External electric filed effect on the Hydrogen adsorption and storage on Palladium – functionalized C20 bowl: A computational investigation
الموضوعات : Journal of NanoanalysisS Shayanmehr 1 , Reza Ghiasi 2 , Behrooz Mirza 3 , B Mohtat 4
1 - Department of Chemistry, East Tehran Branch, Islamic Azad University, Tehran, Iran
2 - East Tehran branch of Islamic azad university
3 - Department of Chemistry, Islamic Azad University, Karaj Branch, Alborz, Iran
4 - Department of Chemistry, East Tehran Branch, Islamic Azad University, Tehran, Iran
الکلمات المفتاحية: C20 bowl, Hydrogen storage, Adsorption, External Electric Field (EEF).,
ملخص المقالة :
This study investigated the adsorption of hydrogen molecule on palladium-functionalized C20 bowl in the absence and presence of external electric field (EEF) along z-axis by B3LYP-D3 model. EEF effect on the stability of the different isomers of the hydrogen adsorption was investigated. In these systems, the corrected adsorption energy amounts are estimated. Alterations in the dipole moment as well as structural factors were displayed in the presence and absence of EEF. Effect of EEF strength on the electronic and structures factors were studied. Also, H-H stretching wavenumber (H-H) of the studied systems were calculated. Linear correlations between adsorption energy, relative energy, dipole moment and H-H values with EEF strength were provided. Adsorption of hydrogen molecule on palladium-functionalized C20 bowl with B3LYP-D3 model in the absence and present of EEF indicated that the I-isomer was more stable isomer compared to II-isomer. The adsorption energies exhibited that the tendency to adsorb hydrogen molecule reduced with an elevation in EEF strength along z-axis. Adsorption of hydrogen on the Pd-doped C20 bowl was stronger in I-isomer than II- isomer in absence of EEF along Z-axis. Identical was observed in the presence of EEF at 0.001-0.007 a.u. But, stronger hydrogen adsorption was occurred in II-isomer than I- isomer in the presence of EEF at 0.009-0.011 a.u. Largest wavenumber was belonged to H-H stretching (H-H).
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External electric field effect on hydrogen adsorption and storage on a Palladium-functionalized C20 bowl: A computational investigation | |
Sonia Shayanmehr1, Reza Ghiasi2,*, Behrooz Mirza1, Bita Mohtat1 | |
1Department of Chemistry, Karaj Branch, Islamic Azad University, Karaj, Iran 2Department of Chemistry, East Tehran Branch, Islamic Azad University, Tehran, Iran
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ARTICLE INFO
Article History: Received 2022-09-26 Accepted 2024-06-12 Published 2023-05-05
Keywords: C20 bowl, Hydrogen storage, Adsorption, External Electric Field (EEF).
| ABSTRACT
This study investigated the adsorption of hydrogen molecule on a palladium-functionalized C20 bowl in the absence and presence of an external electric field (EEF) along the z-axis using the B3LYP-D3 model. The EEF effect on the stability of the different isomers of hydrogen adsorption was investigated. In the absence and presence of EEF, the I-isomer was a more stable isomer compared to the II-isomer. In these systems, the corrected adsorption energy amounts are estimated. Alterations in the dipole moment as well as structural factors were displayed in the presence and absence of EEF. The effects of EEF strength on electronic and structural factors were studied. Also, the H-H stretching wavenumber (nH-H) of the studied systems was calculated. Larger nH-H values were found in the presence of EEF than in the absence of EEF. Linear correlations between adsorption energy, relative energy, dipole moment, and nH-H values with EEF strength were provided.
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How to cite this article Shayanmehr S., Ghiasi R., Mirza B., Mohtat B., External electric field effect on hydrogen adsorption and storage on a Palladium-functionalized C20 bowl: A computational investigation. J. Nanoanalysis., 10 (2): 505-514, Spring 2023.
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INTRODUCTION
Hydrogen is the most common and simple chemical element, consisting of only one electron and one proton. Hydrogen is produced by renewable raw materials, particularly natural gas, as the most cost-effective candidate for hydrogen supply [1]. It demonstrates high sustainability, renewability, and energy efficiency. It is a clean energy carrier, and hydrogen combustion in the fuel cell generates power, heat or electricity with no pollution of the environment or effect on the climate [2]. So, hydrogen can be considered an energy carrier for transportation systems like aircraft and vehicles.
