Electrochemical
reduction of oxygen molecules can produce H2O2, which is an important chemical for a green
and sustainable society; therefore, the development of catalysts for
this reaction is necessary. We propose mesoporous nitrogen-doped carbon
prepared from (1-methyl-1H-pyrrole-2-yl)methanol in the presence of
a mesoporous SiO2 template (KIT-6). The nitrogen content
of the resulting carbon can be controlled in the range of 0–10
at. % and all prepared samples have well-ordered mesopores
with diameters of 3.4–4.0 nm. Electrochemical studies indicate
the present materials have high catalytic activities with high selectivity
toward H2O2 over 90%. Such high selectivity
toward H2O2 is probably due to good mass transport
in the catalyst layer, which is enhanced by the mesoporous structure.
Two kinds of polyhedral oligomeric silsesquioxane (POSS)-containing block copolymers (BCPs), namely PS-b-PMAPOSS and PMMA-b-PMAPOSS, were synthesized by living anionic polymerization. A wide range of molecular weights were obtained with a very narrow polydispersity index of less than 1.09. The bulk samples prepared by slow evaporation from a polymer solution in chloroform exhibit well-defined microphase-separated structures with long-range order. Thermal annealing induced hierarchical structures consisting of a smaller length scale ordered crystalline POSS domains within the larger microphase-separated structures. We report detailed structural characterization of these hierarchical structures in bulk and thin films by transmission electron microscopy and grazing incidence wide-angle X-ray scattering (GIWAXS). On the basis of this structural analysis, we propose a model for the formation of an orthorhombic lattice structure through the aggregation of POSS segments which formed a helix-like structure.
A series of semiaromatic polyimides containing polyhedral oligomeric silsesquioxane (POSS) in
main chain (POSS−PIs) from a double-decker-shaped silsesquioxane diamine (DDSQ−diamine) (4) with various
aromatic tetracarboxylic dianhydrides were prepared and the structures were characterized by IR and NMR spectra.
A double-decker-shaped silsesquioxane dianhydride (DDSQDA) (3) was synthesized by hydrosilylation reaction
from double-decker-shaped silsesquioxane (DDSQ) (1) and cis-5-norbornene-endo-2,3-dicarboxylic anhydride
(2), which then reacted with 4,4‘-oxydianiline (ODA) to produce the DDSQ-diamine. The POSS−PIs possessed
good thermal stability and mechanical properties, low water absorption, and alkali resistance as well as low
dielectric constant. The 5% weight loss temperatures (T
d
5) in air were observed at 495−514 °C. The polymer
films had good mechanical properties with elongation at breakage of 2.9−6.0%, in which POSS−PI 8c derived
from 4,4‘-oxydiphthalic anhydride (ODPA) exhibits the highest elongation of 6.0%. The water absorption of
POSS−PI 8b (<1%) was much lower than that of PI from pyromellitic dianhydride (PMDA)/ODA (6.0%). POSS−PIs 8 possessed excellent alkaline and acid resistance. POSS−PI 8b kept its flexible mechanical properties when
immersed in 5% NaOH solution at 40 °C for 72 h. The dielectric constant of POSS−PI 8c measured by precision
impedance method was 2.36.
We report the self-assembly of organic-inorganic block copolymers (BCP) in thin-films by simple solvent annealing on unmodified substrates. The resulting vertically oriented lamellae and cylinders are converted to a hard silica mask by a single step highly selective oxygen plasma etching. The size of the resulting nanostructures in the case of cylinders is less than 10 nm.
Self‐organization on three length scales is exhibited by a block copolymer of styrene and an oligothiophene‐bearing isoprene in cast films. For example, a phase‐separated nanostructure consisting of π‐conjugated oligothiophene molecules is self‐aligned perpendicular to the substrate, as revealed in a TEM image of a section through the film (see picture).
A new series of star‐shaped bipolar host molecules, tris(4′‐(1‐phenyl‐1H‐benzimidazol‐2‐yl)biphen‐yl‐4‐yl) amine (TIBN), tris(2′‐methyl‐4′‐(1‐phenyl‐1H‐benzimida zol‐2‐yl)biphenyl‐4‐yl)amine (Me‐TIBN), and tris(2,2′‐dimethyl‐4′‐(1‐phenyl‐1H‐benzimidazol‐2‐yl)biphenyl‐4‐yl)amine (DM‐TIBN), that contain hole‐transporting triphenylamine and electron‐transporting benzimidazole moieties are designed based on calculations using density functional theory and successfully prepared. The theoretical calculation of energy levels of TIBN derivatives affords helpful ideas to design molecules with a favorable localization of highest occupied/lowest unoccupied molecular orbital (HOMO/LUMO) levels and a predefined enhancement of the triplet energy gap. The TIBN derivatives are employed as hosts to fabricate phosphorescent organic light‐emitting diodes (OLEDs) by the two methods of spin‐coating and vacuum deposition. Notably, the spin‐coated Me‐TIBN and DM‐TIBN devices exhibit a much better performance than the vacuum‐deposited ones, in which the spin‐coated DM‐TIBN device (47 500 cd m−2, 27.3 cd A−1, 7.3 lm W−1) is outstanding with respect to other seminal work for solution‐processed OLEDs. More importantly, the new concept of localizing HOMO and LUMO levels for bipolar molecules is illustrated, and a facile strategy to tailor the energy levels by breaking the conjugation of hole‐ and electron‐transporting moieties is demonstrated.
Preparation of low dielectric constant polyimides containing double-decker-shaped silsesquioxane (DDSQ) in the main chain with high molecular weights (η inh ) 0.61 dL/g) is reported. Double-decker-shaped silsesquioxane aromatic tetracarboxylic dianhydride (DDSQDA) was prepared by reaction of DDSQ aromatic diamine and pyromellitic dianhydride through functional group conversion method. The polyimides were synthesized from DDSQDA and several aromatic diamines by a one-step high temperature solution method. Introduction of DDSQ unit in polyimides endowed properties such as solubility in organic solvents, 10% weight loss temperatures (T d10 ) up to 570 °C in nitrogen, the glass transition temperatures (T g ) higher than 300 °C, good mechanical properties (tensile strengths of 72.3-82.1 MPa, initial modulus of 1.8-2.6 GPa, and elongation at breakage of 8.0-15.9%), transmittances over 80% at 400 nm, and a dielectric constant of 2.43 at 1 MHz. The polyimides were soluble in organic solvents such as DMAc, chloroform, THF, and acetone.
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