Institution
Fritz Haber Institute of the Max Planck Society
Facility•Berlin, Germany•
About: Fritz Haber Institute of the Max Planck Society is a facility organization based out in Berlin, Germany. It is known for research contribution in the topics: Catalysis & Adsorption. The organization has 3490 authors who have published 5017 publications receiving 183731 citations. The organization is also known as: Fritz Haber Institute of the Max Planck Society.
Papers published on a yearly basis
Papers
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TL;DR: This work builds upon the previously developed many-body dispersion framework and proposes an effective range-separation of the coupling between the atomic response functions that extends the already broad applicability of the MBD method to non-metallic materials with highly anisotropic responses, such as layered nanostructures.
Abstract: An accurate determination of the electron correlation energy is an essential prerequisite for describing the structure, stability, and function in a wide variety of systems. Therefore, the development of efficient approaches for the calculation of the correlation energy (and hence the dispersion energy as well) is essential and such methods can be coupled with many density-functional approximations, local methods for the electron correlation energy, and even interatomic force fields. In this work, we build upon the previously developed many-body dispersion (MBD) framework, which is intimately linked to the random-phase approximation for the correlation energy. We separate the correlation energy into short-range contributions that are modeled by semi-local functionals and long-range contributions that are calculated by mapping the complex all-electron problem onto a set of atomic response functions coupled in the dipole approximation. We propose an effective range-separation of the coupling between the atomic response functions that extends the already broad applicability of the MBD method to non-metallic materials with highly anisotropic responses, such as layered nanostructures. Application to a variety of high-quality benchmark datasets illustrates the accuracy and applicability of the improved MBD approach, which offers the prospect of first-principles modeling of large structurally complex systems with an accurate description of the long-range correlation energy.
509 citations
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TL;DR: In this article, the potential difference between monolayer and bulk deposition is closely related to the difference in the work functions of substrate and deposit, causing a partial charge of the adatoms.
500 citations
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TL;DR: It is shown that a conceptually simple top-down grid partitioning scheme achieves essentially the same efficiency as the more rigorous bottom-up approaches.
481 citations
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TL;DR: It is shown that the inclusion of the many-body collective response of the substrate electrons inside the inorganic bulk enables us to reliably predict the HIOS geometries and energies.
Abstract: The electronic properties and the function of hybrid inorganic-organic systems (HIOS) are intimately linked to their interface geometry. Here we show that the inclusion of the many-body collective response of the substrate electrons inside the inorganic bulk enables us to reliably predict the HIOS geometries and energies. This is achieved by the combination of dispersion-corrected density-functional theory (the DFTþ van der Waals approach) [Phys. Rev. Lett. 102, 073005 (2009)], with the Lifshitz-Zaremba-Kohn theory for the nonlocal Coulomb screening within the bulk. Our method yields geometries in remarkable agreement (� 0:1 � A) with normal incidence x-ray standing wave measurements for the 3, 4, 9, 10-perylene-tetracarboxylic acid dianhydride (C24O6H8, PTCDA) molecule on Cu(111), Ag(111), and Au(111) surfaces. Similarly accurate results are obtained for xenon and benzene adsorbed on metal surfaces.
474 citations
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TL;DR: The flexible electronic structure of the surface Fe sites, and their synergy with nearest-neighbor M sites through formation of O-bridged Fe-M reaction centers, stabilize OER intermediates that are unfavorable on pure M-M centers and single Fe Sites, fundamentally accounting for the high catalytic activity of MFe LDHs.
Abstract: NiFe and CoFe (MFe) layered double hydroxides (LDHs) are among the most active electrocatalysts for the alkaline oxygen evolution reaction (OER). Herein, we combine electrochemical measurements, operando X-ray scattering and absorption spectroscopy, and density functional theory (DFT) calculations to elucidate the catalytically active phase, reaction center and the OER mechanism. We provide the first direct atomic-scale evidence that, under applied anodic potentials, MFe LDHs oxidize from as-prepared α-phases to activated γ-phases. The OER-active γ-phases are characterized by about 8% contraction of the lattice spacing and switching of the intercalated ions. DFT calculations reveal that the OER proceeds via a Mars van Krevelen mechanism. The flexible electronic structure of the surface Fe sites, and their synergy with nearest-neighbor M sites through formation of O-bridged Fe-M reaction centers, stabilize OER intermediates that are unfavorable on pure M-M centers and single Fe sites, fundamentally accounting for the high catalytic activity of MFe LDHs. NiFe and CoFe layered double hydroxides are among the most active electrocatalysts for the alkaline oxygen evolution reaction. Here, by combining operando experiments and rigorous DFT calculations, the authors unravel their active phase, the reaction center and the catalytic mechanism.
459 citations
Authors
Showing all 3514 results
Name | H-index | Papers | Citations |
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Jens K. Nørskov | 184 | 706 | 146151 |
Qiang Zhang | 161 | 1137 | 100950 |
William A. Goddard | 151 | 1653 | 123322 |
Matthias Scheffler | 125 | 752 | 61011 |
Tao Zhang | 123 | 2772 | 83866 |
Gerhard Ertl | 120 | 720 | 57560 |
James A. Dumesic | 118 | 615 | 58935 |
Angel Rubio | 110 | 930 | 52731 |
Pavel Hobza | 107 | 564 | 48080 |
Hans-Joachim Freund | 106 | 962 | 46693 |
Xinhe Bao | 103 | 828 | 46524 |
Peter Strasser | 100 | 357 | 37374 |
Dang Sheng Su | 99 | 615 | 36117 |
Robert Schlögl | 92 | 706 | 33795 |
Gianfranco Pacchioni | 91 | 622 | 32262 |