Adsorption Of Hydrogen Molecules Research Articles

Flow-Induced Autonomic Ordering of Hydrogen Molecules under a Non-Equilibrium Flow.

A non-equilibrium molecular flow through a carbon nanotube (CNT) serves as a key system for revealing molecular transport and establishing nanofluidics. It has been challenging to simulate a non-equilibrium flow of hydrogen molecules exhibiting strong nuclear quantumness. Taking advantage of the quantum molecular dynamics method that can calculate real-time trajectories of hydrogen molecules even under a non-equilibrium flow, we found that the non-equilibrium flow makes hydrogen molecules more condensed and accelerates their adsorption near a CNT surface, letting the molecules flow more smoothly by propagating velocity momenta more efficiently along the CNT axis and by suppressing transverse molecular dynamics on the CNT cross section. Such flow-induced autonomic ordering indicates the importance of monitoring and investigating dynamics and adsorption of hydrogen molecules under a non-equilibrium circumstance as well as in a quiet equilibrium state, opening a new strategy for efficient hydrogen liquefaction and storage.

Y decorated all-boron B38 nanocluster for reversible molecular hydrogen storage: A first-principles investigation

Using first-principles calculations, the adsorption and storage of hydrogen molecules on Y decorated B 38 fullerene (Y 4 @B 38 ) are investigated. It is shown that Y atoms strongly attach to the hexagon cavities of B 38 , and that isolated Y atoms on B 38 are energetically more stable than the Y 4 cluster, hence avoiding the aggregation issue. Moreover, Y 4 @B 38 weakly interact with each other to build larger clusters. Polarization effects, as well as the Kubas mechanism, play essential roles in H 2 adsorption and storage on Y 4 @B 38 . The adsorption energy per H 2 molecule on Y 4 @B 38 ranges from −0.180 to −0.249 eV, which is within the recommended range for an optimal H 2 storage material. Each Y atom in Y 4 @B 38 may hold up to six H 2 molecules, corresponding to a gravimetric density of 4.96%. The stability of H 2 adsorbed structures and its dependence on temperature and pressure are evaluated using the modified van't Hoff equation. • Y atoms are strongly adsorbed on the hexagon cavities of B 38 . • The gravimetric density of hydrogen molecules on Y 4 @B 38 is 4.96%. • The effects of temperature and pressure are studied by the modified van't Hoff equation. • Clustering of Y 4 @B 38 fullerenes has a minor influence on H 2 storage capacity.

Enhancement in hydrogen storage capabilities of Cr, Mo, and W-embedded graphitic carbon nitride nanosheets: A DFT investigation

Hydrogen molecules (HMs) adsorption on W, Mo, and Cr-modified heptazine graphitic carbon nitride (hg-C3N4) were investigated using first-principle computations. The results displayed that with the modification of the hg-C3N4 system by W, Mo, and Cr elements, the adsorption capacities of hg-C3N4 to HMs significantly increased. The results revealed that the adsorption energy (Eads) of HMs on the W-modified hg-C3N4 (Eads = -2.616 eV) is remarkably negative than those of the other reported adsorbents. Based on the adsorption energy results, it can be inferred that the maximum storage number of adsorbed H2 on the modified hg-C3N4 systems are six molecules. Additionally, the results showed that the binding energy between Nedge and W elements of W-modified hg-C3N4 is more negative than those of the Cr and Mo-modified materials. Also, it was found that with adsorption of HMs on the modified hg-C3N4 systems, the electrical conductivity, relaxed structures, and magnetic moments substantially modulated thanks to the protruding structure of hg-C3N4 and also the charge transfer between HMs and modified hg-C3N4. Furthermore, the partial density of states and the electronic band structures were computed to realize the interactions and electron transfer among the constituent elements. The results illustrated that with adsorption of HMs on the hg-C3N4, valence and conduction energy levels have crossed each other adjacent to the Fermi energy level, resulting in the formation of conductive materials. This research shows that the W-embedded hg-C3N4 could be a promising material to efficiently store hydrogen molecules.

