We have studied the effect of confinement and correlations on the plasmon dispersion in an atom-scale metallic wire by determining the electron density response function. The wire electrons are modelled as comprising a quasi-one-dimensional homogeneous gas, with different transverse confinement models. The response function is calculated by including electron correlations beyond the random-phase approximation within the self-consistent mean-field approach of Singwi et al (1968 Phys. Rev. 176 589). The plasmon dispersion results are found to be in very good agreement with the recent electron-energy-loss spectroscopy measurements by Nagao et al (2006 Phys. Rev. Lett. 97 116802). However, our predictions are found to depend strongly on the nature of the confinement model, the structure of the one-dimensional electronic band and the electron effective mass, implying a crucial role for the wire structure.
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http://dx.doi.org/10.1088/0953-8984/22/13/135003 | DOI Listing |
J Am Chem Soc
January 2025
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore.
The bifunctional mechanism, involving multiactive compositions to simultaneously dissociate water molecules and optimize intermediate adsorption, has been widely used in the design of catalysts to boost water electrolysis for sustainable hydrogen energy production but remains debatable due to difficulties in accurately identifying the reaction process. Here, we proposed the concept of well-defined Lewis pairs in single-atom catalysts, with a unique acid-base nature, to comprehensively understand the exact role of multiactive compositions in an alkaline hydrogen evolution reaction. By facilely adjusting active moieties, the induced synergistic effect between Lewis pairs (M-P/S/Cr pairs, M = Ru, Ir, Pt) can significantly facilitate the cleavage of the H-OH bond and accelerate the removal of intermediates, thereby switching the rate-determining step from the Volmer step to the Heyrovsky step.
View Article and Find Full Text PDFAdv Mater
November 2024
Department of Physics, Nanoscience Center, University of Jyväskylä, Jyväskylä, FI-40014, Finland.
Hybrid nanostructures between biomolecules and inorganic nanomaterials constitute a largely unexplored field of research, with the potential for novel applications in bioimaging, biosensing, and nanomedicine. Developing such applications relies critically on understanding the dynamical properties of the nano-bio interface. This work introduces and validates a strategy to predict atom-scale interactions between water-soluble gold nanoclusters (AuNCs) and a set of blood proteins (albumin, apolipoprotein, immunoglobulin, and fibrinogen).
View Article and Find Full Text PDFACS Cent Sci
June 2024
Department of Chemistry, University of Washington, Seattle, Washington 98195, United States.
Directing groups guide substitution patterns in organic synthetic schemes, but little is known about pathways to control reactivity patterns, such as regioselectivity, in complex inorganic systems such as bioinorganic cofactors or extended surfaces. Interadsorbate effects are known to encode surface reactivity patterns in inorganic materials, modulating the location and binding strength of ligands. However, owing to limited experimental resolution into complex inorganic structures, there is little opportunity to resolve these effects on the atomic scale.
View Article and Find Full Text PDFJ Hazard Mater
June 2024
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China. Electronic address:
The metal organic framework (MOFs)-derived porous carbon materials with highly dispersed metal active sites were of the exclusive application foreground in many field, such as catalyst, electrochemistry, adsorption desulfurization and so on. However, the loss issue of metal active sites in MOFs frame was indispensable during the high temperature carbonization because of the lower boiling point of many metals, thus fundamentally affecting the atom-scale uniform distribution merit of MOFs-derived porous carbon materials. This work was to provide a novel strategy to address the loss issue of the active metal volatilization in the fabrication of MOFs-derived porous carbon materials.
View Article and Find Full Text PDFNat Commun
April 2024
State Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Tianfu Institute of Research and Innovation, Southwest University of Science and Technology, Mianyang, 621010, China.
Engineering atom-scale sites are crucial to the mitigation of polysulfide shuttle, promotion of sulfur redox, and regulation of lithium deposition in lithium-sulfur batteries. Herein, a homonuclear copper dual-atom catalyst with a proximal distance of 3.5 Å is developed for lithium-sulfur batteries, wherein two adjacent copper atoms are linked by a pair of symmetrical chlorine bridge bonds.
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