydrogen-storing materials due to their rich specific surface area, adjustable topological and pore structures, and modified functional groups. In this work, we developed automatically parallel computational workflows for high-throughput screening of ∼11,600 MOFs from the CoRE database and discovered 69 top-performing MOF candidates with work capacity greater than 1.00 wt % at 298.5 K and a pressure swing between 100 and 0.1 bar, which is at least twice that of MOF-5. In particular, ZITRUP, OQFAJ01, WANHOL, and VATYIZ showed excellent hydrogen storage performance of 4.48, 3.16, 2.19, and 2.16 wt %. We specifically analyzed the relationship between pore-limiting diameter, largest cavity diameter, void fraction, open metal sites, metal elements or nonmetallic atomic elements, and deliverable capacity and found that not only geometrical and physical features of crystalline but also chemical properties of adsorbate sites determined the H2 storage capacity of MOFs at room temperature. It is highlighted that we first proposed the modified crystal graph convolutional neural networks by incorporating the obtained geometrical and physical features into the convolutional high-dimensional feature vectors of period crystal structures for predicting H2 storage performance, which can improve the prediction accuracy of the neural network from the former mean absolute error (MAE) of 0.064 wt % to the current MAE of 0.047 wt % and shorten the consuming time to about 10-4 times of high-throughput computational screening. This work opens a new avenue toward high-throughput screening of MOFs for H2 adsorption capacity, which can be extended for the screening and discovery of other functional materials.

Aquatic toxicity, bioaccumulation potential, and human estrogen/androgen activity of three oxo-Liquid Organic Hydrogen Carrier (oxo-LOHC) systems.

The Liquid Organic Hydrogen Carrier (LOHC) technology offers a technically attractive way for hydrogen storage. If LOHC systems were to fully replace liquid fossil fuels, they would need to be handled at the multi-million tonne scale. To date, LOHC systems on the market based on toluene or benzyltoluene still offer potential for improvements. Thus, it is of great interest to investigate potential LOHCs that promise better performance and environmental/human hazard profiles. In this context, we investigated the acute aquatic toxicity of oxygen-containing LOHC (oxo-LOHC) systems. Toxic Ratio (TR) values of oxo-LOHC compounds classify them baseline toxicants (0.1 < TR < 10). Additionally, the mixture toxicity test conducted with D. magna suggests that the overall toxicity of a benzophenone-based system can be accurately predicted using a concentration addition model. The estimation of bioconcentration factors (BCF) through the use of the membrane-water partition coefficient indicates that oxo-LOHCs are unlikely to be bioaccumulative (BCF < 2000). None of the oxo-LOHC compounds exhibited hormonal disrupting activities at the tested concentration of 2 mg/L in yeast-based reporter gene assays. Therefore, the oxo-LOHC systems seem to pose a low level of hazard and deserve more attention in ongoing studies searching for the best hydrogen storage technologies.

Nanoencapsulated MgBu2@ZIF-67 to Construct High Loading Mg-Co@C Nanocomposites: Breaking Through the Barrier of Room Temperature Onset Dehydrogenation.

The synergies of nanoconfinement and catalysis is an effective strategy to improve the kinetic and thermodynamic properties of Mg-based materials. However, obtaining Mg-based materials with high loading, anti-aggregation, and containing nanocatalysts to achieve dehydrogenation at room temperature remains a huge challenge. Herein, a novel and universal preparation strategy for Mg-Co@C nanocomposites with 9.5 nm Mg nanoparticles and 9.4 nm Co nanocatalysts embedded in carbon scaffold is reported. The 9.3 nm MgBu2 nanosheets precipitated by solvent displacement are encapsulated in ZIF-67 to prepare MgBu2@ZIF-67 precursors, then removing excess MgBu2 on the precursor surface and pyrolysis to obtain Mg-Co@C. It is worth noting that the Mg loading rate of Mg-Co@C is as high as rare 69.7%. Excitingly, the Mg-Co@C begins to dehydrogenate at room temperature with saturate capacity of 5.1 wt.%. Meanwhile, its dehydrogenation activation energy (Ea(des) = 68.8 kJ mol-1) and enthalpy (ΔH(des) = 61.6 kJ mol-1) significantly decrease compared to bulk Mg. First principles calculations indicate that the hydrogen adsorption energy on the Mg2CoH5 surface is only -0.681 eV. This work provides a universally applicable novel method for the preparation of nanoscale Mg-based materials with various nanocatalysts added, and provides new ideas for Mg-based materials to achieve room temperature hydrogen storage.

