The continuous selective oxidation of p-xylene (p-X) by O 2 (generated by thermal decomposition of aqueous H 2 O 2 ) catalyzed by MnBr 2 in supercritical H 2 O at ca. 400 °C is reported for the first time. The selectivity for terephthalic acid (TA) is > 90%. Compared to existing industrial processes, the reaction has the potential for a significant increase in energy efficiency and a substantial reduction in waste. This reaction is significant because the presence of H 2 O lowers the catalytic activity of MnBr 2 in the conventional route to TA via oxidation of p-X in CH 3 COOH.
A new preparative route for vanadium phosphate catalysts is described using supercritical CO2 as an antisolvent. The amorphous microspheroidal VPO produced is shown to be more active than comparable crystalline VPO catalysts for the selective oxidation of n-butane to maleic anhydride and, furthermore, does not require an extensive pre-treatment or activation period to establish full catalytic activity. VPO catalysts prepared using supercritical CO2 as an antisolvent maintain their amorphous nature throughout the catalyst test period. In contrast, amorphous VPO catalysts can also be prepared using liquid CO2 as antisolvent, or by solvent evaporation in vacuo, however, these materials are found to partially crystallise during the oxidation of n-butane. The wholly amorphous catalysts are characterised using transmission electron microscopy, X-ray absorption spectroscopy, 31 P spin echo mapping NMR spectroscopy and X-ray photoelectron spectroscopy. The role of amorphous material in vanadium phosphate catalysis is discussed in detail.
Chemokine-induced T lymphocyte recruitment to the lung is critical for allergic inflammation, but chemokine signaling pathways are incompletely understood. Regulator of G protein signaling (RGS)16, a GTPase accelerator (GTPase-activating protein) for Gα subunits, attenuates signaling by chemokine receptors in T lymphocytes, suggesting a role in the regulation of lymphocyte trafficking. To explore the role of RGS16 in T lymphocyte-dependent immune responses in a whole-organism model, we generated transgenic (Tg) mice expressing RGS16 in CD4+ and CD8+ cells. rgs16 Tg T lymphocytes migrated to CC chemokine ligand 21 or CC chemokine ligand 12 injection sites in the peritoneum, but not to CXC chemokine ligand 12. In a Th2-dependent model of allergic pulmonary inflammation, CD4+ lymphocytes bearing CCR3, CCR5, and CXCR4 trafficked in reduced numbers to the lung after acute inhalation challenge with allergen (OVA). In contrast, spleens of sensitized and challenged Tg mice contained increased numbers of CD4+CCR3+ cells producing more Th2-type cytokines (IL-4, IL-5, and IL-13), which were associated with increased airway hyperreactivity. Migration of Tg lymphocytes to the lung parenchyma after adoptive transfer was significantly reduced compared with wild-type lymphocytes. Naive lymphocytes displayed normal CCR3 and CXCR4 expression and cytokine responses, and compartmentation in secondary lymphoid organs was normal without allergen challenge. These results suggest that RGS16 may regulate T lymphocyte activation in response to inflammatory stimuli and migration induced by CXCR4, CCR3, and CCR5, but not CCR2 or CCR7.
The intercalation of ethane and ethene into the octahedral interstitial sites of the C60 lattice can be achieved by antisolvent precipitation, using supercritical C2H4 and C2H6. This method of crystallization (see picture), which has yielded unprecedented intercalation compounds with hydrocarbons once thought too large to form such species, should be applicable to other gases, solvents, and fullerenes.
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