High-throughput Screening Computation for Discovery of Porous Zeolites for Hydrogen Storage

Revealing enhancement mechanism of volumetric hydrogen storage capacity of nano-porous frameworks by molecular simulation

Volumetric Hydrogen Storage Capacity in Metal–Organic Frameworks

Macroscopically long ropes of aligned single-walled carbon nanotubes (SWNTs), synthesized by a hydrogen and argon arc discharge method, were cold pressed into tablets without any binder for measurements of their volumetric hydrogen storage capacity. The typical apparent density of the tablets was measured to be around 1.7 g/cm3 with respect to a molding pressure of 0.75 Gpa. A volumetric and mass hydrogen storage capacity of 68 kg H2/m3 and 4.0 wt %, respectively, was achieved at room temperature under a pressure of 11 MPa for suitably pretreated SWNT tablets, and more than 70% of the hydrogen adsorbed can be released under ambient pressure at room temperature. Pore structure analysis indicated that the molding process diminished the mesopore volume of the SWNT ropes, but exerts little influence on their intrinsic pore textures.

Grand Canonical Monte Carlo simulations of hydrogen and methane storage capacities of two novel Al-nia MOFs at room temperature

The inherent tradeoff between gravimetric and volumetric hydrogen storage capacities in metal-organic frameworks (MOFs) limits their commercial viability. While benchmarked MOFs like MOF-5, IRMOF-20, and PCN-610 perform well at 77 K, maintaining their performance at elevated temperatures (298 K) remains challenging. To address this, a multi-objective particle swarm optimization framework was developed to identify promising MOFs for hydrogen storage. The optimization was guided by predictions from the bootstrapped-random forest trees. This optimization yielded 152 theoretical MOF feature combinations, which were matched with 733,792 existing structures. A nearest neighbor search identified 43 promising MOFs, with Zn-based MOF-2087 emerging as the global best, exhibiting consistent hydrogen storage performance across temperatures. Grand Canonical Monte Carlo simulations confirmed its high hydrogen uptake (5.3 wt% and 7.4 gH2 L− 1 at 298 K). Molecular dynamics simulations further revealed C-clusters and metal sites as key adsorption centers, supporting the enhanced hydrogen storage behavior of MOF-2087. These findings highlight MOF-2087 as a computationally promising MOF for hydrogen storage up to 298 K and demonstrate the effectiveness of the optimization-driven screening strategy.Supplementary InformationThe online version contains supplementary material available at 10.1038/s41598-025-09654-z.

Exploring the hydrogen and methane storage capacities of novel DUT MOFs at room temperature: A Grand Canonical Monte Carlo simulation study

We first report the atomistic grand canonical Monte Carlo simulations of the synthesis of two realistic ordered microporous carbon replica in two siliceous forms of faujasite zeolite (cubic Y-FAU and hexagonal EMT). Atomistic simulations of hydrogen adsorption isotherms in these two carbon structures and their Li-doped composites were carried out to determine their storage capacities at 77 and 298 K. We found that these new forms of carbon solids and their Li-doped versions show very attractive hydrogen storage capacities at 77 and 298 K, respectively. However, for a filling pressure of 300 bars and at room temperature, bare carbons do not show advantageous performances compared to a classical gas cylinder despite of their crystalline micropore network. In comparison, Li-doped nanostructures provide reversible gravimetric and volumetric hydrogen storage capacities twice larger (3.75 wt % and 33.7 kg/m(3)). The extreme lattice stiffness of their skeleton will prevent them from collapsing under large external applied pressure, an interesting skill compared to bundle of carbon nanotubes, and metal organic frameworks (MOFs). These new ordered composites are thus very promising materials for hydrogen storage issues by contrast with MOFs.

Precision decoupling nucleation and growth kinetics remains a grand challenge to enable high‐performance MOFs for efficient hydrogen storage. Herein, by using a decelerating nucleation kinetics (denuk) strategy (k nucleation /k growth = 0.0002), a fully‐coordinated acetic acid‐tethered MOF‐808 (MOF‐808‐0.5AA‐mm) is synthesized with a volumetric hydrogen storage capacity of 50 g L −1 under 77 K and 100 bar, retaining 100% hydrogen uptake after 2000 cycles. In situ neutron powder diffraction (NPD), grand canonical Monte Carlo (GCMC) simulation, and density functional theory (DFT) calculation results collectively suggest that hydrogen initially occupies the small tetrahedral cage (site I) and gradually fills both small (site I) and large adamantane cages (site II) as pressure increases. A 100g‐H 2 ‐scale MOF‐based solid‐state hydrogen storage system integrated with a 200‐W fuel cell demonstrates ultrafast H 2 adsorption and release kinetics, maintaining 100% capacity after 100 cycles. Techno‐economic analysis (TEA) results suggest MOF‐808‐0.5AA‐mm can achieve a 45% lower levelized cost of hydrogen storage (2.34 $ kg H2 −1 ) than liquid hydrogen (4.3 $ kg H2 −1 ), approaching the compressed gas (0.9–1.2 $ kg H2 −1 ) under identical conditions. The work thus prospects a new crystallization control paradigm to achieve high‐capacity, mechanically robust, long‐duration, and cost‐effective MOF adsorbents for speed‐demanding and space‐limiting hydrogen storage applications.