In normal circumstances, hydrogen is a highly volatile gas that should be stored in fuel-cells for practical uses. It can be stored as either a liquid (cryogenic temperature) or a gas (by high-pressure, 5000–10000 psi tank pressure) on board a vehicle [3]. Therefore, adequate transportation and storage techniques are essential to applying hydrogen as a fuel in fuel-cell systems. Its safety and storage challenges on fuel cell vehicles (as a lightweight, small, and immune container) are important problems for hydrogen fuel cars [4, 5]. Various computational investigations have been reported about hydrogen storage in different systems [6-14]. In a computational investigation, hydrogen storage and adsorption on Palladium-functionalized graphene as well as hydrogen the boron nitride analogue were investigated [15]. A density functional theory investigation on (Mg(BH4))n (n = 1–4) clusters to be used as a material for hydrogen storage has been published [16].
Fullerene is an allotrope of carbon and is composed of individual molecules characterized by an infinite number of discrete. Fullerene was detected after graphite and diamond, and in contrast to graphite and diamond, each Fullerene type possesses its own specific features [17]. Fullerene is commonly generated by pyrolysis, electric arc vaporization, combustion, or laser ablation [18-22]. Cage, bowl, and ring are the lowest energy members in the C20 family. Although fullerene is not soluble in water, it shows limited solubility in conventional organic solvents [23]. It partially masks the polar fullerene surface or covalently modifies the aromatic structure to overcome its compatibility restriction with biological media [23]. A computational investigation of hydrogen adsorption and storage on palladium-functionalized C20 bowl and C20H10 bowl molecules including hydrogen saturation, has been reported [24].
The external electric fields (EEFs) impact the variations matching the geometric and electronic structure of many conjugated molecules; the chemical reactivity as well as the global and local reactivity measures were displayed [25-39].
In this work, we study the adsorption of hydrogen molecule on a palladium-functionalized C20 bowl in the presence and absence of EEF along the z-axis using the B3LYP-D3 model. The EEF effect on the structural and electronic parameters of the complex has been assessed.
COMPUTIONAL TECHNIQUES
We used Gaussian 09 software for data analysis [40]. The Def2-TZVPPD basis set [41-46] and the standard 6-311G(d,p) basis set [42-44, 47-51] were employed respectively for the Pt element and main groups of elements. The evaluated molecules were regarded in the singlet and neutral forms. For excluding direct computation of the correlation and exchange integrals of 18 electrons for the Pd atom, effective core potential (ECP) to the Def2-TZVPPD basis set employed [52].
B3LYP-D3 model was used for Geometry optimizations. B3LYP-D3 model can maintain the B3LYP method benefit and also it can simulate the weak interactions well using Grimme term D3 [53].
For proving no imaginary frequency of the optimized structures, harmonic vibrational frequencies computed.
RESULTS AND DISCUSSION
Energetic aspect
Figure 1 indicates structures of C20 bowl and two mode adsorption of hydrogen molecule on the Pd-doped C20 bowl. Optimized geometries of various modes of adsorption of hydrogen molecule on the Pd doped-C20-bowl are displayed in Figure 2. The absolute energy as well as relative energy values of these isomers are computed in the absence and presence of EEF along z-axis (Table 1). Such values indicate I-isomer is most energetically stable isomer both in presence and absence of EEF. Relative energy values are decreased with increasing of EEF strength. There are good linear correlations relative energy values with EEF strength (Figure 3).
DE = -288.32 Ez + 34.06;
R² = 0.9861
Figure 1. Structures of (a) C20 bowl (b) two mode adsorption of hydrogen molecule on the Pd-doped C20 bowl
|
|
I-Isomer | II-Isomer |
Figure 2. Optimized geometrized of the various isomers of C20PdH2 complex.
1. Adsorption energy values
The adsorption energy (DEad) can be assessed as follows:
E (Pd-doped C20-bowl) indicates the energy related to the isolated Pd-doped C20-bowl; E (H2) represents the hydrogen molecule energy, and E (Pd-doped C20-bowl…H2) indicates the energy related to hydrogen adsorbed on the Pd-doped C20-bowl surface.
Corrected adsorption energy is calculated as follows:
Where E indicates the basis set superposition error (BSSE) corrected for adsorption energy [54, 55].
The Corrected adsorption energy values of many isomers of adsorption of hydrogen molecule on the Pd-doped C20-bowl are computed in the absence and presence of the EEF along the z-axis (Table 1). The negative DEad values indicate the desirable complex generation energetically. The range of calculated DEad values is acceptable for chemisorption. The adsorption energies indicate that the tendency to adsorb hydrogen molecule decreases with an increase in EEF strength along the z-axis Adsorption of hydrogen on the Pd-doped C20 bowl is stronger in the I-isomer than the II- isomer in the absence of EEF along the z-axis. Identical is observed in the presence of EEF at 0.001-0.007 a.u. But, stronger hydrogen adsorption occurs in the II-isomer than the I-isomer in the presence of EEF at 0.009-0.011 a.u. There are good linear correlations between corrected adsorption energy values and EEF strength (Figure 4).