Dissociative Adsorption of Hydrogen and Methane Molecules at High-Angle Grain Boundary of Pipeline Steels Studied by Density Functional Theory Modeling

Dissociative Adsorption of Hydrogen and Methane Molecules at High-Angle Grain Boundary of Pipeline Steels Studied by Density Functional Theory Modeling

A neural network potential for the IRMOF series and its application for thermal and mechanical behaviors.

Metal-organic frameworks (MOFs) with their exceptional porous and organized structures have been the subject of numerous applications. Predicting the bulk properties from atomistic simulations requires the most accurate force fields, which is still a major problem due to MOFs' hybrid structures governed by covalent, ionic and dispersion forces. Application of ab initio molecular dynamics to such large periodic systems is thus beyond the current computational power. Therefore, alternative strategies must be developed to reduce computational cost without losing reliability. In this work, we construct a generic neural network potential (NNP) for the isoreticular metal-organic framework (IRMOF) series trained by PBE-D4/def2-TZVP reference data of MOF fragments. We confirmed the success of the resulting NNP on both fragments and bulk MOF structures by prediction of properties such as equilibrium lattice constants, phonon density of states and linker orientation. The RMSE values of energy and force for the fragments are only 0.0017 eV atom-1 and 0.15 eV Å-1, respectively. The NNP predicted equilibrium lattice constants of bulk structures, even though not included in training, are off by only 0.2-2.4% from experimental results. Moreover, our fragment based NNP successfully predicts the phenylene ring torsional energy barrier, equilibrium bond distances and vibrational density of states of bulk MOFs. Furthermore, the NNP enables revealing the odd behaviors of selected MOFs such as the dual thermal expansion properties and the effect of mechanical strain on the adsorption of hydrogen and methane molecules. The NNP based molecular dynamics (MD) simulations suggest IRMOF-4 and IRMOF-7 to have positive-to-negative thermal expansion coefficients while the rest to have only negative thermal expansion at the studied temperatures of 200 K to 400 K. The deformation of the bulk structure by reduction of the unit cell volume has been shown to increase the volumetric methane uptake in IRMOF-1 but decrease the volumetric methane uptake in IRMOF-7 due to the steric hindrance. To the best of our knowledge, this study presents the first pre-trained model publicly available giving the opportunity for the researchers in the field to investigate different aspects of IRMOFs by performing large-scale simulation at the first-principles level of accuracy.

Upgrading the Hydrogen Storage of MOF-5 by Post-Synthetic Exchange with Divalent Metal Ions

In metal-organic frameworks (MOFs), mixed-metal clusters have the opportunity to adsorb hydrogen molecules due to a greater charge density of the metal. Such interactions may subsequently enhance the gravimetric uptake of hydrogen. However, only a few papers have explored the ability of mixed-metal MOFs to increase hydrogen uptake. The present work reveals the preparation of mixed metal metal-organic frameworks M-MOF-5 (where M = Ni2+, Co2+, and Fe2+) (where MOF-5 designates MOFs such as Zn2+ and 1,4-benzenedicarboxylic acid ligand) using the post-synthetic exchange (PSE) technique. Powder X-ray diffraction patterns and scanning electron microscopy images indicate the presence of crystalline phases after metal exchange, and the inductively coupled plasma–mass spectroscopy analysis confirmed the exchange of metals by means of the PSE technique. The nitrogen adsorption isotherms established the production of microporous M-MOF-5. Although the additional metal ions decreased the surface area, the exchanged materials displayed unique features in the gravimetric uptake of hydrogen. The parent MOF-5 and the metal exchanged materials (Ni-MOF-5, Co-MOF-5, and Fe-MOF-5) demonstrated hydrogen capacities of 1.46, 1.53, 1.53, and 0.99 wt.%, respectively. The metal-exchanged Ni-MOF-5 and Co-MOF-5 revealed slightly higher H2 uptake in comparison with MOF-5; however, the Fe-MOF-5 showed a decrease in uptake due to partial discrete complex formation (discrete complexes with one or more metal ions) with less crystalline nature. The Sips model was found to be excellent in describing the H2 adsorption isotherms with a correlation coefficient ≅ 1. The unique hydrogen uptakes of Ni− and Co-MOF-5 shown in this study pave the way for further improvement in hydrogen uptake.

