Exploring enhanced hydrogen adsorption on Ti doped Al nanoclusters: A DFT study

Boruah, Bishwajit; Kalita, Bulumoni

doi:10.1016/j.chemphys.2018.04.018

Cited by 11 publications

(5 citation statements)

References 53 publications

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“…This confirms the interaction between Ni atoms of NinMgm clusters and H 2 molecules. These interactions are in well agreement with previous studies [8,50].…”

Section: Density Of States Analysissupporting

confidence: 94%

“…Previous studies have shown that molecular adsorption of hydrogen takes place due to the interaction of the host material with the bonding and anti-bonding orbitals of hydrogen molecule [8,54]. To confirm this, we have carried out the partial density of states (PDOS) and the overlap population density of states (OPDOS) calculations of the hydrogenated clusters, which are plotted in Figure 4.…”

Section: Density Of States Analysismentioning

confidence: 71%

“…In the recent years, interest has been given to the light elements such as Li, Be, B, C, Na, Mg, Al and K etc. due to their reasonably less molecular masses in order to achieve high gravimetric density of H 2 for practical applications [4,5,6,7,8,9,10,11].In a recent density functional theory (DFT) study, Jaiswal et al have been able to achieve hydrogen gravimetric density of 18.7 wt% in alkali metal decorated silicon clusters [9]. In another study on aromatic bimetallic clusters, K. Srinivasu and co-workers found high hydrogen gravimetric density in hydrogenated Al 4 M 2 , Be 3 M 2 , M g 3 M 2 etc.…”

Section: Introductionmentioning

confidence: 99%

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Alloying Ratio Versus Cluster Size for Reversible Hydrogen Storage in Ni Doped Small Mg Clusters: Dispersion Corrected DFT Study

Boruah¹,

Kalita²

2022

Preprint

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Dispersion corrected density functional theory (ωB97X-D DFT) method is used to study the molecular hydrogen adsorption in N i n M g m (1 ≥ n ≥ 3, 1 ≥ m ≥ 9) clusters. All these clusters can effectively adsorb multiple H 2 in the preferred binding energy (BE) range between physisorption and chemisorption, i.e., 0.1eV ≥ BE ≥ 0.8eV. H 2 adsorption on N i k M g k (Ni:Mg=1:1), N i k M g 2k (Ni:Mg=1:2) and N i k M g 3k (Ni:Mg=1:3) (k=1-3) clusters shows fascinating behaviours in terms of Ni:Mg alloying ratio and cluster size. In each Ni:Mg ratio, the number of adsorbed H 2 in the heavier clusters (k=2, 3) becomes integral multiples of that in the lightest configuration (k=1). As a consequence, the gravimetric density of molecular hydrogen remains fixed at each Ni:Mg ratio irrespective of the cluster size. The corresponding values are 17.94 wt% (1:1), 14.46 wt% (1:2) and 13.28 wt% (1:3), which are significantly higher than the ultimate target of 6.5 wt% set by DOE, US. Molecular dynamics simulations further reveal that room temperature desorption of almost all H 2 molecules are possible for all the clusters.

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“…This confirms the interaction between Ni atoms of NinMgm clusters and H 2 molecules. These interactions are in well agreement with previous studies [8,50].…”

Section: Density Of States Analysissupporting

confidence: 94%

Section: Density Of States Analysismentioning

confidence: 71%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Alloying Ratio Versus Cluster Size for Reversible Hydrogen Storage in Ni Doped Small Mg Clusters: Dispersion Corrected DFT Study

Boruah¹,

Kalita²

2022

Preprint

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“…In experimental and theoretical investigations of the dissociative adsorption of H 2 by metallic Al surfaces, which is conceptually the growth of Al NCs from AlH 3 reversed, incorporation of Ti into Al surfaces catalyzes H 2 splitting. − These studies imply that Al NCs synthesized with Ti(OiPr) 4 could be doped with metallic Ti atoms. In this situation, all four isopropoxy ligands would be removed from Ti(OiPr) 4 by AlH 3 to generate metallic Ti.…”

Section: Resultsmentioning

confidence: 99%

Ligand-Dependent Colloidal Stability Controls the Growth of Aluminum Nanocrystals

