5 research outputs found
sj-rar-1-dcm-10.1177_17504813231158526 – for A contrastive study of discoursal emotions between China’s and American newspapers from the perspective of Socio-emotional Theory: The case of the reports on Hong Kong National Security Law
sj-rar-1-dcm-10.1177_17504813231158526 for A contrastive study of discoursal emotions between China’s and American newspapers from the perspective of Socio-emotional Theory: The case of the reports on Hong Kong National Security Law by Zhuo Peng and Jianbo Hou in Discourse & Communication</p
Copolymerization of Ethylene and 1,4–Pentadiene: Structure Characterization and Reaction Mechanism
Copolymerization of ethylene and 1,4-pentadiene was conducted
by
using a homogeneous catalyst to understand the insertion mode of 1,4-pentadiene.
The polymer microstructure of the synthesized material was subjected
to structural characterization using quantitative NMR spectroscopy,
diffusometry, two-dimensional correlation spectroscopy, and selectively
refocused insensitive nuclei enhanced by polarization transfer (Sel-RINEPT).
The multimodal NMR characterization allows effective differentiation
of chain ends and backbone signals, filters irrelevant spectral information,
and provides site-specific information to achieve unambiguous structural
elucidation. The experimental results reveal that pentadiene has been
primarily converted to cis- and trans-dialkyl-substituted cyclohexane moieties along the polymer backbone
over the course of polymerization. The analysis also confirms that
unreacted pendant allyl groups from pentadiene remain at a concentration
that is significantly lower than the cyclic structures. In comparison
to the literature results, some discrepancies in structural assignment
have been identified and the results will be discussed. Detailed molecular
structure elucidation provides critical insights into advancing the
understanding of the reaction mechanism
Development of Improved Amidoquinoline Polyolefin Catalysts with Ultrahigh Molecular Weight Capacity
A new
synthetic route to amidoquinoline olefin polymerization catalysts
has been developed involving significantly less expensive and more
readily available starting materials. The new methodology was used
to prepare <i>N</i>-mesityl-2-methylquinolin-8-amine, which
in turn was converted into trialkyl complexes of Hf, Zr, and Ti. The
new complexes were characterized by elemental analysis, 1D and 2D
NMR spectroscopy, and X-ray crystallography. A batch reactor ethylene/1-octene
copolymerization evaluation at 140 °C showed that the new Hf
congener outperformed a series of previously reported molecular olefin
polymerization catalysts. In particular, the new Hf catalyst exhibits
excellent activity and a remarkable capacity to produce ultrahigh
molecular weight copolymers at elevated reaction temperatures
Minimal Proton Channel Enables H<sub>2</sub> Oxidation and Production with a Water-Soluble Nickel-Based Catalyst
Hydrogenase
enzymes use first-row transition metals to interconvert
H<sub>2</sub> with protons and electrons, reactions that are important
for the storage and recovery of energy from intermittent sources such
as solar, hydroelectric, and wind. Here we present NiÂ(P<sup>Cy</sup><sub>2</sub>N<sup>Gly</sup><sub>2</sub>)<sub>2</sub>, a water-soluble
molecular electrocatalyst with the amino acid glycine built into the
diphosphine ligand framework. Proton transfer between the outer coordination
sphere carboxylates and the second coordination sphere pendant amines
is rapid, as observed by cyclic voltammetry and FTIR spectroscopy,
indicating that the carboxylate groups may participate in proton transfer
during catalysis. This complex oxidizes H<sub>2</sub> (1–33
s<sup>–1</sup>) at low overpotentials (150–365 mV) over
a range of pH values (0.1–9.0) and produces H<sub>2</sub> under
identical solution conditions (>2400 s<sup>–1</sup> at pH
0.5).
Enzymes employ proton channels for the controlled movement of protons
over long distancesî—¸the results presented here demonstrate
the effects of a simple two-component proton channel in a synthetic
molecular electrocatalyst
Interaction of Au with Thin ZrO<sub>2</sub> Films: Influence of ZrO<sub>2</sub> Morphology on the Adsorption and Thermal Stability of Au Nanoparticles
The model catalysts of ZrO<sub>2</sub>-supported Au nanoparticles
have been prepared by deposition of Au atoms onto the surfaces of
thin ZrO<sub>2</sub> films with different morphologies. The adsorption
and thermal stability of Au nanoparticles on thin ZrO<sub>2</sub> films
have been investigated using synchrotron radiation photoemission spectroscopy
(SRPES) and X-ray photoelectron spectroscopy (XPS). The thin ZrO<sub>2</sub> films were prepared by two different methods, giving rise
to different morphologies. The first method utilized wet chemical
impregnation to synthesize the thin ZrO<sub>2</sub> film through the
procedure of first spin-coating a zirconium ethoxide (ZrÂ(OC<sub>2</sub>H<sub>5</sub>)<sub>4</sub>) precursor onto a SiO<sub>2</sub>/SiÂ(100)
substrate at room temperature followed by calcination at 773 K for
12 h. Scanning electron microscopy (SEM) investigations indicate that
highly porous “sponge-like nanostructures” were obtained
in this case. The second method was epitaxial growth of a ZrO<sub>2</sub>(111) film through vacuum evaporation of Zr metal onto Pt(111)
in 1 × 10<sup>–6</sup> Torr of oxygen at 550 K followed
by annealing at 1000 K. The structural analysis with low energy electron
diffraction (LEED) of this film exhibits good long-range ordering.
It has been found that Au forms smaller particles on the porous ZrO<sub>2</sub> film as compared to those on the ordered ZrO<sub>2</sub>(111)
film at a given coverage. Thermal annealing experiments demonstrate
that Au particles are more thermally stable on the porous ZrO<sub>2</sub> surface than on the ZrO<sub>2</sub>(111) surface, although
on both surfaces, Au particles experience significant sintering at
elevated temperatures. In addition, by annealing the surfaces to 1100
K, Au particles desorb completely from ZrO<sub>2</sub>(111) but not
from porous ZrO<sub>2</sub>. The enhanced thermal stability for Au
on porous ZrO<sub>2</sub> can be attributed to the stronger interaction
of the adsorbed Au with the defects and the hindered migration or
coalescence resulting from the porous structures