Computational Study of Hydrogen Molecules Adsorption on Boron Nitride with/without Adopted by One of Elements from Group IV

In this study, we reported the adsorption of two hydrogen (H2) molecules on six boron nitride (BN) studied models with or without adopted by one of the elements from Group IV. By employing the computational method of density functional theory (DFT), the hydrogen binding energies and electronic structures were analyzed and discussed. The computed results presented that the most favorable adsorption sites were found for the two H2 molecules in all studied systems. The computed optimal binding energies of all BN studied systems were determined to be 0.01 eV – 0.05 eV per H2 molecule, which is smaller than that of the previous literature study. Moreover, the energies of HOMO–LUMOs were predicted in the range of 1.64 eV – 6.18 eV. For the surface plots of molecular electrostatic potentials (MEPs), the H atoms at the N–edges possess the most positive electrostatic potentials, while the negative electrostatic potentials fall in the atoms of H at the B–edges. A similar trend was presented on the distribution of atomic charge. Using the scheme of Mulliken population analysis (MPA), there are two different charge values on the atom of H in this study. The H atoms at the B–edges possess the negative charges, whereas the positive charge values were found on the atoms of H at the N–edges. In addition, the findings also noted that the positive charge values were presented for all B atoms in the study. While the negative charges fall in the atoms of N.

Reversible hydrogen storage on alkali metal (Li and Na) decorated C20 fullerene: A density functional study

This work reports the reversible hydrogen storage capacities of Li and Na decorated C20 fullerene using dispersion corrected density functional theory calculation. The alkali metal (AM) atoms are found to bind on the C–C bridge position of C20 through non-covalent closed-shell interaction. Their thermodynamic stabilities are verified through HOMO-LUMO gaps and different reactivity descriptors. Each Li and Na atoms decorated on C20 adsorb maximum up to five H2 molecules through Niu-Rao-Jena interaction. The adsorption energy decreases with successive addition of H2 molecules with average binding energy lying in the range of 0.12 eV–0.13 eV. The systems can have a maximum gravimetric density of 13.08 wt% and 10.82 wt% for C20Li4–20H2 and C20Na4–20H2 respectively. ADMP molecular dynamic simulations illustrate the reversibility of adsorbed hydrogen molecules at higher temperature (≧ 300 K). The calculated thermodynamic useable hydrogen capacity shows the room temperature H2 desorption condition of AM decorated C20. Consistent with criteria set by the US-DOE, C20Li4 and C20Na4 can be used as promising hydrogen storage materials.

Adsorption of hydrogen molecule on alkali metal-decorated hydrogen boride nanotubes: A DFT study

Adsorption of Li, Na, and K atom on surfaces of armchair (5,5) and zigzag (10,0) hydrogen boride nanotubes (HBNTs) was investigated using the periodic-DFT method. It was found that the average diameter (5,5) HBNT is shorter than the (10,0) HBNT by 1.246 Å and the (5,5) HBNT is more stable than the (10,0) HBNT by 0.991 eV. Adsorption strength of the (5,5) HBNT on alkali metals was found to be higher than the (10,0) HBNT. Adsorption abilities of H2 on the (5,5) HBNT and (5,5) HBNT are in the same order: Li > Na > K. The adsorption energies of H2 on Li-, Na-, and K-(5,5) HBNTs are −0.242, −0.165, and −0.121 eV, respectively, and on Li-, Na-, and K-(10,0) HBNTs are −0.277, −0.168, and −0.094 eV, respectively. The Li-HBNTs, Li-(5,5) HBNT, and (10,0) HBNT are the highest adsorption abilities on H2 adsorption and the most significant change of metal charges. Therefore, the Li-(5,5) HBNT and (10,0) HBNT used as H2 storage materials were suggested.