Adsorption and storage of hydrogen- A computational model approach.

Due to the imperative global energy transition crisis, hydrogen storage and adsorption technologies are becoming popular with the growing hydrogen economy. Recently, complex hydrides have been one of the most reliable materials for storing and transporting hydrogen gas to various fuel cells to generate clean energy with zero carbon emissions. With the ever-increasing carbon emissions, it is necessary to substitute the current energy sources with green hydrogen-based efficient energy-integrated systems. Herein, we propose an input-output model that comprehends complex hydrides such as lithium and magnesium alanates, amides and borohydrides to predict, estimate, and directly analyse hydrogen storage and adsorption. A critical and thorough comparative analysis of the respective complex hydrides for hydrogen adsorption and storage is discussed, elucidating the storage applications in water bodies. Several industrial scale-up processes, economic analysis, and plant design of hydrogen storage and adsorption approaches are suggested through volumetric and gravimetric calculations.

Additively manufactured high-entropy alloys for hydrogen storage: Predictions.

This review paper covers an analysis of the empirical calculations, additive manufacturing (AM) and hydrogen storage of refractory high-entropy alloys undertaken to determine the structural compositions, particularly focusing on their applicability in research and experimental settings. The inventors of multi-component high-entropy alloys (HEAs) calculated that trillions of materials could be manufactured from elements in the periodic table, estimating a vast number, N = 10^100, using Stirling's approximation. The significant contribution of semi-empirical parameters such as Gibbs free energy ΔG, enthalpy of mixing ΔH mix , entropy of mixing ΔS mix , atomic size difference Δδ, valence electron concentration VEC, and electronegativity difference Δχ are to predict BCC and/or FCC phases in HEAs. Additive manufacturing facilitates the determination of refractory HEAs systems with the most stable solid-solution and single-phase, and their subsequent hydrogen storage capabilities. Hydride materials, especially those from HEAs manufactured by AM as bulk and solid materials, have great potential for H2 storage, with storage capacities that can be as high as 1.81 wt% of H2 adsorbed for a ZrTiVCrFeNi system. Furthermore, laser metal deposition (LMD) is the most commonly employed technique for fabricating refractory high entropy alloys, surpassing other methods in usage, thus making it particularly suitable for H2 storage.

Recent Advances in the Preparation Methods of Magnesium-Based Hydrogen Storage Materials.

Magnesium-based hydrogen storage materials have garnered significant attention due to their high hydrogen storage capacity, abundance, and low cost. However, the slow kinetics and high desorption temperature of magnesium hydride hinder its practical application. Various preparation methods have been developed to improve the hydrogen storage properties of magnesium-based materials. This review comprehensively summarizes the recent advances in the preparation methods of magnesium-based hydrogen storage materials, including mechanical ball milling, methanol-wrapped chemical vapor deposition, plasma-assisted ball milling, organic ligand-assisted synthesis, and other emerging methods. The principles, processes, key parameters, and modification strategies of each method are discussed in detail, along with representative research cases. Furthermore, the advantages and disadvantages of different preparation methods are compared and evaluated, and their influence on hydrogen storage properties is analyzed. The practical application potential of these methods is also assessed, considering factors such as hydrogen storage performance, scalability, and cost-effectiveness. Finally, the existing challenges and future research directions in this field are outlined, emphasizing the need for further development of high-performance and cost-effective magnesium-based hydrogen storage materials for clean energy applications. This review provides valuable insights and references for researchers working on the development of advanced magnesium-based hydrogen storage technologies.

Magnesium-Based Hydrogen Storage Alloys: Advances, Strategies, and Future Outlook for Clean Energy Applications.