= 26.756 Ez - 15.766; R² = 0.9961
= 146.01 Ez - 16.717; R² = 0.9716
2. Dipole moment
Dipole moment values related to evaluated molecules are measured in the presence and absence of EEF along the z-axis (Table 1). The more stable isomer (I-isomer) of adsorption of hydrogen molecule on the Pd-doped C20 bowl possesses the larger dipole moment value in absence and the presence of EEF at 0.001-0.007 a.u. II-isomer indicates larger dipole moment values in the presence of EEF at 0.009-0.011 a.u than I-isomer. Linear correlations between dipole moment values and EEF strength are:
m (I-isomer) = 84.47 Ez + 4.0282;
R² = 0.8936
m(II-isomer) = 356.83 Ez + 1.5751;
R² = 0.9973
It can be found, better linear relationship between two parameters for the II-isomer in compared to the I-isomer.
3. Structural parameters
Pd-C, H…H, and Pd-H distances in the Pd-doped C20 bowl complexes are summarized in Table 1 after and before hydrogen adsorption. It can be observed that the average of Pd-C bond distances and H-H bond lengths is shorter in the EEF presence alone z-axis than in the absence of EEF. These bond distances decrease with an increase in EEF strength. In the case of hydrogen adsorption, longer H-H distances are found compared to free hydrogen (74.4 pm).
Also, the mean Pd-H bond distances are longer in the EEF presence alone z-axis in comparison with the absence of EEF. Such bond distances are increased with an increase of EEF strength. Vibrational analysis
Vibrational analysis of the C20PdH2 complexes is investigated in the presence and absence of EEF along the a-axis. It can be found that the largest wavenumber is attributed to H-H stretching (nH-H). The wavenumber values of this vibration are listed in Table 2. Free hydrogen molecule reveals H-H stretching at 4419.4 cm-1 at B3LYP-D3/6-311G (d,P) level of theory. It can be observed that the position of this vibration is shifted to lower energy values after hydrogen adsorption occurs. Larger nH-H values are observed in the presence of EEF in comparison the absence of EEF. Such values enhance with an increase in EEF strength along the z-axis. The nH-H values are associated with EEF strength along z-axis (Figure 5).
nH-H (I-isomer) = 5723.5 Ez + 3479.6; R² = 0.9976
nH-H (II-isomer) = 19987 Ez + 3425.4; R² = 0.9963
Figure 3. Linear correlations relative energy values of in the various C20PdH2 complexes with EEF strength along z-axis.
Figure 4. Linear correlations between corrected adsorption energy values with EEF strength along z-axis in the various C20PdH2 complexes.
Table 1. Energy (E, a.u), relative energy (DE, kcal/mol), corrected adsorption energy and dipole moment (m, Debye) values of the two modes of adsorption hydrogen molecule on the Pd-doped C20 bowl in absence and presence of external electric filed along z-axis with Ez strength (in a.u).
Ez | E(I) | E(II) | DE(I) | DE(II) |
|
| m(I) | m(II) |
0 | -890.8959 | -890.8419 | 0.00 | 33.90 | -15.77 | -16.84 | 4.1652 | 1.6835 |
0.001 | -890.8961 | -890.8424 | 0.00 | 33.72 | -15.74 | -16.60 | 4.1585 | 1.9409 |
0.003 | -890.8969 | -890.8439 | 0.00 | 33.30 | -15.68 | -16.21 | 4.1977 | 2.5721 |
0.005 | -890.8982 | -890.8460 | 0.00 | 32.78 | -15.64 | -15.87 | 4.3139 | 3.2765 |
0.007 | -890.9000 | -890.8487 | 0.00 | 32.17 | -15.57 | -15.60 | 4.5075 | 4.0207 |
0.009 | -890.9023 | -890.8521 | 0.00 | 31.48 | -15.52 | -15.39 | 4.7759 | 4.7917 |
0.011 | -890.9051 | -890.8561 | 0.00 | 30.70 | -15.48 | -15.25 | 5.1198 | 5.5860 |
| R(Pd-C) | R(Pd-H) | R(H-H) | nH-H | ||||
Ez | I | II | I | II | I | II | I | II |
0.000 | 201.7 | 217.6 | 180.5 | 178.0 | 80.7 | 81.2 | 3480.10 | 3418.52 |
0.001 | 201.6 | 217.2 | 180.7 | 178.5 | 80.6 | 81.0 | 3486.27 | 3445.71 |
0.003 | 201.6 | 216.3 | 180.9 | 179.5 | 80.5 | 80.7 | 3496.64 | 3488.18 |
0.005 | 201.6 | 215.4 | 181.0 | 180.5 | 80.5 | 80.4 | 3506.32 | 3530.45 |
0.007 | 201.5 | 214.6 | 181.3 | 181.5 | 80.4 | 80.1 | 3519.07 | 3569.83 |
0.009 | 201.5 | 213.9 | 181.5 | 182.5 | 80.3 | 79.8 | 3530.59 | 3606.52 |
0.011 | 201.5 | 213.1 | 181.8 | 183.5 | 80.2 | 79.6 | 3544.10 | 3638.36 |
Figure 5. Linear correlations between nH-H values with EEF strength along z-axis in the various C20PdH2 complexes.
