Bond Contraction Research Articles

An X‐Ray Absorption Spectroscopy Investigation into the Fundamental Structure of Liquid Metal Alloys

Gallium and gallium alloys have gained significant interest due to gallium's low melting point. This property allows for gallium‐based catalysts to take advantage of the unique reaction environments only available in the liquid state. While understanding of the catalytic properties of liquid metals is emerging, a comprehensive investigation into the fundamental structures of these materials has yet to be undertaken. Herein, the structure of liquid gallium, along with related liquid alloys EGaIn, EGaSn, and Galinstan are explored using X‐ray absorption spectroscopy (XAS). In contrast to some other studies that show dimers, analysis of the XAS data both in X‐ray absorption near edge structure and extended X‐ray absorption fine structure shows that when fully dissolved the materials are largely homogenous with no obvious signs of local structures. Ga shows a bond contraction when melted which is consistent with its increase in density; however, an expansion in bond length is observed when alloyed with In and Sn. XAS data indicate that the effective nuclear charge (Zeff) of In and Sn follows the trend expected based on electronegativity. Molecular dynamic (MD) simulations are performed to simulate the structure and trends between MD and XAS; the trends agree well but MD overestimates bond lengths.

Investigation of the H2 dissociation and strengthening mechanism in vacancy-induced graphene

Atomic vacancies play a crucial role in hydrogen storage and local strengthening of a substance with a mechanism that is elusive. First-principles examinations of monolayer graphene unveiled the following: (i) the neighboring carbon atoms move radially away from the vacancy center with a 3–10% C–C bond contraction, generating a circumferential density ribbon of energy and electrons; (ii) the dense electrons within the ribbon polarize the edge atoms into dipoles pointing to the center; (iii) the polarized electrons coupled together to for the vacancy dipole, resulting in the Dirac-Fermion resonant peak at Fermi energy and the energy density gai raise the local strength; and (iv) the vacancy dipole induces the adsorbed H2 molecule into H+-H- dipole to stabilize H2 adsorption. The findings of vacancy reinforcement, dipole formation, and stable H2 adsorption should provide a promising mechanism contributing to the advancement of hydrogen storage theory.

Synthesis of polyhedral Pt-Pd-Ni nanobelts regulated by W(CO)6 and applied as a highly performing oxygen reduction reaction electrocatalyst

Pt-Pd-Ni polyhedral nanobelt (PNBs) composite catalysts are synthesized in presence of tungsten hexacarbonyl [W(CO)6] by a simple solvothermal method, combining both higher specific surface area and more index active site than the corresponding single-structure catalysts. The thermal decomposition of W(CO)6 plays a crucial role in the morphology formation. The tenuous composite with a moderate nanobelt width of 7.46 nm formed after heating for 6 h (Pt-Pd-Ni PNBs2) shows better ORR performance and durability than the ternary (Pt-Pd-Ni) and binary (Pt-Pd) single structures. It exhibits a mass activity of 1.49 (A mgPt−1), which only degrades by about 10.63 % after 50,000 durability cycles. The metal regulatory effects induced by the carbonyl compounds cause the contraction of the Pt-Pt bonds. Density functional theory calculations indicate that the compressive strain of Pt-Pd-Ni PNBs2 leads to a decrease in the d-band center and overpotential negatively shifted, thus provide a more sufficient and faster ORR proceeding process in thermodynamics, facilitating a higher energy conversion efficiency.

Probing the Long- and Short-Range Structural Chemistry in the C-Type Bixbyite Oxides Th0.40Nd0.48Ce0.12O1.76, Th0.47Nd0.43Ce0.10O1.785, and Th0.45Nd0.37Ce0.18O1.815 via Synchrotron X-ray Diffraction and Absorption Spectroscopy.

