Heterogeneous catalysts that contain bimetallic nanoparticles may undergo segregation of the metals, driven by oxidizing and reducing environments. The structure and composition of core-shell Rh 0.5 Pd 0.5 and Pt 0.5 Pd 0.5 nanoparticle catalysts were studied in situ, during oxidizing, reducing, and catalytic reactions involving NO, O 2 , CO, and H 2 by x-ray photoelectron spectroscopy at near-ambient pressure. The Rh 0.5 Pd 0.5 nanoparticles underwent dramatic and reversible changes in composition and chemical state in response to oxidizing or reducing conditions. In contrast, no substantial segregation of Pd or Pt atoms was found in Pt 0.5 Pd 0.5 nanoparticles. The different behaviors in restructuring and chemical response of Rh 0.5 Pd 0.5 and Pt 0.5 Pd 0.5 nanoparticle catalysts under the same reaction conditions illustrates the flexibility and tunability of the structure of bimetallic nanoparticle catalysts during catalytic reactions.
A combination of photoemission and scanning tunnelling spectroscopy measurements provide compelling evidence that single layers of 1T'-WTe2 are a class of quantum spin Hall insulator. A quantum spin Hall (QSH) insulator is a novel two-dimensional quantum state of matter that features quantized Hall conductance in the absence of a magnetic field, resulting from topologically protected dissipationless edge states that bridge the energy gap opened by band inversion and strong spin–orbit coupling1,2. By investigating the electronic structure of epitaxially grown monolayer 1T'-WTe2 using angle-resolved photoemission (ARPES) and first-principles calculations, we observe clear signatures of topological band inversion and bandgap opening, which are the hallmarks of a QSH state. Scanning tunnelling microscopy measurements further confirm the correct crystal structure and the existence of a bulk bandgap, and provide evidence for a modified electronic structure near the edge that is consistent with the expectations for a QSH insulator. Our results establish monolayer 1T'-WTe2 as a new class of QSH insulator with large bandgap in a robust two-dimensional materials family of transition metal dichalcogenides (TMDCs).
24 July 2014 in Physical Chemistry Chemical Physics
From Steps to Clusters: When a flat surface of a single crystal is formed by cutting or cleavage, the atoms may move little from their bulk positions, or the surface may reconstruct as the atoms move to more energetically favorable positions. The adsorption of molecules can also change the energetic landscape and cause reconstruction.
Tao
et al. (p. 850 ; see the Perspective by Altman ) examined “stepped” platinum surfaces, the (557) and (332) surfaces in which flat terraces are connected by atomic steps. Scanning tunneling microscopy and x-ray photoelectron spectroscopy revealed a reversible breakup into nanometer-scale clusters when CO surface coverages were very high. Density functional theory calculations suggest that this new morphology increases the number of edge sites for adsorption and relieves unfavorable CO-CO repulsions.
5 January 2016 in The Journal of Physical Chemistry C
Heterogeneous chemical reactions at vapor/solid interfaces play an important role in many processes in the environment and technology. Ambient pressure X-ray photoelectron spectroscopy (APXPS) is a valuable tool to investigate the elemental composition and chemical specificity of surfaces and adsorbates on the molecular scale at pressures of up to 130 mbar. In this review we summarize the historical development of APXPS since its introduction over forty years ago, discuss different approaches to minimize scattering of electrons by gas molecules, and give a comprehensive overview about the experimental systems (vapor/solid interfaces) that have been studied so far. We also present several examples for the application of APXPS to environmental science, heterogeneous catalysis, and electrochemistry.