Adsorption of diatomic molecules on nitrogenated holey graphene: Theoretical insights

Physical adsorption of three diatomic molecules (H2, CO, and HF) on graphene and recently synthesized N-doped holey graphene (4N-graphene) has been studied by using a set of theoretical methods to reveal peculiarities of their non-covalent interactions. Adsorption of hydrogen molecules shows approximately doubled interaction energies (Eint) for 4N-graphene compared with pristine one. At the same time, the CO molecule also shows considerable enhancements in Eint values for physisorption on 4N-graphene. The most significant advantage can be observed for the HF molecule. We connect the nearly ten times enhancement with the occurrence of the tetrafurcated bond. Ab initio molecular dynamics simulations witness that at T=77 K, CO and HF molecules remain at the position nearly the pore during the whole course of simulation. It confirms the potential usage of 4N-graphene as a candidate for gas storage. The present work, which observes the prospective model system, can propose a simple way of describing the complicated events that occur in doped pore regions of graphene-based adsorbents.

Hydrogen molecule adsorption on pristine and selected‐elements (periods 2‐4)‐doped armchair (5,5) and zigzag (10,0) beryllium oxide nanotubes as hydrogen storage materials

The electronic properties of armchair (5,5) beryllium oxide nanotube (BeONT), zigzag (10,0) BeONT, and their surfaces doped by the selected elements of periods 2 (B, C, and N), 3 (Mg, Al, Si, P, and S), and 4 (Ca, Ga, Ge, As, and Se), and their hydrogen molecule adsorptions were studied using periodic density functional theory-D method. The C(O)- and Ge(O)-(5,5) BeONTs, C(O)-, Si(O)-, and Ge(O)-(10,0) BeONTs were suggested to be new hydrogen molecule sensing materials based on the electrical resistivity measurement. The C(O)-, Si(O)-, and Ge(O)-doped (5,5) BeONTs, and C(O)- and Si(O)-doped (10,0) BeONTs were suggested to be utilized as hydrogen storage materials.

Ultra-high capacity of physisorption of hydrogen molecule on AlC3 monolayer: First-principles calculations

In this research, we have investigated through the first principal calculations the adsorption of hydrogen molecule on AlC3 monolayer. In the beginning, we determined the most stable positions of hydrogen molecule adsorption on AlC3 substrate. The calculations indicate that the position of greatest stability is in the center of the carbon atom hexagon when the hydrogen molecule is placed perpendicularly on AlC3 surface, and the adsorption energy Eads is near to −0,2189 eV, where the most stable distance is 2.50 Å. The hydrogen molecule adsorption at various positions on AlC3 surface maintains its semiconducting character. The examination of the diffusion paths between the various sites indicates an ability of the hydrogen molecule to migrate between the sites, which are spaced by a slight energy barrier of 0.0163 eV. It is shown that AlC3 monolayer possess the ability to adsorb 16 hydrogen molecules, with 11.8 wt% as gravimetric capacity, as well as a desorption temperature of 173.35 K. Based on the findings, the AlC3 monolayer may be a promising candidate for hydrogen storage.