Magnesium-based hydrogen storage alloys have attracted significant attention as promising materials for solid-state hydrogen storage due to their high hydrogen storage capacity, abundant reserves, low cost, and reversibility. However, the widespread application of these alloys is hindered by several challenges, including slow hydrogen absorption/desorption kinetics, high thermodynamic stability of magnesium hydride, and limited cycle life. This comprehensive review provides an in-depth overview of the recent advances in magnesium-based hydrogen storage alloys, covering their fundamental properties, synthesis methods, modification strategies, hydrogen storage performance, and potential applications. The review discusses the thermodynamic and kinetic properties of magnesium-based alloys, as well as the effects of alloying, nanostructuring, and surface modification on their hydrogen storage performance. The hydrogen absorption/desorption properties of different magnesium-based alloy systems are compared, and the influence of various modification strategies on these properties is examined. The review also explores the potential applications of magnesium-based hydrogen storage alloys, including mobile and stationary hydrogen storage, rechargeable batteries, and thermal energy storage. Finally, the current challenges and future research directions in this field are discussed, highlighting the need for fundamental understanding of hydrogen storage mechanisms, development of novel alloy compositions, optimization of modification strategies, integration of magnesium-based alloys into hydrogen storage systems, and collaboration between academia and industry.

Ball Milling Innovations Advance Mg-Based Hydrogen Storage Materials Towards Practical Applications.

Mg-based materials have been widely studied as potential hydrogen storage media due to their high theoretical hydrogen capacity, low cost, and abundant reserves. However, the sluggish hydrogen absorption/desorption kinetics and high thermodynamic stability of Mg-based hydrides have hindered their practical application. Ball milling has emerged as a versatile and effective technique to synthesize and modify nanostructured Mg-based hydrides with enhanced hydrogen storage properties. This review provides a comprehensive summary of the state-of-the-art progress in the ball milling of Mg-based hydrogen storage materials. The synthesis mechanisms, microstructural evolution, and hydrogen storage properties of nanocrystalline and amorphous Mg-based hydrides prepared via ball milling are systematically reviewed. The effects of various catalytic additives, including transition metals, metal oxides, carbon materials, and metal halides, on the kinetics and thermodynamics of Mg-based hydrides are discussed in detail. Furthermore, the strategies for synthesizing nanocomposite Mg-based hydrides via ball milling with other hydrides, MOFs, and carbon scaffolds are highlighted, with an emphasis on the importance of nanoconfinement and interfacial effects. Finally, the challenges and future perspectives of ball-milled Mg-based hydrides for practical on-board hydrogen storage applications are outlined. This review aims to provide valuable insights and guidance for the development of advanced Mg-based hydrogen storage materials with superior performance.

Advances and Prospects of Nanomaterials for Solid-State Hydrogen Storage.

Hydrogen energy, known for its high energy density, environmental friendliness, and renewability, stands out as a promising alternative to fossil fuels. However, its broader application is limited by the challenge of efficient and safe storage. In this context, solid-state hydrogen storage using nanomaterials has emerged as a viable solution to the drawbacks of traditional storage methods. This comprehensive review delves into the recent advancements in nanomaterials for solid-state hydrogen storage, elucidating the fundamental principles and mechanisms, highlighting significant material systems, and exploring the strategies of surface and interface engineering alongside catalytic enhancement. We also address the primary challenges and provide future perspectives on the development of nanomaterial-based hydrogen storage technologies. Key discussions include the role of nanomaterial size effects, surface modifications, nanocomposites, and nanocatalysts in optimizing storage performance.

Computational evaluation of novel XCuH3 (X = Li, Na and K) perovskite-type hydrides for hydrogen storage applications using LDA and GGA approach.

Hydrogen energy has attracted a lot of interest from researchers as a sustainable and renewable energy source, but there are some technical challenges related to its storage. Hydride materials demonstrate the ability to store hydrogen adequately and safely. In the current study, we have investigated the structural and optoelectronic properties of the XCuH3 (where X = Li, Na and K) perovskite-type hydride using LDA and GGA formalisms for hydrogen storage application. Electronic properties such as band structure, density of states reveal the metallic character of the studied XCuH3 hydrides. Various optical parameters such as the complex dielectric function, refractive index, extinction coefficient, absorption coefficient, reflectivity, optical conductivity, energy loss function, and joint density of states have been computed and compared. The gravimetric hydrogen storage capacity for LiCuH3, NaCuH3 and KCuH3 are found to be 4.11, 3.37 and 2.86 wt%, respectively. The computed values of the gravimetric ratio manifest that XCuH3 hydrides are potential candidates for hydrogen storage applications. These calculations are made for the first time for XCuH3 hydrides and will be inspirational in the future for comparison and for hydrogen storage purposes.

