We report the first use of high-energy monochromatic in situ X-ray powder diffraction to gain unprecedented insights into the chemical processes occurring during high temperature, lab-scale metal oxide syntheses. During the flux synthesis of the n = 4 Aurivillius phase, BiTiFeCrO at 950 °C in molten NaSO we observe the progression of numerous metastable phases. Using sequential multiphase Rietveld refinement of the time-dependent in situ XRD data, we are able to obtain mechanistic understanding of this reaction under a range of conditions.
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http://dx.doi.org/10.1039/c6cc08133a | DOI Listing |
ACS Nano
January 2025
Faculty III Process Sciences, Institute of Materials Science and Technology, Chair of Advanced Ceramic Materials, Technische Universität Berlin, Straße des 17. Juni 135, 10623 Berlin, Germany.
Metastable, , kinetically favored but thermodynamically not stable, interstitial solid solutions of carbon in iron are well-understood. Carbon can occupy the interstitial atoms of the host metal, altering its properties. Alloying of the host metal results in the stabilization of the FeC phases, widening its application.
View Article and Find Full Text PDFCommun Chem
January 2025
Energy & Materials Transition, Netherlands Organization for Applied Scientific Research (TNO), Urmonderbaan 22, Geleen, 6167RD, The Netherlands.
Time-resolved coherent Raman spectroscopy (CRS) is a powerful non-linear optical technique for quantitative, in-situ analysis of chemically reacting flows, offering unparalleled accuracy and exceptional spatiotemporal resolution. Its application to large polyatomic molecules, crucial for understanding reaction dynamics, has thus far been limited by the complexity of their rotational-vibrational Raman spectra. Progress in developing comprehensive spectral codes for these molecules, a longstanding goal, has been hindered by prohibitively long computation times required for their spectral synthesis.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
William H. Miller III Department of Physics and Astronomy, The Johns Hopkins University, Baltimore, MD 21218.
Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet CrFPiv. The octagonal rings of magnetic Cr atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Northeast Normal University, Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education, Institute of Functional Material Chemistry, Local United Engineering Lab for Power Battery, CHINA.
Construction of metal-organic cages (MOCs) with internal modifications is a promising avenue to build enzyme-like cavities and unlocking the mystery of highly catalytic activity and selectivity of enzymes. However, current interests are mainly focused on single-metal-node cages, little achievement has been expended to metalloclusters-based architectures, and the in situ endogenous generation of metal clusters. Herein, based on the hard-soft-acids-bases (HSAB), the metalloclusters-based heterometallic MOC (Cu3VMOP) constructed of [Cu3OPz3]+ and [V6O6(OCH3)9(SO4)(CO2)3]2- clusters was obtained by one-pot method.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Department of Chemical and Biomolecular Engineering, 250 Nieuwland Hall, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Nonthermal plasma-surface interactions enable transformative advancements in green chemistry, healthcare, materials processing, pollution abatement, and the ever-growing area of plasma catalysis. In the context of plasma catalysis, the fate of the active sites during plasma treatment has remained enigmatic, and observation of low-temperature plasma-catalyst events has been challenging. The induction of strong metal-support interactions (SMSI) through high-temperature hydrogen treatment is a well-documented and established, yet limited, method to impact selectivity and stability of noble metal catalysts on reducible supports.
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