The long- and short-range structural chemistry of the C-type bixbyite compounds Th0.40Nd0.48Ce0.12O1.76, Th0.47Nd0.43Ce0.10O1.785, and Th0.45Nd0.37Ce0.18O1.815 is systematically examined using synchrotron X-ray powder diffraction (S-PXRD), high-energy resolution fluorescence detection X-ray absorption near edge (HERFD-XANES), and extended X-ray absorption fine structure spectroscopy (EXAFS) measurements supported by electronic structure calculations. S-PXRD measurements revealed that the title compounds all form classical C-type bixbyite structures in space group Ia3̅ that have disordered cationic crystallographic sites with further observation of characteristic superlattice reflections corresponding to oxygen vacancies. Despite the occurrence of oxygen vacancies, HERFD-XANES measurements on the Ce L3-edge revealed that Ce incorporates as Ce4+ into the structures but involves local distortion that resembles cluster behavior and loss of nearest-neighbors. In comparison, HERFD-XANES measurements on the Nd L3-edge supported by electronic structure calculations reveal that Nd3+ adopts a local coordination environment similar to the long-range C-type structure while providing charge balancing for the formation of oxygen defects. Th L3-edge EXAFS analysis reveals shorter average Th-O distances in the title compounds in comparison to pristine ThO2 in addition to shorter Th-O and Th-Ce distances compared to Th-Th or Ce-Ce in the corresponding F-type binary oxides (ThO2 and CeO2). These distances are further found to decrease with the increased Nd content of the structures despite simultaneous observation of the overall lattice structure progressively expanding. Linear combination calculations of the M-O bond lengths are used to help explain these observations, where the role of oxygen defects, via Nd3+ incorporation, induces local bond contraction and enhanced Th cation valence, leading to the observed increased lattice expansion with progressive Nd3+ incorporation. Overall, the investigation points to the significance of dissimilar cations exhibiting variable short-range chemical behavior and how it can affect the long-range structural chemistry of complex oxides.

Deciphering Charge Transfer Processes in Transition Metal Complexes from the Perspective of Ultrafast Electronic and Nuclear Motions.

Chemical transformations in charge transfer states result from the interplay between electronic dynamics and nuclear reorganization along excited-state trajectories. Here, we investigate the ultrafast structural dynamics following photoinduced electron transfer from the metal-metal-to-ligand charge transfer state of an electron donor, a Pt dimer complex, to a covalently linked electron acceptor group using ultrafast time-resolved wide-angle X-ray scattering and optical transient absorption spectroscopy methods to disentangle the interdependence of the excited-state electronic and nuclear dynamics. Following photoexcitation, Pt-Pt bond formation and contraction takes up to 1 ps, much slower than the corresponding process in analogous complexes without electron acceptor groups. Because the Pt-Pt distance change is slow with respect to excited-state electron transfer, it can affect the rate of electron transfer. These results have potential impacts on controlling electron transfer rates via structural alterations to the electron donor group, tuning the charge transfer driving force.

Thermonanomechanics of graphene oxide-M13 bacteriophage nanocomposites -towards graphene-based nanodevices

The self-assembly of graphene oxide (GO) and M13 bacteriophage results in the formation of micro-porous structures, known as GraPhage13 aerogels (GPA). Given the limited applications of aerogels in industry due to their nanomechanical properties, along with the previously observed temperature-dependent characteristics in graphene-based nanocomposites, a thorough exploration of the thermosensitive nanomechanical properties of GPA is essential. Herein, a comprehensive characterisation of the morphology, composition, and spectroscopic analysis of the GPA for a range of temperatures has been conducted and correlated with its nanomechanical properties. Elevated temperatures have been found to lead to gradual removal of oxygen-containing functional groups (OCFGs) from GPA, resulting in increased structural defects and reduced stiffness. Notably, unique nanomechanical behaviours of GPA have been further identified, where the thermal expansion of sp3 bonds exceeds that of a crystalline sp3 structure, while the thermal contraction of sp2 bonds in GPA is found to be between graphite and GO. This underscores the impact of GO functionalisation on the thermal expansion behaviour of GPA. The obtained insights enhance the overall comprehension of the temperature annealing impact on GPA and highlight the tunability of its nanomechanical properties, showcasing a broad potential of this novel nanocomposite across a diverse range of applications.