Chemical-based Hydrogen Storage Systems: Recent Developments, Challenges, and Prospectives.

Hydrogen (H2) is being acknowledged as the future energy carrier due to its high energy density and potential to mitigate the intermittency of other renewable energy sources. H2 also ensures a clean, carbon-neutral, and sustainable environment for current and forthcoming generations by contributing to the global missions of decarbonization in the transportation, industrial, and building sectors. Several H2 storage technologies are available and have been employed for its secure and economical transport. The existing H2 storage and transportation technologies like liquid-state, cryogenic, or compressed hydrogen are in use but still suffer from significant challenges regarding successful realization at the commercial level. These factors affect the overall operational cost of technology. Therefore, H2 storage demands novel technologies that are safe for mobility, transportation, long-term storage, and yet it is cost-effective. This review article presents potential opportunities for H2 storage technologies, such as physical and chemical storage. The prime characteristics and requirements of H2 storage are briefly explained. A detailed discussion of chemical-based hydrogen storage systems such as metal hydrides, chemical hydrides (CH3OH, NH3, and HCOOH), and liquid organic hydrogen carriers (LOHCs) is presented. Furthermore, the recent developments and challenges regarding hydrogen storage, their real-world applications, and prospects have also been debated.

MXenes and MXene-Based Metal Hydrides for Solid-State Hydrogen Storage: A Review.

Hydrogen-driven energy is fascinating among the everlasting energy sources, particularly for stationary and onboard transportation applications. Efficient hydrogen storage presents a key challenge to accomplishing the sustainability goals of hydrogen economy. In this regard, solid-state hydrogen storage in nanomaterials, either physically or chemically adsorbed, has been considered a safe path to establishing sustainability goals. Though metal hydrides have been extensively explored, they fail to comply with the set targets for practical utilization. Recently, MXenes, both in bare form and hybrid state with metal hydrides, have proven their flair in ascertaining the hydrides' theoretical and experimental hydrogen storage capabilities far beyond the fancy materials and current state-of-the-art technologies. This review encompasses the significant accomplishments achieved by MXenes (primarily in 2019-2024) for enhancing the hydrogen storage performance of various metal hydride materials such as MgH2, AlH3, Mg(BH4)2, LiBH4, alanates, and composite hydrides. It also discusses the bottlenecks of metal hydrides for hydrogen storage, the potential use of MXenes hybrids, and their challenges, such as reversibility, H2 losses, slow kinetics, and thermodynamic barriers. Finally, it concludes with a detailed roadmap and recommendations for mechanistic-driven future studies propelling toward a breakthrough in solid material-driven hydrogen storage using cost-effective, efficient, and long-lasting solutions.

New-Generation Materials for Hydrogen Storage in Medium-Entropy Alloys.

This study presents the design, preparation, and characterization of thirty new medium-entropy alloys (MEAs) in three systems: Al-Ti-Nb-Zr, Al-Ti-Nb-V, and Al-Ti-Nb-Hf. The hardness of the alloys ranged from 320 to 800 HV0.3. Among the alloys studied, Al15Ti40Nb30Zr15 exhibited the highest-reversible hydrogen storage capacity (1.03 wt.%), with an H/M value of 0.68, comparable to LaNi5, but with a reduced density (5.11 g·cm-3) and without rare earth elements. This study further reveals a strong correlation between hardness and hydrogen absorption/desorption; higher hardness is responsible for reduced hydrogen uptake. This finding highlights the interplay between a material's properties and hydrogen storage behavior in MEAs, and has implications for the development of efficient hydrogen storage materials.

Improved dehydrogenation performance of LiAlH4 doped with BaMnO3.

