Absence of spillover of hydrogen adsorbed on small palladium clusters anchored to graphene vacancies

Granja-DelRío, Alejandra; Alducin, M.; Juaristi, J. I.; López, M. J.; Alonso, J. A.

doi:10.1016/j.apsusc.2021.149835

Cited by 21 publications

(14 citation statements)

References 69 publications

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“…60,163 For this reason, realistic dynamical simulations have been performed with the palladium clusters firmly anchored to graphene vacancies. 157 A difference with respect to the case of pristine graphene is that dissociation of H 2 on Pd clusters anchored to graphene vacancies may induce a change in the cluster structure. For instance, a change from the octahedral to the incomplete pentagonal bipyramid in Pd 6 .…”

Section: Hydrogen Adsorption On Carbon Surfaces Doped With Palladiummentioning

confidence: 99%

“…155 These structural changes might have influence on the spillover. Five hundred constant-energy dynamical DFT simulations were performed to investigate the adsorption dynamics of H 2 landing on Pd 6 quasi-saturated with nine H 2 molecules (three dissociated and the rest in the molecular form), with the substrate initially at 0 K. 157 The simulations were run for times of 4 ps. Since cluster saturation coverage is achieved for ten H 2 molecules, in most simulations the landing molecule is scattered back after bouncing against the cluster, because nearly all adsorption sites are already blocked, and only in a few cases the H 2 molecule is adsorbed.…”

Section: Hydrogen Adsorption On Carbon Surfaces Doped With Palladiummentioning

confidence: 99%

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Palladium clusters, free and supported on surfaces, and their applications in hydrogen storage

Alonso

López

2022

Phys. Chem. Chem. Phys.

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Section: Hydrogen Adsorption On Carbon Surfaces Doped With Palladiummentioning

confidence: 99%

Section: Hydrogen Adsorption On Carbon Surfaces Doped With Palladiummentioning

confidence: 99%

Palladium clusters, free and supported on surfaces, and their applications in hydrogen storage

Alonso

López

2022

Phys. Chem. Chem. Phys.

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“…They found that, upon the dissociation at the Pd site, one H atom tends to stay near the Pd site while the other H spills over to a nearby Cu site. In addition, H spillover from Pt and Pd clusters to their graphene substrate was investigated using AIMD, , but the results suggested that the barriers are too high.…”

mentioning

confidence: 99%

“…23 They found that, upon the dissociation at the Pd site, one H atom tends to stay near the Pd site while the other H spills over to a nearby Cu site. In addition, H spillover from Pt and Pd clusters to their graphene substrate was investigated using AIMD, 28,29 but the results suggested that the barriers are too high. On metal surfaces, adsorbate diffusion and reactions are always subjected to energy dissipation via interactions with electron−hole pairs (EHPs) and lattice vibrations, i.e., phonons.…”

mentioning

confidence: 99%

Dynamics of Initial Hydrogen Spillover from a Single Atom Platinum Active Site to the Cu(111) Host Surface: The Impact of Substrate Electron–Hole Pairs

Wei

Cao

et al. 2021

J. Phys. Chem. Lett.

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The initial impulsive diffusion of hot hydrogen atoms resulted from the dissociative chemisorption of H 2 at atomically dispersed Pt atoms embedded in Cu( 111) is investigated using ab initio molecular dynamics. Upon dissociation, one of the two hydrogen atoms tends to roam away from the dissociation site while the other remains trapped. It is shown that the fraction of diffusion and the average diffusion length increase with the incident energy and H 2 vibrational excitation, due apparently to the increased initial kinetic energy of the hot atoms. Most importantly, the strong interaction with surface electron−hole pairs, modeled using an electronic friction model, is shown to play an important role in rapid energy dissipation and significant retardation of the impulsive diffusion.

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“…In order to gauge the accuracy and reduction in computational complexity arising from our Graph-| Q ⟩⟨ C | method presented above, we have applied this approach to a range of hydrogen molecular cluster problems. These systems are critical for applications related to energy storage. − In particular, the safe and efficient storage ,− of molecular hydrogen is of paramount importance to potential developments in new fuel cell technologies. − Furthermore, the study of ortho- and para-hydrogen − at low-temperatures has been a fundamental challenge that has implications toward the study of exotic new states of matter that may have important applications in low-temperature physics. − …”

Section: Resultsmentioning

confidence: 99%

Graph-|Q⟩⟨C|, a Graph-Based Quantum/Classical Algorithm for Efficient Electronic Structure on Hybrid Quantum/Classical Hardware Systems: Improved Quantum Circuit Depth Performance

Zhang

Iyengar

2022

J. Chem. Theory Comput.

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We present a procedure to reduce the depth of quantum circuits and improve the accuracy of results in computing post-Hartree–Fock electronic structure energies in large molecular systems. The method is based on molecular fragmentation where a molecular system is divided into overlapping fragments through a graph-theoretic procedure. This allows us to create a set of projection operators that decompose the unitary evolution of the full system into separate sets of processes, some of which can be treated on quantum hardware and others on classical hardware. Thus, we develop a procedure for an electronic structure that can be asynchronously spawned onto a potentially large ensemble of classical and quantum hardware systems. We demonstrate this method by computing Unitary Coupled Cluster Singles and Doubles (UCCSD) energies for a set of [H2] n clusters, with n ranging from 4 to 128. We implement our methodology using quantum circuits, and when these quantum circuits are processed on a quantum simulator, we obtain energies in agreement with the UCCSD energies in the milli-hartree energy range. We also show that our circuit decomposition approach yields up to 9 orders of magnitude reduction in the number of CNOT gates and quantum circuit depth for the large-sized clusters when compared to a standard quantum circuit implementation available on IBM’s Quantum Information Science kit, known as Qiskit.

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Absence of spillover of hydrogen adsorbed on small palladium clusters anchored to graphene vacancies

Cited by 21 publications

References 69 publications

Palladium clusters, free and supported on surfaces, and their applications in hydrogen storage

Palladium clusters, free and supported on surfaces, and their applications in hydrogen storage

Dynamics of Initial Hydrogen Spillover from a Single Atom Platinum Active Site to the Cu(111) Host Surface: The Impact of Substrate Electron–Hole Pairs

Graph-|Q⟩⟨C|, a Graph-Based Quantum/Classical Algorithm for Efficient Electronic Structure on Hybrid Quantum/Classical Hardware Systems: Improved Quantum Circuit Depth Performance

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