Hydrogen molecule capacity physisorption on BC3 monolayer: First-principles calculations

In this investigation, we studied the hydrogen molecule adsorption on the BC3 sheet via first-principles calculations. First, we have identified the most stable sites of hydrogen molecule adsorption on the BC3 surface. It is estimated from the calculations that the most stable site is located in the center of the hexagon of carbon atoms where the hydrogen molecule is positioned vertically above BC3 sheet, as well as the adsorption energy Eads is about −7.2642 kcal mol−1, whereas the 3.10 Å is the closest stable distance. The density of state calculation shows that upon adsorption of H2 molecules onto the BC3 surface, it keeps its semiconducting behavior with both methods the Marzarie Vanderbilt and the Tetrahedron method. An investigation of the migration paths between the different positions shows a capability of hydrogen molecule to diffuse between the positions, separated by a small barrier of energy amounting to 2.25 meV. The BC3 sheet is demonstrated to possess the capability of adsorbing 11 hydrogen molecules, with a gravimetric capacity of 10.51 wt%, with a desorption temperature of 205.33 K. According to the above results, the BC3 sheet can be a very interesting prospect for hydrogen storage.

Thermodynamics of spontaneous dissociation and dissociative adsorption of hydrogen molecules and hydrogen atom adsorption and absorption on steel under pipelining conditions

While hydrogen pipelines have attracted increased attention, safety of the pipelines has been a concern in terms of hydrogen embrittlement (HE) occurring upon hydrogen atom (H) generation and permeation in the steels. In this work, thermodynamic analyses regarding H generation and adsorption on pipeline steels by two potential mechanisms, i.e., spontaneous dissociation and dissociative adsorption, were conducted through theoretical calculations based on Gibbs free energy change of the H generation reactions. Moreover, H adsorption free energy and configurations were determined based on density functional theory (DFT) calculations. Effects of H adsorption site, H coverage and hydrostatic stress on H adsorption and absorption were discussed. Spontaneous dissociation of hydrogen gas molecules to generate hydrogen atoms is thermodynamically impossible. Dissociative adsorption is thermodynamically feasible at wide temperature and pressure ranges. Particularly, an increased hydrogen gas partial pressure and elevated temperature favor the dissociative adsorption of hydrogen. Hydrogen atoms generated by dissociative adsorption mechanism can adsorb stably at On-Top (OT) and 2-fold (2F) Cross-Bridge sites of Fe (100), while hydrogen adsorption at 2F site is more stable due to a higher electron density and a stronger electronic hybridization between Fe and H. The influence of H atom coverage on dissociative adsorption occurs at low coverages only, i.e., 0.25–1.00 ML as determined in this work. External stresses make dissociative adsorption more difficult to occur compared with a fully relaxed steel. Both tetrahedral sites (TS) and octahedral sites (OS) can potentially host absorbed H atoms at subsurface of the steel. Absorbed H atoms will be predominantly trapped at TS due to a low energy path and exothermic feature. Diffusion of H atoms from steel surface to the subsurface is more difficult compared with the dissociative adsorption.

A DFT study on the outstanding hydrogen storage performance of the Ti-decorated MoS2 monolayer

The hydrogen storage performances of the pure MoS2 monolayer and the one decorated with Ti atoms were studied via the first-principles DFT calculations. The Ti atom was calculated to be successfully and chemically decorated on the surface of MoS2 monolayer with a large binding energy of -4.979 eV, the absolute value of which was higher than the cohesive energy of Ti bulk (4.85 eV). The hydrogen molecule interacted weakly with the pure MoS2 with a low adsorption energy of only -0.0226 eV but was strongly adsorbed on the introduced active site of the Ti atom in the decorated MoS2 with an improved adsorption energy of -0.472 eV. There were four hydrogen molecules in maximum stored on the modified MoS2 monolayer via chemical interactions with an average adsorption energy being -0.413 eV. Moreover, the adsorbed hydrogen molecules released 1.29 e to the substrate of decorated MoS2 during the storage process. The stored hydrogen molecules of the MoS2 decorated with two Ti atoms were further improved to be eight with transferred charges being 2.42 e. Finally, the gravimetric density of hydrogen storage of the Ti-decorated MoS2 with a full coverage being 1 on its both sides could be enhanced to be as high as 5.93 wt%, well meeting the criteria of the United States Department of Energy. Our research indicates that the MoS2 monolayer decorated with Ti atoms is promising to effectively store the hydrogen molecules and is potentially applied as an excellent hydrogen gas sensor.

Computational insights of alkali metal (Li / Na / K) atom decorated buckled bismuthene for hydrogen storage

The mechanism of hydrogen molecule adsorption on 2D buckled bismuthene (b-Bi) monolayer decorated with alkali metal atoms was studied using density functional theory based first principles calculations. The decorated atoms Li, Na and K exhibited distribution on surface of b-Bi monolayer with increasing binding energy of 2.6 eV, 2.9 eV and 3.6 eV respectively. The adsorption of H2 molecule on the slabs appeared stable which was further improved upon inclusion of van der Waals interactions. The adsorption behaviour of H2 molecules on the decorated slabs is physisorption whereas the slabs were able to bind up to five H2 molecules. The average adsorption energy per H2 molecules are in range of 0.1–0.2 eV which is good for practical applications. The molecular dynamics simulation also confirmed the thermodynamic stabilities of five H2 molecules adsorbed on the decorated slabs. The storage capacity values are found 2.24 wt %, 2.1 wt %, and 2 wt %, for respective cases of Li, Na and K atoms decorated b-Bi. The analysis of the adsorbed cases pointed to electrostatic interaction of Li and H2 molecule. The adsorption energies, binding energies, charge analysis, structural stability, density of states, and hydrogen adsorption percentage specifies that the decorated b-Bi may serve as an efficient hydrogen storage material and could be an effective medium to interact with hydrogen molecules at room temperature.

The effect of Na addition on the first hydrogen absorption kinetics of cast hypoeutectic Mg–La alloys

With superior properties of Mg such as high hydrogen storage capacity (7.6 wt% H/MgH2), low price, and low density, Mg has been widely studied as a promising candidate for solid-state hydrogen storage systems. However, a harsh activation procedure, slow hydrogenation/dehydrogenation process, and a high temperature for dehydrogenation prevent the use of Mg-based metal hydrides for practical applications. For these reasons, Mg-based alloys for hydrogen storage systems are generally alloyed with other elements to improve hydrogen sorption properties. In this article, we have added Na to cast Mg–La alloys and achieved a significant improvement in hydrogen absorption kinetics during the first activation cycle. The role of Na in Mg–La has been discussed based on the findings from microstructural observations, crystallography, and first principles calculations based on density functional theory. From our results in this study, we have found that the Na doped surface of Mg–La alloy systems have a lower adsorption energy for H2 compared to Na-free surfaces which facilitates adsorption and dissociation of hydrogen molecules leading to improvement of absorption kinetic. The effect of Na on the microstructure of these alloys, such as eutectic refinement and a density of twins is not highly correlated with absorption kinetics.

