Competition of quantum effects inH2/D2sieving in narrow single-wall carbon nanotubes

Mondelo-Martell, Manel; Huarte-Larrañaga, Fermı́n

doi:10.1080/00268976.2021.1942277

Cited by 4 publications

(3 citation statements)

References 58 publications

(70 reference statements)

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“…The present work shows this for weak couplings, but we plan to extend to system–bath systems that show stronger couplings. Atoms or molecules in fullerenes, ,− carbon nanotubes, , clathrate (aluminosilicates), and metal–organic frameworks are all accessible with this new approach. For more complex systems involving several molecules encapsulated in a nanoscale environment, the calculations are formally doable.…”

Section: Discussionmentioning

confidence: 99%

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Chen

Benoit

Scribano

et al. 2022

J. Chem. Theory Comput.

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A Smolyak algorithm adapted to system−bath separation is proposed for rigorous quantum simulations. This technique combines a sparse grid method with the system−bath concept in a specific configuration without limitations on the form of the Hamiltonian, thus achieving a highly efficient convergence of the excitation transitions for the "system" part. Our approach provides a general way to overcome the perennial convergence problem for the standard Smolyak algorithm and enables the simulation of floppy molecules with more than a hundred degrees of freedom. The efficiency of the present method is illustrated on the simulation of H 2 caged in an sII clathrate hydrate including two kinds of cage modes. The transition energies are converged by increasing the number of normal modes of water molecules. Our results confirm the triplet splittings of both translational and rotational (j = 1) transitions of the H 2 molecule. Furthermore, they show a slight increase of the translational transitions with respect to the ones in a rigid cage.

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Section: Discussionmentioning

confidence: 99%

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Chen

Benoit

Scribano

et al. 2022

J. Chem. Theory Comput.

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“…Specially appealing in regards to the impact of quantum effects on the diffusion of H 2 and D 2 along carbon nanotubes is the experimental finding of reserved trends in their rates upon cooling (Nguyen et al, 2010), with the D 2 isotope becoming the faster inspite of its higher mass (Nguyen et al, 2010). The impact of quantum effects in confined H 2 and D 2 motion has been theoretically confirmed as well (Mondelo-Martell and Huarte-Larrañaga, 2016;Mondelo-Martell et al, 2017;Mondelo-Martell and Huarte-Larrañaga, 2021).…”

Section: Introductionmentioning

confidence: 93%

Mini Review: Quantum Confinement of Atomic and Molecular Clusters in Carbon Nanotubes

Lara‐Castells

Mitrushchenkov

2021

Front. Chem.

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We overview our recent developments on a computational approach addressing quantum confinement of light atomic and molecular clusters (made of atomic helium and molecular hydrogen) in carbon nanotubes. We outline a multi-scale first-principles approach, based on density functional theory (DFT)-based symmetry-adapted perturbation theory, allowing an accurate characterization of the dispersion-dominated particle–nanotube interaction. Next, we describe a wave-function-based method, allowing rigorous fully coupled quantum calculations of the pseudo-nuclear bound states. The approach is illustrated by showing the transition from molecular aggregation to quasi-one-dimensional condensed matter systems of molecular deuterium and hydrogen as well as atomic 4He, as case studies. Finally, we present a perspective on future-oriented mixed approaches combining, e.g., orbital-free helium density functional theory (He-DFT), machine-learning parameterizations, with wave-function-based descriptions.

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“…Recently, a number of porous solid adsorbents, including metal–organic frameworks (MOFs), − covalent organic frameworks (COFs), zeolites, , organic cages, carbon, , have been explored for the separation of hydrogen and deuterium via kinetic quantum sieving (KQS) effect or chemical affinity quantum sieving (CAQS) effect. A large number of MOF membranes have also been screened by the combination of physics-based and data-based models to identify useful geometric features for efficient deuterium–hydrogen separation .…”

Section: Introductionmentioning

confidence: 99%

Highly Effective H₂/D₂ Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving

Ding

Xiong

et al. 2023

ACS Appl. Mater. Interfaces

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Realizing ideal deuterium separation from isotopic mixtures remains a daunting challenge because of their almost identical sizes, shapes, and physicochemical properties. Using the quantum sieving effect in porous materials with suitable pore size and open metal sites (OMSs) enables efficient hydrogen isotope separation. Herein, synthetic HKUST-1-derived microporous mixed-valence Cu(I)Cu(II)-BTC (BTC = benzene-1,3,5-tricarboxylate), featuring a unique network of distinct Cu(I) and Cu(II) coordination sites, can remarkably boost the D2/H2 isotope separation, which has a high selectivity (S D2/H2 ) of 37.9 at 30 K, in comparison with HKUST-1 and other porous materials. Density functional theory (DFT) calculations indicate that the introduction of Cu(I) macrocycles in the framework decreases the pore size and further leads to relatively enhanced interaction of H2/D2 molecules on Cu(II) sites. The significantly enhanced selectivity of Cu(I)Cu(II)-BTC at 30 K can be mainly attributed to the synergistic effect of kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS). The results reveal that Cu(I) OMSs exhibit counterintuitive behaviors and play a crucial role in tuning quantum sieving without a complex structural design, which provides a deeper insight into quantum sieving mechanisms and a new strategy for the intelligent design of highly efficient isotope systems.

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Competition of quantum effects inH₂/D₂sieving in narrow single-wall carbon nanotubes

Cited by 4 publications

References 58 publications

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Mini Review: Quantum Confinement of Atomic and Molecular Clusters in Carbon Nanotubes

Highly Effective H₂/D₂ Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving

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Competition of quantum effects inH2/D2sieving in narrow single-wall carbon nanotubes

Cited by 4 publications

References 58 publications

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Smolyak Algorithm Adapted to a System–Bath Separation: Application to an Encapsulated Molecule with Large-Amplitude Motions

Mini Review: Quantum Confinement of Atomic and Molecular Clusters in Carbon Nanotubes

Highly Effective H2/D2 Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving

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Product

Resources

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Competition of quantum effects inH₂/D₂sieving in narrow single-wall carbon nanotubes

Highly Effective H₂/D₂ Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving