Control of structural ordering in noble metals is very important for the exploration of their properties and applications, and thus it is highly desired to have an in-depth understanding of their structural transitions. Herein, through high-pressure treatment, the mutual transformations between crystalline and amorphous phases are achieved in Pd nanosheets (NSs) and nanoparticles (NPs). The amorphous domains in the amorphous/crystalline Pd NSs exhibit pressure-induced crystallization (PIC) phenomenon, which is considered as the preferred structural response of amorphous Pd under high pressure. On the contrary, in the spherical crystalline@amorphous core-shell Pd NPs, pressure-induced amorphization (PIA) is observed in the crystalline core, in which the amorphous-crystalline phase boundary acts as the initiation site for the collapse of crystalline structure. The distinct PIC and PIA phenomena in two different heterophase Pd nanostructures might originate from the different characteristics of Pd NSs and NPs, including morphology, amorphous-crystalline interface, and lattice parameter. This work not only provides insights into the phase transition mechanisms of amorphous/crystalline heterophase noble metal nanostructures, but also offers an alternative route for engineering noble metals with different phases.
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http://dx.doi.org/10.1002/smll.202106396 | DOI Listing |
J Phys Chem C Nanomater Interfaces
December 2024
Department of Chemistry, College of Staten Island, Staten Island, New York 10314, United States.
Density functional theory calculations and a finite deformation method are used to calculate second- and, most notably, third-order elastic constants of amorphous silicon and amorphous silicon dioxide, as represented by model structures generated via melt-quench force-field molecular dynamics simulations. Linear and nonlinear elastic constants are used to deduce macroscopic elastic moduli, such as the bulk and shear moduli, their pressure derivatives, and the elastic Grüneisen parameter. Our calculations show that the elastic properties of amorphous silicon reach the isotropic elastic limit within the nanometer length scale, attaining characteristics, both linear and nonlinear, comparable to those of crystalline silicon.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Physics, Brooklyn College of the City University of New York, Brooklyn, New York 11210, USA.
We perform classical molecular dynamics (MD) and path-integral MD (PIMD) simulations of H2O and D2O using the q-TIP4P/F model over a wide range of temperatures and pressures to study the nuclear quantum effects (NQEs) on (i) the vitrification of liquid water upon isobaric cooling at different pressures and (ii) pressure-induced transformations at constant temperature between low-density amorphous and high-density amorphous ice (LDA and HDA) and hexagonal ice Ih and HDA. Upon isobaric cooling, classical and quantum H2O and D2O vitrify into a continuum of intermediate amorphous ices (IA), with densities in-between those of LDA and HDA (depending on pressure). Importantly, the density of the IA varies considerably if NQEs are included (similar conclusions hold for ice Ih at all pressures studied).
View Article and Find Full Text PDFInt J Pharm
January 2025
Pharmaceutical Materials Science and Engineering Laboratory, Department of Pharmaceutics, College of Pharmacy, University of Minnesota, Minneapolis, MN 55455, USA. Electronic address:
Spectrochim Acta A Mol Biomol Spectrosc
January 2025
Guangdong Provincial Key Laboratory of Mineral Physics and Materials, 510640, China.
The high-pressure Raman spectra in the low-wavenumber region (50-1200 cm) and the hydroxyl stretching vibration region (2600-3800 cm) of fluorapophyllite-(K) were collected in the interval of 0.0-50.7 GPa.
View Article and Find Full Text PDFJ Phys Chem B
September 2024
Hangzhou Dianzi University, Hangzhou 310018, China.
The barocaloric effect of a solid material is an intense research topic due to its potential application in solid-state refrigeration. Among the proposed candidates, elastic polymers are distinctive because their barocaloric responses are independent from a pressure-induced phase transition which makes it possible to realize a broad working temperature range in principle. However, the barocaloric performance of most elastic polymers diminishes significantly as temperature decreases.
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