Understanding the Mechanism of Hydrogen Adsorption into Metal-Organic Frameworks

ABSTRACTHydrogen adsorption mechanism into the porous metal-organic frameworks (MOFs) has been studied by density functional theory calculation. The selected functionals for the prediction of interaction energies between hydrogen and potential adsorption sites of MOFs were utilized after the evaluation with the various functionals for interaction energy of H2···C6H6 model system. The adsorption energy of hydrogen molecule into MOFs was investigated with the consideration of the favorable adsorption sites and the orientations. We also calculated the second favorable adsorption sites by geometry optimization using every combination of two first absorbed hydrogen molecules. Based on the calculation of first and second adsorption sites and energies, it has been suggested that the hydrogen adsorption into MOFs follows a cooperative mechanism in which the initial metal sites initiate the propagation of the hydrogen adsorption on the whole frameworks. In addition, the interaction mode between the simple benzene ring with hydrogen is significantly changed when the benzene ring has been incorporated into the framework of MOFs.

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Investigation, using density function theory, of coverage of the kaolinite (001) surface during hydrogen adsorption

Clay Minerals ◽

10.1180/clm.2018.28 ◽

2018 ◽

Vol 53 (3) ◽

pp. 393-402 ◽

Cited By ~ 1

Author(s):

Jian Zhao ◽

Wei Gao ◽

Zhi-Gang Tao ◽

Hong-Yun Guo ◽

Man-Chao He

Keyword(s):

Density Functional ◽

Hydrogen Adsorption ◽

Function Theory ◽

Lattice Relaxation ◽

Electronic Density ◽

Functional Theory ◽

Adsorption Sites ◽

Coverage Dependence ◽

Hydrogen Molecules ◽

Wide Range

ABSTRACTKaolinite can be used for many applications, including the underground storage of gases. Density functional theory was employed to investigate the adsorption of hydrogen molecules on the kaolinite (001) surface. The coverage dependence of the adsorption sites and energetics was studied systematically for a wide range of coverage, Θ (from 1/16 to 1 monolayer). The three-fold hollow site is the most stable, followed by the bridge, top-z and top sites. The adsorption energy of H2 decreased with increasing coverage, thus indicating the lower stability of surface adsorption due to the repulsion of neighbouring H2 molecules. The coverage has obvious effects on hydrogen adsorption. Other properties of the H2/kaolinite (001) system, including the lattice relaxation and changes of electronic density of states, were also studied and are discussed in detail.

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Direct Observation of Hydrogen Adsorption Sites and Nanocage Formation in Metal-Organic Frameworks

Physical Review Letters ◽

10.1103/physrevlett.95.215504 ◽

2005 ◽

Vol 95 (21) ◽

Cited By ~ 212

Author(s):

T. Yildirim ◽

M. Hartman

Keyword(s):

Direct Observation ◽

Hydrogen Adsorption ◽

Metal Organic Frameworks ◽

Adsorption Sites ◽

Metal Organic

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Ti-coated BC2N nanotubes as hydrogen storage materials

Canadian Journal of Chemistry ◽

10.1139/cjc-2012-0386 ◽

2013 ◽

Vol 91 (7) ◽

pp. 598-604 ◽

Cited By ~ 5

Author(s):

Seifollah Jalili ◽

Farzad Molani ◽

Jeremy Schofield

Keyword(s):

Dft Calculations ◽

Density Functional ◽

Hydrogen Adsorption ◽

Molecular Form ◽

Hydrogen Storage Materials ◽

Hydrogen Atoms ◽

Functional Theory ◽

Adsorption Sites ◽

Hydrogen Molecules ◽

Bc2n Nanotubes

Density functional theory (DFT) calculations have been performed to investigate Ti adsorption on BC2N nanotubes and the hydrogen adsorption capacity of Ti-coated structures. Different adsorption sites have been examined for the Ti adatom, and it is found that the most stable structure has a configuration with alternating columns of carbon and boron–nitrogen hexagons. The DFT calculations indicate that an adsorbed Ti atom on a carbon hexagon can bind four hydrogen molecules in molecular form, while Ti atoms on boron–nitride hexagons can adsorb three hydrogen molecules and two hydrogen atoms. Based on the calculations, the gravimetric efficiency corresponding to decoration of 67% of six carbon rings with Ti adatoms is estimated to be 8 wt %. Computation of the charge transfer reveals that the Ti atom on BC2N is in a cationic state. In addition, Ti adsorption has a significant influence on the electronic structure of the nanotubes and allows for the conversion of nanotubes from semiconductors in the pristine state to conductors upon doping. The interactions between the nanotubes, the Ti atom and hydrogen molecules have also been analyzed using Dewar coordination and Kubas interactions.

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A First-Principles Study on Titanium-Decorated Adsorbent for Hydrogen Storage

Energies ◽

10.3390/en14206845 ◽

2021 ◽

Vol 14 (20) ◽

pp. 6845

Author(s):

Kai Ma ◽

Erfei Lv ◽

Di Zheng ◽

Weichun Cui ◽

Shuai Dong ◽

...