1. Molecular orbital analysis
Table 3 lists the HOMO-LUMO gap and the frontier orbital energy values in the evaluated systems. The values reveal that the frontier orbitals of the I-C20PdH2 complex are more destabilized in the EEF presence along the z-axis than in the absence. These destabilizations increase with the increasing of strength of the EEF. In the II-C20PdH2 complex, HOMO is destabilized in the presence EEF along the z-axis than in the absence of EEF. Such destabilization increases with an increase in the strength of the EEF along z-axis. But LUMO of the II-C20PdH2 complex is stabilized in the presence of EEF along the z-axis rather than in the absence of EEF. This stability increases with an elevation in the strength of the EEF along the z-axis.
The HOMO-LUMO gap value of the I-C20PdH2 complex increases in its presence along the z-axis than in the absence of EEF. This value increases with an increase in the strength of EEF along the z-axis. The HOMO-LUMO gap value of the II-C20PdH2 complex decreases in EEF presence along the z-axis than in EEF absence. Such value reduces with an increase in the strength of EEF along the z-axis.
Table 3. Frontier orbital energy and HOMO-LUMO gap values of the two modes of adsorption hydrogen molecule on the Pd-doped C20 bowl in absence and presence of external electric filed along z-axis (in eV).
| I | II | Gap | |||
Ez | E(HOMO) | E(LUMO) | E(HOMO) | E(LUMO) | I | II |
0 | -6.59 | -3.14 | -6.45 | -3.37 | 3.45 | 3.09 |
0.001 | -6.58 | -3.13 | -6.44 | -3.38 | 3.45 | 3.07 |
0.003 | -6.58 | -3.11 | -6.43 | -3.40 | 3.47 | 3.03 |
0.005 | -6.57 | -3.09 | -6.42 | -3.43 | 3.49 | 3.00 |
0.007 | -6.57 | -3.07 | -6.42 | -3.45 | 3.50 | 2.96 |
0.009 | -6.56 | -3.05 | -6.42 | -3.49 | 3.52 | 2.93 |
0.011 | -6.56 | -3.03 | -6.42 | -3.52 | 3.53 | 2.89 |
CONCLUSION
Adsorption of hydrogen molecule on a palladium-functionalized C20 bowl with the B3LYP-D3 model in the absence and presence of EEF indicated that the I-isomer was a more stable isomer compared to the II-isomer. The adsorption energies exhibited that the tendency to adsorb molecules decreased with an elevation in EEF strength along the z-axis. Adsorption of hydrogen on the Pd-doped C20 bowl was stronger in the I-isomer than the II- isomer in the absence of EEF along the z-axis. Identical behavior was observed in the presence of EEF at 0.001-0.007 a.u. But stronger hydrogen adsorption occurred in the II-isomer than the I-isomer in the presence of EEF at 0.009-0.011 a.u. The largest wavenumber belonged to H-H stretching (nH-H). The position of this vibration was shifted to lower energy values after hydrogen adsorption occurred. Larger nH-H values were reported in the presence of EEF than in the absence of EEF. Such values increase with an increase in EEF strength along the z-axis. There are good relationships between nH-H values and EEF strength along the z-axis. The HOMO-LUMO gap value of the I-C20PdH2 complex was larger in the presence of EEF along the z-axis than in the absence of EEF. A larger gap value was found with an increase in the strength of the EEF.
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*Corresponding Author Email: reza.ghiasi@iau.ac.ir
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