Clark¹,

DeSantis²,

et al. 2019

J. Am. Chem. Soc.

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The precise size- and shape-controlled synthesis of monodisperse Al nanocrystals remains an open challenge, limiting their utility for numerous applications that would take advantage of their size and shape-dependent optical properties. Here we pursue a molecular-level understanding of the formation of Al nanocrystals by titanium(IV) isopropoxide-catalyzed decomposition of AlH3 in Lewis base solvents. As determined by electron paramagnetic resonance spectroscopy of intermediates, the reaction begins with the formation of Ti3+-AlH3 complexes. Proton nuclear magnetic resonance spectroscopy indicates isopropoxy ligands are removed from Ti by Al, producing aluminum(III) isopropoxide and low-valent Ti3+ catalysts. These Ti3+ species catalyze elimination of H2 from AlH3 inducing the polymerization of AlH3 into colloidally unstable low-valent aluminum hydride clusters. These clusters coalesce and grow while expelling H2 to form colloidally stable Al nanocrystals. The colloidal stability of the Al nanocrystals and their size is determined by the molecular structure and density of coordinating atoms in the reaction, which is controlled by choice of solvent composition.

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“…This parameter is directly proportional to the number of adsorbed H 2 molecules and inversely proportional to the molecular mass of the host. Therefore, the light elements such as Be, Na, Mg, Al, K and Li due to their reasonably less molecular masses are given importance to achieve high gravimetric density of H 2 for on-board applications [4,5,6,7,8].In a previous study on aromatic bimetallic clusters via density functional theory (DFT) calculation, K. Srinivasu and co-workers have reported high gravimetric density of hydrogen in hydrogenated Al 4 M 2 , Be 3 M 2 , M g 3 M 2 etc (M=Li, Na, K) clusters and proposed the formation of complexes Al 4 M 2 (H 2 ) 2n and Be 3 M 2 (H 2 ) 2n by Al 4 M 2 and Be 3 M 2 clusters through adsorption of multiple hydrogen molecules [7]. Recently Mg based materials have been widely studied to design H 2 storage medium because of their many advantageous properties such as cost effectiveness, abundance, non-toxicity and storage capacity [9,10,11,12,13,14,15,16,17,18,19].…”

Section: Introductionmentioning

confidence: 99%

Accentuating the Competency of $3d$ Transition Metal Doped $Mg_4$ Clusters towards Molecular Hydrogen Adsorption: A DFT Study

Boruah¹,

Kalita²

2021

Preprint

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Density functional theory (DF T ) studies show that doping of 3dT M atoms into M g 0,+ 4 (T M M g 0,+ 3 ) can alter the endothermic nature of molecular hydrogen adsorption on bare M g 0,+4 . H 2 adsorption on T M M g 0,+ 3 clusters depends on the T M (3d) orbital contribution to the frontier molecular orbitals of the clusters. In H 2 T M M g 0,+ 3 complexes, H 2 is adsorbed through donation and back donation of electronic charges with T M M g 0,+ 3 clusters. H 2 binding energy is the maximum for N iM g 3 (-0.76 eV) and F eM g + 3 (-0.48 eV) among the neutral and cationic T M M g 3 clusters, respectively. The geometry of H 2 adsorption complex entirely depends on the geometry of the host cluster. The lowest energy symmetrical structures of both N iM g 3 and F eM g + 3 clusters are less efficient than some slightly higher energy low symmetrical geometrical isomers for adsorption of multiple hydrogen molecules (13.28 H 2 wt% for N iM g 3 and 7.89 H 2 wt% for F eM g + 3 ). Greater exposer of T M 0,+ along with its lower Mg coordination number make host clusters more suitable for hydrogen storage.

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Exploring enhanced hydrogen adsorption on Ti doped Al nanoclusters: A DFT study

Cited by 11 publications

References 53 publications

Alloying Ratio Versus Cluster Size for Reversible Hydrogen Storage in Ni Doped Small Mg Clusters: Dispersion Corrected DFT Study

Alloying Ratio Versus Cluster Size for Reversible Hydrogen Storage in Ni Doped Small Mg Clusters: Dispersion Corrected DFT Study

Ligand-Dependent Colloidal Stability Controls the Growth of Aluminum Nanocrystals

Accentuating the Competency of $3d$ Transition Metal Doped $Mg_4$ Clusters towards Molecular Hydrogen Adsorption: A DFT Study

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