Compressive reactive molecular dynamics on mechanical and structural behaviors of geopolymers: Imposing lateral constraints and varied temperatures

Geopolymer concrete offers superior mechanical properties and microstructure, yet micro-level compressive properties and structural evolutions remain insufficiently understood. This study employed molecular dynamics to simulate the uniaxial compressions of the sodium aluminosilicate hydrate (N-A-S-H) under UCZ, BCZ, and TCZ (z-axial compressions with zero, one, and two dimensions restrictions, respectively) conditions at 263 K, 300 K, and 800 K. The results provided valuable insights linking mechanical behavior with structural properties. Stress fluctuations in the yield stage were attributed to the continuous formation and fracture of Al-O-H bonds during micro-molecule processes. In the later compression stages, the rapid increase in Si-O-H groups suggested that water molecules equally attacked Al and Si tetrahedra due to limited voids. Under UCZ and BCZ conditions, slight bond contraction occurred, with the main structural resistance arising from bond angle bending within the skeleton. In contrast, TCZ experienced notable changes in both bond lengths and bond angles due to bilateral displacement constraints. The evolutionary molecular processes exhibited insensitive response to the temperature, especially under TCZ conditions. Additionally, varying trends were observed in different bond-angle styles (e.g., within or inside tetrahedra), providing a crucial insight for the design of N-A-S-H to determine optimal components.

Role of Fe decoration on the oxygen evolving state of Co3O4 nanocatalysts.

The production of green hydrogen through alkaline water electrolysis is the key technology for the future carbon-neutral industry. Nanocrystalline Co3O4 catalysts are highly promising electrocatalysts for the oxygen evolution reaction and their activity strongly benefits from Fe surface decoration. However, limited knowledge of decisive catalyst motifs at the atomic level during oxygen evolution prevents their knowledge-driven optimization. Here, we employ a variety of operando spectroscopic methods to unveil how Fe decoration increases the catalytic activity of Co3O4 nanocatalysts as well as steer the (near-surface) active state formation. Our study shows a link of the termination-dependent Fe decoration to the activity enhancement and a significantly stronger Co3O4 near-surface (structural) adaptation under the reaction conditions. The near-surface Fe- and Co-O species accumulate an oxidative charge and undergo a reversible bond contraction during the catalytic process. Moreover, our work demonstrates the importance of low coordination surface sites on the Co3O4 host to ensure an efficient Fe-induced activity enhancement, providing another puzzle piece to facilitate optimized catalyst design.

Metal-Ligand Redox Cooperativity in Cerium Amine-/Amido-Phenolate-Type Complexes.

The synthesis and characterization of two cerium complexes of redox-active amine/amido-phenolate-type ligands are reported. A tripodal framework comprising the tris(2-(3',5'-di-tert-butyl-2'-hydroxyphenyl)amino-phenyl) amine (H6Clamp) proligand was synthesized for comparison of its cerium complex with a potassium-cerium heterobimetallic complex of the 4,6-di-tert-butyl-2-[(2,6-diisopropylphenyl)imino]quinone (dippap) proligand. Structural studies indicate differences in the cerium(III) cation coordination spheres, where CeIII(CH3CN)1.5(H3Clamp) (1-Ce(H3Clamp)) exhibits shorter Ce-O distances and longer Ce-N bond distances compared to the analogous distances in K3(THF)3CeIII(dippap)3 (2-Ce(ap)), due to the gross structural differences between the systems. Differences are also evident in the temperature-dependent magnetic properties, where smaller χT products were observed for 2-Ce(ap) compared to 1-Ce(H3Clamp). Solution electrochemical studies for the complexes were interpreted based on ligand- and metal-based oxidation events, and the cerium(III) oxidation of 2-Ce(ap) was observed to be more facile than that of 1-Ce(H3Clamp), behavior that was cautiously attributed to the rigidity of the encrypted 1-Ce(H3Clamp) complex compared to the heterobimetallic framework of 2-Ce(ap). These results contribute to the understanding of how ligand designs can promote facile redox cycling for cerium complexes of redox-active ligands, given the large contraction of cerium-ligand bonds upon oxidation.