Due to its high gravimetric capacity of hydrogen (10.5 wt%), LiAlH4 has been regarded as a promising material for solid-state hydrogen storage material for onboard usage. However, high decomposition temperature, poor kinetics and irreversibility retard its application. To counter this problem, various weight percentages of BaMnO3 are introduced into the LiAlH4 system as an additive in this work. As a result, the starting hydrogen release of LiAlH4 was reduced to 109-115 °C and the second desorption temperature occurred at around 134-158 °C, much lower than pure LiAlH4. The isothermal desorption kinetics also proved that faster desorption kinetics can be observed at 90 °C for 80 min. About 2.00-2.60 wt% of H2 could be desorbed by the composite, whereas only <1.00 wt% of H2 was desorbed by undoped LiAlH4. Additionally, adding BaMnO3 reduced the activation energies by 30 kJ/mol for the first stages and 34 kJ/mol for the second stages. Based on the X-ray diffraction result, the active species formed of MnO2 and Ba or Ba-containing materials are believed to be responsible for the noticeable enhancement in the desorption properties of LiAlH4.

Physical Analysis and Mathematical Modeling of the Hydrogen Storage Process in the MmNi4.2Mn0.8 Compound.

The results of an experimental and mathematical study into the MmNi4.2Mn0.8 compound's hydrogen storage properties are presented in the present research. Plotting and discussion of the experimental isotherms (P-C-T) for different starting temperatures (288 K, 298 K, 308 K, and 318 K) were carried out first. Then, the enthalpy and entropy of formation (ΔH0, ΔS0) were deduced from the plot of van't Hoff. Following that, the P-C-T were contrasted with a mathematical model developed via statistical physics modeling. The steric and energetic parameters, such as the number of the receiving sites (n1, n2), their densities (Nm1, Nm2), and the energy parameters (P1, P2) of the system, were calculated thanks to the excellent agreement between the numerical and experimental results. Therefore, plotting and discussing these parameters in relation to temperature preceded their application in determining the amount of hydrogen in each type of site per unit of metal ([H/M]1, [H/M]2) as well as for the entire system [H/M] versus temperature and pressure besides the absorption energies associated with each kind of site (ΔE1, ΔE2) and the thermodynamic functions (free energy, Gibbs energy, and entropy) that control the absorption reaction.

Challenges of Green Transition in Polymer Production: Applications in Zero Energy Innovations and Hydrogen Storage.

The green transition in the sustainable production and processing of polymers poses multifaceted challenges that demand integral comprehensive solutions. Specific problems of presences of toxic trace elements are often missed and this prevents shifting towards eco-friendly alternatives. Therefore, substantial research and the development of novel approaches is needed to discover and implement innovative, sustainable production materials and methods. This paper is focused on the most vital problems of the green transition from the aspect of establishing universally accepted criteria for the characterization and classification of eco-friendly polymers, which is essential to ensuring transparency and trust among consumers. Additionally, the recycling infrastructure needs substantial improvement to manage the end-of-life stage of polymer products effectively. Moreover, the lack of standardized regulations and certifications for sustainable polymers adds to the complexity of this problem. In this paper we propose solutions from the aspect of standardization protocols for the characterization of polymers foreseen as materials that should be used in Zero Energy Innovations in Hydrogen Storage. The role model standards originate from eco-labeling procedures for materials that come into direct or prolonged contact with human skin, and that are monitored by different methods and testing procedures. In conclusion, the challenges of transitioning to green practices in polymer production and processing demands a concerted effort from experts in the field which need to emphasize the problems of the analysis of toxic ultra trace and trace impurities in samples that will be used in hydrogen storage, as trace impurities may cause terrific obstacles due to their decreasing the safety of materials. Overcoming these obstacles requires the development and application of current state-of-the-art methodologies for monitoring the quality of polymers during their recycling, processing, and using, as well as the development of other technological innovations, financial initiatives, and a collective commitment to fostering a sustainable and environmentally responsible future for the polymer industry and innovations in the field of zero energy applications.

Hydrogen energy systems: Technologies, trends, and future prospects.