Hydrogen adsorption on metal‐functionalized benzene and B‐substituted benzene

Hydrogen storage properties of metal doped benzene complexes vary with positions of boron atom substitution in a benzene ring at MP2/6-311++g(d,p) level. Two carbon atoms of a benzene (C6H6) ring positioned at 1-2, 1-3 and 1-4 are replaced by two boron atoms and the structures named as BB1-2, BB1-3 and BB1-4, respectively. Further, pristine as well as boron substituted benzene complexes are decorated with Li, Be,Ti and Ca atoms. C6H6Li, BB1-2Li, BB1-3Li and BB1-4Li complexes can interact with three, three, two and three H2 molecules, respectively, with 6.64, 6.82, 4.65 and 6.82 wt% H2 uptake capacities. Only one H2 molecule gets adsorbed on each C6H6Be, BB1-2Be, BB1-3Be and BB1-4Be complexes with respective H2 uptake capacity of 2.26, 2.32, 2.32 and 2.32 wt%. One additional hydrogen molecule gets adsorbed on Ti(Ca) decorated boron substituted benzene than C6H6Ti(C6H6Ca) with respective H2 uptake capacity 7.54(7.98) and 6.02(9.46) wt%. Electron density of metal atom gets altered significantly after adsorption of H2 molecules. The averaged H2 adsorption energies with Gibbs free energy correction ΔEG are found to be negative for all Li- and Ca-doped complexes indicates thermodynamically unfavorable H2 adsorption where ΔEG values are positive for all Ti- and Be-doped complexes at room temperature indicating thermodynamically favorable H2 adsorption. Interaction between H2 molecules and Be- as well as Ti-doped complexes is found to be stronger than Li- and Ca-doped complexes. Be-doped complexes considered do not satisfy the target set by DOE regarding H2 uptake capacity. Boron substitution improves molecular hydrogen uptake of Benzene-Ti complex by 1.52 wt% and satisfy the target set by DOE. C6H6Li, BB1-2Li, BB1-3Li and BB1-4Li complexes cannot be used for hydrogen storage since hydrogen adsorption on these complexes is endothermic. Ti-doped boron substituted complexes are found to more promising H2 storage material because of their higher H2 uptake capacity as well as their strong interaction with adsorbed hydrogen molecules than Li-, Be- and Ca-doped complexes.

Enhancement of hydrogen storage properties of metal-organic framework-5 by substitution (Zn, Cd and Mg) and decoration (Li, Be and Na)

Two strategies of decoration by three elements Z = Li, Be and Na in cyclic site, and substitution of Zn by Mg and Cd in unit cell were used in the framework of functional density theory to tune the hydrogen storage properties of metal-organic framework-5 (MOF-5) based on Zn whose decomposition temperature and initial gravimetric capacity are 300 K and 1.57 wt% respectively.Based on the adsorption of hydrogen molecules in the crystal surface at three different adsorption sites with three orientations of H2, we show that our system may reach a maximum gravimetric storage capacity of 4.09 wt% for multiple hydrogen molecules. Moreover, the functionalization of Z combined to the substitution, shows an exceptional improvement of hydrogen storage properties. For example, Mg-MOF-5 decorated with Li2 has a capacity up to 5.41 wt% and 513 K as desorption temperature.

Hydrogen adsorption on pillar[6]arene: A computational study

Abstract A systematical theoretical work on physisorption of H2 molecules by both pristine and Li+-decorated per-hydroxylated pillar[6]arene (PPA ) in the gas phase has been performed by using density functional theory (DFT) and 0th order symmetry-adapted perturbation theory calculations (SAPT0). A complementary analysis using ab initio molecular dynamics (AIMD), atoms-in-molecules (AIM) and independent gradient model (IGM) methods has also been done. Our calculations have shown that H2 molecules can be adsorbed favorably inside the PPA hollow compared with pristine graphene. However, the obtained magnitudes of adsorption energy (Ead ) fall outside the optimal range of energies for hydrogen storage . On the other hand, Li + decoration has drastically improved both Ead and quantity of adsorbed hydrogen molecules. It has been established that each cation center is capable of uptaking from one to five H2 molecules per Li+, and their Ead are in the range from −3.57 to −5.40 kcal/mol. SAPT0 calculations have indicated the prevalence of London dispersion or induction forces in the cases of adsorption inside PPA hollows and on Li+, respectively. AIM and IGM analyses have exhibited that a non-covalent bonding exists between Li+ and H2, and the adsorbed H2 molecules are undissociated. AIMD simulations allow estimating gravimetric densities (GD) at various temperatures, and the maximal GD have been calculated to be 6.0, 4.8, and 3.8% at T = 77, 233, and 300 K, respectively. Besides this, AIMD calculations validate stability of studied structures and the quantity of hydrogen adsorbed. We believe that some of the considerations derived herein establish the high potential of the studied PPA models for hydrogen storage.