A goal in the characterization of supported metal catalysts is to achieve particle-by-particle analysis of the charge state strongly correlated with the catalytic activity. Here, we demonstrate the direct identification of the charge state of individual platinum nanoparticles (NPs) supported on titanium dioxide using ultrahigh sensitivity and precision electron holography. Sophisticated phase-shift analysis for the part of the NPs protruding into the vacuum visualized slight potential changes around individual platinum NPs. The analysis revealed the number (only one to six electrons) and sense (positive or negative) of the charge per platinum NP. The underlying mechanism of platinum charging is explained by the work function differences between platinum and titanium dioxide (depending on the orientation relationship and lattice distortion) and by first-principles calculations in terms of the charge transfer processes.
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http://dx.doi.org/10.1126/science.abq5868 | DOI Listing |
J Phys Chem A
December 2024
Lawrence Livermore National Laboratory, Livermore, California 94550, United States.
Loewdin charges from density functional theory calculations were used here to obtain general, univariate linear correlations for the prediction of experimental Hammett parameters and relative reaction rates. While previous studies have established that Hirshfeld and CM5 charges perform strongly as univariate predictors, the near-ubiquitous Loewdin charges have not yet been evaluated. To this end, we assess the predictive capability of Loewdin charges for three chemical systems.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Henan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
The conversion of methane and carbon dioxide to form C products is of great interest but presents a long-standing grand challenge due to the significant obstacle of activating the inert C-H and C═O bonds as well as forming the C-C bonds. Herein, the consecutive C-C coupling of CH and CO was realized by using heteronuclear metal cations CuTa, and the desorption of HC═C═O molecules was evidenced by state-of-the-art mass spectrometry. The CuTa reaction system is significantly different from the homonuclear metal systems of Cu and Ta.
View Article and Find Full Text PDFJ Sci Food Agric
December 2024
College of Ocean Food and Biological Engineering, Jimei University, Xiamen, China.
Background: It is important to study the physicochemical properties of tilapia (Oreochromis mossambicus) skin gelatin and the changes in dipeptidyl peptidase IV (DPP-IV) inhibition activity during gastrointestinal digestion in order to understand and exploit the potential of tilapia as a source of DPP-IV inhibitory peptides.
Results: The DPP-IV inhibition of fish-skin gelatin increased from 9.92 ± 0.
Chem Sci
December 2024
Department of Physical Chemistry, University of Málaga, Andalucia-Tech Campus de Teatinos s/n 29071 Málaga Spain
The synthesis, electrochemical, spectroelectrochemical, photophysical and light induced electron transfer reactions in two new anthanthrene quinodimethanes have been studied and analyzed in the context of dynamic electrochemistry. Their properties are dependent on the interconversion between folded and twisted forms, which are separated by a relatively small energy range, thus allowing to explore their interconversion by variable temperature measurements. The photophysics of these molecules is mediated by a diradical excited state with a twisted structure that habilitates rapid intersystem crossing.
View Article and Find Full Text PDFVavilovskii Zhurnal Genet Selektsii
November 2024
Institute of Cytology and Genetics of the Siberian Branch of the Russian Academy of Sciences, Novosibirsk, Russia.
We present a series of articles proving the existence of a previously unknown mechanism of interaction between hematopoietic stem cells and extracellular double-stranded DNA (and, in particular, double-stranded DNA of the peripheral bloodstream), which explains the possibility of emergence and fixation of genetic information contained in double-stranded DNA of extracellular origin in hematopoietic stem cells. The concept of the possibility of stochastic or targeted changes in the genome of hematopoietic stem cells is formulated based on the discovery of new, previously unknown biological properties of poorly differentiated hematopoietic precursors. The main provisions of the concept are as follows.
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