This review critically examines hydrogen energy systems, highlighting their capacity to transform the global energy framework and mitigate climate change. Hydrogen showcases a high energy density of 120 MJ/kg, providing a robust alternative to fossil fuels. Adoption at scale could decrease global CO2 emissions by up to 830 million tonnes annually. Despite its potential, the expansion of hydrogen technology is curtailed by the inefficiency of current electrolysis methods and high production costs. Presently, electrolysis efficiencies range between 60 % and 80 %, with hydrogen production costs around $5 per kilogram. Strategic advancements are necessary to reduce these costs below $2 per kilogram and push efficiencies above 80 %. Additionally, hydrogen storage poses its own challenges, requiring conditions of up to 700 bar or temperatures below -253 °C. These storage conditions necessitate the development of advanced materials and infrastructure improvements. The findings of this study emphasize the need for comprehensive strategic planning and interdisciplinary efforts to maximize hydrogen's role as a sustainable energy source. Enhancing the economic viability and market integration of hydrogen will depend critically on overcoming these technological and infrastructural challenges, supported by robust regulatory frameworks. This comprehensive approach will ensure that hydrogen energy can significantly contribute to a sustainable and low-carbon future.

Underground hydrogen storage: The techno-economic perspective.

The changes in the energy sector after the Paris agreement and the establishment of the Green Deal, pressed the governments to embrace new measures to reduce greenhouse gas emissions. Among them, is the replacement of fossil fuels by renewable energy sources or carbon-neutral alternative means, such as green hydrogen. As the European Commission approved green hydrogen as a clean fuel, the interest in investments and dedicated action plans related to its production and storage has significantly increased. Hydrogen storage is feasible in aboveground infrastructures as well as in underground constructions. Proper geological environments for underground hydrogen storage are porous media and rock cavities. Porous media are classified into depleted hydrocarbon reservoirs and aquifers, while rock cavities are subdivided into hard rock caverns, salt caverns, and abandoned mines. Depending on the storage option, various technological requirements are mandatory, influencing the required capital cost. Although the selection of the optimum storage technology is site depending, the techno-economical appraisal of the available underground storage options featured the porous media as the most economically attractive option. Depleted hydrocarbon reservoirs were of high interest as site characterisation and cavern mining are omitted due to pre-existing infrastructure, followed by aquifers, where hydrogen storage requires a much simpler construction. Research on data analytics and machine learning tools will open avenues for consolidated knowledge of geological storage technologies.

Exceptional Hydrogen Uptake in Crystalline InxGa1-xN Semiconductors.

The irradiation of InN and InxGa1-xN samples with low-energy H ions results in exceptionally high hydrogen uptake in a crystalline semiconductor. This phenomenon is attributed to specific In-H complex formation. By exploiting spectral fingerprints of the In-H complexes observable in In L3-edge X-ray absorption spectroscopy, we provide direct evidence of complex formation. Density functional theory calculations assist in interpreting the X-ray absorption spectra and offer insights into the energetics of complex formation. We quantify the total amount of reversibly incorporated hydrogen in these semiconductors and discuss their strengths and weaknesses as innovative materials for hydrogen storage.

Exploring Nanomaterials for Hydrogen Storage: Advances, Challenges, and Perspectives.

Hydrogen energy heralded for its environmentally friendly, renewable, efficient, and cost-effective attributes, stands poised as the primary alternative to fossil fuels in the future. Despite its great potential, the low volumetric density presents a formidable challenge in hydrogen storage. Addressing this challenge necessitates exploring effective storage techniques for a sustainable hydrogen economy. Solid-state hydrogen storage in nanomaterials (physically or chemically) holds promise for achieving large-scale hydrogen storage applications. Such approaches offer benefits, including safety, compactness, lightness, reversibility, and efficient generation of pure hydrogen fuel under mild conditions. This article presents solid-state nanomaterials, specifically nanoporous carbons (activated carbon, carbon fibers), metal-organic frameworks, covalently connected frameworks, nanoporous organic polymers, and nanoscale metal hydrides. Furthermore, new developments in hydrogen fuel cell technology for stationary and mobile applications have been demonstrated. The review outlines significant advancements thus far, identifies key barriers to practical implementation, and presents a perspective for future sustainable energy research. It concludes with recommendations to enhance hydrogen storage performance for cost-effective and long-lasting utilization.