Keyword(s):

Hydrogen Storage ◽

Density Functional ◽

Hydrogen Adsorption ◽

Density Functional Theory Calculation ◽

Partial Density ◽

Ambient Conditions ◽

Functional Theory ◽

Hydrogen Molecules ◽

Theory Calculation ◽

Hydrogen Storage Medium

Based on density functional theory calculation, we screened suitable Ti-decorated carbon-based hydrogen adsorbent structures. The adsorption characteristics and adsorption mechanism of hydrogen molecules on the adsorbent were also discussed. The results indicated that Ti-decorated double vacancy (2 × 2) graphene cells seem to be an efficient material for hydrogen storage. Ti atoms are stably embedded on the double vacancy sites above and below the graphene plane, with binding energy higher than the cohesive energy of Ti. For both sides of Ti-decorated double vacancy graphene, up to six H2 molecules can be adsorbed around each Ti atom when the adsorption energy per molecule is −0.25 eV/H2, and the gravimetric hydrogen storage capacity is 6.67 wt.%. Partial density of states (PDOS) analysis showed that orbital hybridization occurs between the d orbital of the adsorbed Ti atom and p orbital of C atom in the graphene layer, while the bonding process is not obvious during hydrogen adsorption. We expect that Ti-decorated double vacancy graphene can be considered as a potential hydrogen storage medium under ambient conditions.

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ENHANCEMENT EFFECT OF LITHIUM-DOPING FUNCTIONALIZATION ON HYDROGEN ADSORPTION IN METAL-ORGANIC FRAMEWORK

Surface Review and Letters ◽

10.1142/s0218625x17500676 ◽

2016 ◽

Vol 24 (05) ◽

pp. 1750067 ◽

Cited By ~ 2

Author(s):

LIANGZHI XIA ◽

QING LIU ◽

FENGLING WANG ◽

YUPENG LI

Keyword(s):

Hydrogen Adsorption ◽

Metal Organic Framework ◽

Enhancement Effect ◽

Li Doping ◽

Adsorption Sites ◽

Hydrogen Molecules ◽

Metal Organic ◽

Gravimetric Adsorption ◽

Hydrogen Storage Performance ◽

Grand Canonical

Grand canonical Monte-Carlo simulation was carried out to study the effect of linker functionalization by Li atoms. In this work, two new Li-doping structures, MOF-808-Li and MOF-808-OLi were theoretically constructed by physical modification and chemical modification, respectively. The results show that both these methods can improve the hydrogen storage performance significantly, owing to the Li atoms increasing the interaction energy between the hydrogen molecules and the Li-doped MOF-808. Furthermore, MOF-808-OLi shows higher hydrogen capacity in comparison to the H2 adsorption in the MOF-808-Li, this can be attributed to the new adsorption sites created by oxygen atom. The gravimetric adsorption capacity of MOF-808-OLi can reach 3.17[Formula: see text]wt.% at 77[Formula: see text]K and 1[Formula: see text]bar, which are significantly higher than the hydrogen adsorption in the unmodified MOF-808.

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Probing the Adsorption Sites for CO2in Metal Organic Frameworks Materials MIL-53 (Al, Cr) and MIL-47 (V) by Density Functional Theory

The Journal of Physical Chemistry C ◽

10.1021/jp075782y ◽

2008 ◽

Vol 112 (2) ◽

pp. 514-520 ◽

Cited By ~ 109

Author(s):

N. A. Ramsahye ◽

G. Maurin ◽

S. Bourrelly ◽

P. L. Llewellyn ◽

C. Serre ◽

...

Keyword(s):

Density Functional Theory ◽

Density Functional ◽

Metal Organic Frameworks ◽

Functional Theory ◽

Adsorption Sites ◽

Metal Organic

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A density functional theory study on the interaction of hydrogen molecules with aromatic linkers in metal-organic frameworks

Journal of Physics and Chemistry of Solids ◽

10.1016/j.jpcs.2007.10.098 ◽

2008 ◽

Vol 69 (5-6) ◽

pp. 1428-1431 ◽

Cited By ~ 3

Author(s):

Daejin Kim ◽

Dong Hyun Jung ◽

Sang Beom Choi ◽

Ji Hye Yoon ◽

Jaheon Kim ◽

...

Keyword(s):

Density Functional Theory ◽

Density Functional ◽

Metal Organic Frameworks ◽

Density Functional Theory Study ◽

Functional Theory ◽

Hydrogen Molecules ◽

Metal Organic

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Hydrogen adsorption mechanism of MOF-74 metal–organic frameworks: an insight from first principles calculations

RSC Advances ◽

10.1039/d0ra08864a ◽

2020 ◽

Vol 10 (72) ◽

pp. 43940-43949

Author(s):

Trang Nguyen-Thuy ◽

Phong Le-Hoang ◽

Nam Hoang Vu ◽

Thong Nguyen-Minh Le ◽

Tan Le Hoang Doan ◽

...

Keyword(s):

First Principles ◽

Density Functional ◽

Adsorption Mechanism ◽

Hydrogen Adsorption ◽

Metal Organic Frameworks ◽

Dft Method ◽

First Principles Calculations ◽

Microscopic Mechanism ◽

Functional Theory ◽

Metal Organic

The microscopic mechanism of the H2 adsorption of two Mg-MOF-74 isoreticular frameworks, one with a benzenedicarboxylate linker and the other with a dihydroxyfumarate linker, were studied on the basis of density functional theory (DFT) method.

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