Hydrogen is a clean-burning fuel that can be converted to other forms. of energy without generating any greenhouse gases. Currently, hydrogen is stored either by compression to high pressure (>700 bar) or cryogenic cooling to liquid form (<23 K). Therefore, it is essential to develop safe, reliable, and energy-efficient storage technology that can store hydrogen at lower pressures and temperatures. In this work, we systematically designed 2902 Mg-alkoxide-functionalized covalent-organic frameworks (COFs) and performed high-throughput (HT) computational screening for hydrogen storage applications at 111, 231, and 296 K. To accurately model the interaction between Mg-alkoxide sites and molecular hydrogen, we performed MP2 calculations to compute the hydrogen binding energy for different types of functionalized models, and the data were subsequently used to fit modified-Morse force field (FF) parameters. Using the developed FF models, we conducted HT grand canonical Monte Carlo (GCMC) simulations to compute hydrogen uptakes for both original and functionalized COFs. The generated data were subsequently used to evaluate the materials' gravimetric and volumetric storage performance at various temperatures (111, 231, and 296 K). Finally, we developed machine learning (ML) models to predict the hydrogen storage performance of functionalized structures based on the features of the original structures. The developed model showed excellent performance with a mean absolute error (MAE) of 0.061 wt % and 0.456 g/L for predicting the gravimetric and volumetric deliverable capacities, enabling a quick evaluation of structures in a hypothetical COF database. The screening results demonstrated that the Mg-alkoxide functionalization yields greater improvements in volumetric H2 storage capacities for COFs with smaller pores compared to those with larger (mesoporous) pores.

Evaluation and screening of multivariate metal-organic frameworks for hydrogen storage

Magnesium alloys take a special place among the hydrogen storage materials, mainly due to their high gravimetric (7.6 mass%) and volumetric (110 kgm-3) hydrogen storage capacity. Unfortunately, the kinetics of hydrogenation and hydrogen release are rather slow, which limits practical use of magnesium-based materials for hydrogen and heat storage. Refining the microstructure of magnesium alloys, ideally down to nanoscale, is known to accelerate the hydrogenation/dehydrogenation kinetics. A possible way to achieve that is by severe plastic deformation. Our first demonstration of this effect through processing of a Mg alloy (ZK60) by equal-channel angular pressing prompted a stream of further studies employing severe plastic deformation techniques to improve the hydrogen storage-relevant properties of Mg alloys. The present article provides an overview of the literature on the subject, with a natural focus on our own data.

Hydrogen fuel holds promise for clean energy solutions, particularly in onboard applications such as fuel cell vehicles. However, the development of efficient hydrogen storage systems remains a critical challenge. This study addresses this challenge by exploring the potential of high-strength novel materials, including glass, to maximize onboard hydrogen storage capacity. A mathematical approach was employed to evaluate the feasibility and efficacy of various high-strength materials for hydrogen storage. This study focused on capillary arrays as a promising storage medium and utilized mathematical modeling techniques to estimate the storage capacity enhancement achievable with different materials. The analysis revealed significant variations in storage capacity enhancements in different high-strength novel materials, with glass having promising results. Glass-based materials demonstrated the potential to meet or exceed US Department of Energy (DOE) targets for both gravimetric and volumetric hydrogen storage capacities in capillary arrays. By leveraging a mathematical approach, this study identified high-strength novel materials, including glass and polymers, capable of substantially improving onboard hydrogen storage capacity: 29 wt.% with 40 g/L for quartz glass and 25 wt.% with 38 g/L for Kevlar compared to 5.2 wt.% with 26.3 g/L from a conventional type IV tank. These findings underscore the importance of material selection in optimizing hydrogen storage systems and provide valuable insights for the design and development of next-generation hydrogen storage technologies for onboard applications.

High Volumetric Hydrogen Storage Capacity using Interpenetrated Metal–Organic Frameworks

Porous Metal-Organic Frameworks: Promising Materials for Methane Storage

The rising demand for clean energy, especially hydrogen, has heightened the need for efficient storage materials. Perovskites, with their unique structures, show great promise for hydrogen storage and optical uses. To identify promising candidates for hydrogen storage materials, the mechanical, electronic, and optical properties of four ordered vacancy double perovskite structures X2MH6 (Ba2BeH6, Ba2MgH6, Ca2BeH6, and Sr2MgH6) were predicted using density functional theory. These materials were confirmed to be stable, and their hydrogen storage capacity, mechanical properties, electronic structures, and optical performance were thoroughly analyzed. Ca2BeH6 demonstrated the highest gravimetric (6.32%) and volumetric (32.29 g·H2/L) hydrogen storage capacity, showcasing its exceptional potential. It should be noted that the hydrogen storage capacities reported here are theoretical estimates based solely on structural models, and this study does not assess the practical storage and delivery performance of these materials. Its mechanical stiffness and near-isotropic properties further enhance its practicality. Electrical studies revealed all four materials are semiconductors, all of them are direct semiconductors. Optical properties were analyzed via dielectric functions, offering key insights for designing advanced hydrogen storage and optical materials.