Nuclear quantum effects on adsorption of H2 and isotopologues on metal ions

Savchenko, Ievgeniia; Gu, Bing; Heine, Thomas; Jakowski, Jacek; Garashchuk, Sophya

doi:10.1016/j.cplett.2016.12.069

Cited by 12 publications

(9 citation statements)

References 34 publications

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“…There is also much interest in H 2 -M + interactions for applications of reversible storage of hydrogen in porous materials, [7][8][9][10][11] where dopant metal cations act as centers to which hydrogen molecules attach. Moreover, different nuclear quantum effects in H 2 and D 2 have been proposed to exploit selective adsorption 12 and isotope separation 13 in metal-doped materials, processes of paramount importance for the development of new fusion reactors.…”

Section: Introductionmentioning

confidence: 99%

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium

Zárate

Bartolomei

González‐Lezana

et al. 2019

Phys. Chem. Chem. Phys.

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Section: Introductionmentioning

confidence: 99%

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium

Zárate

Bartolomei

González‐Lezana

et al. 2019

Phys. Chem. Chem. Phys.

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“…Although anharmonic effects associated with the H-H stretch mode can be readily treated to improve the ZPE, proper evaluation of the finite-temperature thermal corrections to the enthalpy using quantum chemistry methods requires modification of the RRHO model 101,102 or full solution of a non-local nuclear Schrödinger equation for the soft modes. 103 Entropy of H 2 binding. The limits of static electronic structure calculations become apparent in evaluating the entropy of H 2 binding.…”

Section: Thermodynamic Factors Beyond Binding Energymentioning

confidence: 99%

An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage

Allendorf

Hulvey

Gennett

et al. 2018

Energy Environ. Sci.

216

187

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Nanoporous adsorbents are a diverse category of solid-state materials that hold considerable promise for vehicular hydrogen storage. Although impressive storage capacities have been demonstrated for several materials, particularly at cryogenic temperatures, materials meeting all of the targets established by the U.S. Department of Energy have yet to be identified. In this Perspective, we provide an overview of the major known and proposed strategies for hydrogen adsorbents, with the aim of guiding ongoing research as well as future new storage concepts. The discussion of each strategy includes current relevant literature, strengths and weaknesses, and outstanding challenges that preclude implementation. We consider in particular metal-organic frameworks (MOFs), including surface area/volume tailoring, open metal sites, and the binding of multiple H 2 molecules to a single metal site. Two related classes of porous framework materials, covalent organic frameworks (COFs) and porous aromatic frameworks (PAFs), are also discussed, as are graphene and graphene oxide and doped porous carbons. We additionally introduce criteria for evaluating the merits of a particular materials design strategy. Computation has become an important tool in the discovery of new storage materials, and a brief introduction to the benefits and limitations of computational predictions of H 2 physisorption is therefore presented. Finally, considerations for the synthesis and characterization of hydrogen storage adsorbents are discussed. IntroductionStorage of hydrogen with sufficient gravimetric and volumetric capacity for vehicular use remains a significant obstacle to the widespread adoption of hydrogen fuel cell electric vehicles (FCEVs). Several FCEV models are now commercially available in limited locations around the world, and in these vehicles hydrogen is stored as a gas at room temperature with a fill Table 1 along with the current performance of 700 bar systems. These values pertain to the entire storage system, which includes the mass and volume of hydrogen in addition to the tank and associated balance-ofplant (BOP) components. Notably, it is physically impossible to meet the 2025 and ultimate volumetric capacity target with pressurized gas, as the density of H 2 gas at 700 bar and room temperature is just 40 g L À1 without accounting for the BOP.The search for solid-state H 2 storage materials that can supplant compressed gas systems has been ongoing for at least two decades. The development of a viable storage material Broader contextThe widespread use of hydrogen as a clean, sustainable energy carrier has the potential to provide several significant benefits, including a reduction in oil dependency and emissions, improved energy security and grid resiliency, and substantial economic opportunities across many sectors. Hydrogen-fueled vehicles are already appearing internationally, and one of the critical enabling technologies for increasing their availability is on-board hydrogen storage. Stakeholders in developing a hydrogen in...

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“…Processes such as electron transfer, charge transport, electronic friction at metal surfaces and nonradiative decay after photoexcitation often involve multiple PESs, with nonadiabatic (NA) transitions among them. In addition, for systems containing small mass elements, for example, hydrogen, zero‐point motion and tunneling effects may not be ignored and as a result require a quantum mechanical description of the nuclei . To address all these issues, the most ambitious approach is to treat the entire system, including the nuclei, quantum‐mechanically.…”

Section: Introductionmentioning

confidence: 99%

“…In addition, for systems containing small mass elements, for example, hydrogen, zero-point motion and tunneling effects may not be ignored and as a result require a quantum mechanical description of the nuclei. [33][34][35] To address all these issues, the most ambitious approach is to treat the entire system, including the nuclei, quantum-mechanically. Unfortunately, the formidable computational costs restrict the scope of the application and can only be applied to small systems within short time scales under the current computation resources.…”

Section: Introductionmentioning

confidence: 99%

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

Zheng

Chu

Zhao

et al. 2019

WIREs Comput Mol Sci

240

258

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The ultrafast dynamics of photoexcited charge carriers in condensed matter systems play an important role in optoelectronics and solar energy conversion. Yet it is challenging to understand such multidimensional dynamics at the atomic scale. Combining the real‐time time‐dependent density functional theory with fewest‐switches surface hopping scheme, we develop time‐dependent ab initio nonadiabatic molecular dynamics (NAMD) code Hefei‐NAMD to simulate the excited carrier dynamics in condensed matter systems. Using this method, we have investigated the interfacial charge transfer dynamics, the electron–hole recombination dynamics, and the excited spin‐polarized hole dynamics in different condensed matter systems. The time‐dependent dynamics of excited carriers are studied in energy, real and momentum spaces. In addition, the coupling of the excited carriers with phonons, defects and molecular adsorptions are investigated. The state‐of‐art NAMD studies provide unique insights to understand the ultrafast dynamics of the excited carriers in different condensed matter systems at the atomic scale. This article is categorized under: Structure and Mechanism > Computational Materials Science Molecular and Statistical Mechanics > Molecular Dynamics and Monte‐Carlo Methods Electronic Structure Theory > Ab Initio Electronic Structure Methods Software > Simulation Methods

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Nuclear quantum effects on adsorption of H2 and isotopologues on metal ions

Cited by 12 publications

References 34 publications

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium

An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

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Nuclear quantum effects on adsorption of H2 and isotopologues on metal ions

Cited by 12 publications

References 34 publications

Snowball formation for Cs+ solvation in molecular hydrogen and deuterium

Snowball formation for Cs+ solvation in molecular hydrogen and deuterium

An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

Contact Info

Product

Resources

About

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium

Snowball formation for Cs⁺ solvation in molecular hydrogen and deuterium