Relation between Halogen Bond Strength and IR and NMR Spectroscopic Markers.

The relationship between the strength of a halogen bond (XB) and various IR and NMR spectroscopic quantities is assessed through DFT calculations. Three different Lewis acids place a Br or I atom on a phenyl ring; each is paired with a collection of N and O bases of varying electron donor power. The weakest of the XBs display a C-X bond contraction coupled with a blue shift in the associated frequency, whereas the reverse trends occur for the stronger bonds. The best correlations with the XB interaction energy are observed with the NMR shielding of the C atom directly bonded to X and the coupling constants involving the C-X bond and the C-H/F bond that lies ortho to the X substituent, but these correlations are not accurate enough for the quantitative assessment of energy. These correlations tend to improve as the Lewis acid becomes more potent, which makes for a wider range of XB strengths.

Jahn-Teller distortion in bis(terpyridine)nickel(III) – Elongation or compression?

DFT methods were used to evaluate the type of Jahn-Teller distortion in the low spin d7 bis(terpyridine)nickel(III) doublet. The strain of the tridentate terpyridine ligand in bis(terpyridine)nickel(III) leads to longer Ni(III)-N terminal bond lengths than the Ni(III)-N central bonds. In addition, in all DFT optimized bis(terpyridine)nickel(III) molecules, the one set of Ni(III)-N terminal bonds are longer than the other set of Ni(III)-N terminal bonds. Three pairs of Ni(III)-N bonds are present in bis(terpyridine)nickel(III), namely 2 longer Ni(III)-Nterminal1 terminal bonds, 2 medium length Ni(III)-Nterminal2 terminal bonds and 2 shorter Ni(III)-Ncentral central bonds, similar to orthorhombic Jahn-Teller distortion in octahedral complexes. Evaluation of bond length differences, contraction of bonds, spin density plots and the character of the singly occupied molecular orbital (SOMO) and singly unoccupied molecular orbital (SUMO), led to a set of criteria to consider in evaluating the type of Jahn-Teller distortion in the low spin d7 bis(terpyridine)nickel(III) doublet. Jahn-Teller distortion can lead to elongation (z-out) or compression (z-in) of a pair of opposite Ni-N bonds. One key criteria found, is, if the difference in bond length between Ni(III)-Nterminal1 and Ni(III)-Nterminal2 is smaller than the difference in bond length of Ni(III)-Nterminal2 and Ni(III)-Ncentral, then it is a Jahn-Teller compression geometry (and vice versa for a Jahn-Teller elongation geometry).

Constructing Active Cu2+-O-Fe3+ Sites at the CuO-Fe3O4 Interface to Promote Activation of Surface Lattice Oxygen.

Activating surface lattice oxygen (Olatt) through the modulation of metal-oxygen bond strength has proven to be an effective route for facilitating the catalytic degradation of volatile organic compounds (VOCs). Although this strategy has been implemented via the construction of the TM1-O-TM2 (TM represents a transition metal) structure in various reactions, the underlying principle requires exploration when using different TMs. Herein, the Cu2+-O-Fe3+ structure was created by developing CuO-Fe3O4 composites with enhanced interfacial effect, which exhibited superior catalytic activity to their counterparts, with T90 (the temperature of toluene conversion reaching 90%) decreasing by approximately 50 °C. Structural analyses and theoretical calculations demonstrated that the active Cu2+-O-Fe3+ sites at the CuO-Fe3O4 interface improved low-temperature reducibility and oxygen species activity. Particularly, X-ray absorption fine structure spectroscopy revealed the contraction and expansion of Cu-O and Fe-O bonds, respectively, which were responsible for the activation of the surface Olatt. A mechanistic study revealed that toluene can be oxidized by rapid dehydrogenation of methyl assisted by the highly active surface Olatt and subsequently undergo ring-opening and deep mineralization into CO2 following the Mars-van Krevelen mechanism. This study provided a novel strategy to explore interface-enhanced TM catalysts for efficient surface Olatt activation and VOCs abatement.

Discriminative Mechanical and Thermal Response of the H-N Bonds for the Energetic LLM-105 Molecular Assembly.

Molecular interactions in energetic materials form the key not only to the "structure stability, energy storage, ignition, and detonation" dynamics but also to the sensitivity to the loading of perturbation and the power intensity of radiation for the energetic substance, with the nature of the interactions remaining elusive. With the aid of perturbative Raman spectroscopy and the pressure-resolved density functional theory, we uncovered that the H-N bond of the intermolecular O:H-N bonds for LLM-105 shares the same negative compressibility and thermal expansivity of the H-O bond for the coupling O:H-O bond of water [Phys. Rep. 2023, 998, 1-68]. In contrast, the dangling H-N bond vibrating at a 3440 cm-1 high frequency does otherwise due to the absence of coupling interaction and the undercoordination-driven bond contraction. These findings should deepen our insight into interactions involving electron lone pairs and offer an efficient means for discriminating the performance of individual bonds.

Investigating the temperature and frequency dependence of dielectric response using AC impedance spectroscopy on SnO2

In this investigation, we explored tin oxide's dielectric properties and impedance spectroscopy, focusing on its temperature dependence across a frequency range of 20 Hz to 2 MHz. We analyzed the x-ray diffraction pattern using Rietveld refinement and established that the sample has a tetragonal phase with P42/mnm space group. Afterward, the surface structure of the SnO2 was examined using (FESEM) and Raman spectroscopy. Through FESEM, we analyzed the morphology of the prepared sample, which were nanospheres in structure. In contrast, we discovered the non-degenerated A1g and B2g modes through Raman spectroscopy, which matches well with the literature and displays the contraction and expansion of Sn-O bonds. We performed dielectric studies at varying frequencies and temperatures to further analyze the properties. We discovered that the ac conductivity increased as temperature and frequency increased. The activation energy was calculated using dc electrical conductivity measurement. The DC conductivity exhibits a temperature dependence that can be described by the Arrhenius equation, which reveals that the tin oxide has to conduct behavior with an estimated activation energy of 0.025 eV, 0.035 eV, and 0.082 eV for three temperature ranges of 80–120 K, 120–175 K, and 175–270 K, respectively. Additionally, the AC conductivity data conforms to Jonscher's universal power law. The frequency-dependent parameter “s” increases as the temperature elevates. A transition from the QMT (Quantum mechanical tunneling) model to NSPT (non-overlapping small polaron tunneling) was employed to analyze the data.

(Invited) Size, Composition Effects and Active State Formation of Nanostructured Cobalt and Iron-Cobalt Oxide-Based Catalysts during Oxygen Evolution Reaction

The efficient water electrolysis is a key technology to establish a CO2-neutral, electrochemical (green) hydrogen production. Nonetheless, the electrocatalysts’ near-surface structure during the anodic oxygen evolution reaction (OER) is still largely unknown, which hampers knowledge-driven optimization. Here, we provide quantitative near-surface structural insights into oxygen-evolving CoOX(OH)Y nanoparticles by tracking their size-dependent catalytic activity down to 1 nm and their structural adaptation to OER conditions combining operando X-ray absorption spectroscopy and density functional theory calculations. We uncover a superior intrinsic OER activity of sub-5 nm nanoparticles and a size-dependent oxidation leading to a near-surface Co-O bond contraction and charge redistribution during OER.I will also report on the role of Fe in the performance of Co-oxide-based electrocalysts. By comparing epitaxial Co3O4(111), Co1+δFe2-δO4(111) (|δ|<=0.2), and Fe3O4(111) thin film electrocatalysts combining quasi in-situ preparation and characterization in ultra-high vacuum (UHV) with electrochemistry experiments. Interestingly, Co1+δFe2-δ O4(111) was found to be up to five times more active than Co3O4(111) and Fe3O4(111) with the activity depending acutely on the Co/Fe concentration ratio. Under OER conditions, all three oxides are covered by oxyhydroxide but the characteristics of this overlayer, including its thickness, stability, structural and chemical evolution was found to depend on the Fe content.

Asymmetrically examining the impact of green finance and renewable energy consumption on environmental degradation and renewable energy investment: The impact of the COVID-19 outbreak on the Chinese economy

The recent global recession due to Covid-19 has led to a drop in natural resource prices, which has contracted energy demand. Amid this concern, environmentally sustainable renewable energy projects have become uncompetitive and an obstacle to achieving the Sustainable Development Goals (SDGs). Following the nonlinear autoregressive distributed lag (NARDL) model proposed by Shin et al. (2014), to asymmetrically explore the impact of green bonds on renewable energy investment and environmental pollution and the impact of renewable energy consumption on environmental degradation in China over the period 1970–2020.​ The results show that the expansion of green bonds (GB+) significantly promotes renewable energy investment and reduces environmental pollution, while the contraction of green bonds (GB−) significantly reduces renewable energy investment and stimulates environmental damage. Likewise, expansion of renewable energy consumption (REC+) significantly reduced environmental degradation, while contraction of renewable energy consumption (REC−) significantly contributed to environmental degradation. Moreover, the result also validates the existence of inverted U-shaped EKC hypothesis in China The VECM Granger causality test indicate that renewable energy investment, green finance, renewable energy consumption, CO2 emission, and Gross Domestic Product (GDP) have long term causality. Chinese policymakers must focus on strengthening green finance, which will encourage renewable energy investment and renewable energy generation. Moreover, renewable electricity output greatly facilitates renewable energy investment, so China must innovate policies to take into account renewable electricity rather than fossil fuel generation in order to achieve the Sustainable Development Goals (SDGs).

Unconventional Self-Reconstructed Trimer-like Metal Zigzag Edge of 1T-Phase Transition Metal Dichalcogenides

Undercoordination-induced slight bond contraction of the pristine edge is a conventional edge self-reconstructed pattern in two-dimensional materials that generally cannot drive the edge into its ground state. Despite reports of unconventional edge self-reconstructed patterns of 1H-phase transition metal dichalcogenides (TMDCs), there have been no reports of sister 1T-phase TMDCs. Here, we predict an unconventional (2 × 1) edge self-reconstructed pattern for 1T-TMDCs by considering 1T-TiTe2. A novel self-reconstructed trimer-like metal zigzag edge (TMZ edge) with one-dimensional metal atomic chains and Ti3 trimers is uncovered. Its metal triatomic 3d orbital coupling leads to Ti3 trimerization. This TMZ edge occurs in group IV, V, and X 1T-TMDCs and has an energetic advantage far beyond conventional bond contraction. The unique triatomic synergistic effect results in better catalysis of the hydrogen evolution reaction (HER) for the 1T-TMDCs than with commercial platinum-based catalysts. This study provides a new strategy for maximizing the HER catalytic efficiency of 1T-TMDCs by using atomic edge engineering.

Dielectric properties of V2O3 and (V0.989Cr0.011)2O3 from temperature-dependent ac impedance measurements

The dielectric properties of the various insulating phases in pure ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$ and ${({\mathrm{V}}_{0.989}{\mathrm{Cr}}_{0.011})}_{2}{\mathrm{O}}_{3}$ crystals have been investigated. Large dielectric constants on the scale of ${10}^{3}$ were obtained, which were attributed to the backflow effect of normal carriers and also the periodic charge configuration relevant to V-V dimers in an antiferromagnetic insulating state or the bond contraction of V-Cr-V in a paramagnetic insulating phase. We propose that if Cr dopants are arranged nearly uniformly, the charge density of ${({\mathrm{V}}_{0.989}{\mathrm{Cr}}_{0.011})}_{2}{\mathrm{O}}_{3}$ in the paramagnetic insulating phase will exhibit a doping-induced wavelike distribution in real space, and thus the polarization of the system will be enhanced.

In Situ Detection of Iron in Oxidation States ≥ IV in Cobalt‐Iron Oxyhydroxide Reconstructed during Oxygen Evolution Reaction

AbstractCobalt‐iron oxyhydroxides (CoFeOOHx) are among the most active catalysts for the oxygen evolution reaction (OER). However, their redox behavior and the electronic and chemical structure of their active sites are still ambiguous. To shed more light on this, the complete and rapid reconstruction of four helical cobalt‐iron borophosphates with different Co:Fe ratios into disordered cobalt‐iron oxyhydroxides can be achieved, which are electrolyte‐penetrable and thus most transition metal sites can potentially participate in the OER. To track the redox behavior and to identify the active structure, quasi in situ X‐ray absorption spectroscopy is applied. Iron in high oxidation states ≥ IV (Fe4+) and its substantial redox behavior with an average oxidation state of around 2.8 to above 3.2 is detected. Furthermore, a 6% contraction of the Fe‐O bond length compared to Fe3+OOH references is observed during OER and a strong distortion of the [MO6] octahedra is identified. It is hypothesized that this bond contraction is caused by the presence of oxyl radicals and that di‐µ‐oxyl radical bridged cobalt‐iron centers are the active sites. It is anticipated that the detailed electronic and structural description can substantially contribute to the debate on the nature of the active site in bimetallic iron‐containing OER catalysts.

Revealing the interfacial phenomenon of metal-hydride formation and spillover effect on C48H16 sheet by platinum metal catalyst (Pt (n=1-4)) for hydrogen storage enhancement

Hydrogen is a worldwide green energy carrier, however due its low storage capacity, it has yet to be widely used as an energy carrier. Therefore, the quantum chemical method is being employed in this investigation for better understand the hydrogen storage behaviour on Pt (n = 1-4) cluster decorated C48H16 sheet. The Pt(n = 1-4) clusters are strongly bonded on the surface of C48H16 sheet with binding energies of −3.06, −4.56, −3.37, and −4.03 eV respectively, while the charge transfer from Pt(n = 1-4) to C48H16 leaves an empty orbital in Pt atom, which will be crucial for H2 adsorption. Initially, the molecular hydrogen is adsorbed on Pt(n = 1-4) decorated C48H16 sheet through the Kubas interaction with adsorption energies of −0.85, −0.66, −0.72, and −0.57 eV respectively, while H–H bond is elongated due to the transfer of electron from σ (HH) orbital to unfilled d orbital of the Pt atom, resulting in a Kubas metal-dihydrogen complexes. Furthermore, the dissociative hydrogen atoms adsorbed on Pt(n = 1-4) decorated C48H16 sheet have adsorption energies of −1.14 eV, −1.02 eV, −0.95 eV, and −1.08 eV, which are greater than the molecular hydrogen adsorption on Pt(n = 1-4) cluster supported C48H16 sheet with lower activation energy of 0.007, 0.109, 0.046, and 0.081 eV respectively. To enhance the dissociative hydrogen adsorption energy, positive and negative external electric fields are applied in the charge transfer direction. Increasing the positive electric field makes H–H bond elongation and good adsorption, whereas increasing the negative electric field results H–H bond contraction and poor adsorption. Thus, by applying a sufficient electric field, the H2 adsorption and desorption processes are can be easily tailored.