It is a challenging task to design efficient Au/Ti-containing catalysts for propene epoxidation with H2 and O2 that simultaneously achieve high catalytic stability and selectivity to propylene oxide (PO). This contribution first describes the synthesis of a nano-crystalline mesoporous titanium silicalite-1 (MTS-1) by dry-gel conversion that employs cheap triblock copolymers as template. Compared with TS-1, MTS-1 has shortened reactant/product diffusion length as a result of smaller crystal size (<100 nm) and presence of mesopores (ca. 3 nm).Surprisingly, this designed catalyst shows simultaneously improved PO selectivity over 95% as well as stability over 40 h, much better than traditional Au/TS-1 catalyst. Moreover, the intrinsic reason for the enhanced performance is elucidated. The better mass transfer ability together with higher hydrophobicity of Au/MTS-1 result in lower coke weight and absence of refractory aromatic coke. In this way, the side reactions and deactivation caused by blocking of micropore are inhibited.
Self-delivery of photosensitizer
and immune modulator to tumor
site is highly recommendable to improve the photodynamic immunotherapy
yet remains challenging. Herein, self-delivery photoimmune stimulators
(designated as iPSs) are developed for photodynamic sensitized tumor
immunotherapy. Carrier-free iPSs are constructed by optimizing the
noncovalent interactions between the pure drugs of chlorine e6 (Ce6)
and NLG919, which avoid the excipients-raised toxicity and immunogenicity.
Intravenously administrated iPSs prefer to passively accumulate on
tumor tissues for a robust photodynamic therapy (PDT) with the induction
of immunogenetic cell death (ICD) cascade to activate cytotoxic T
lymphocytes (CTLs) and initiate antitumor immune response. Meanwhile,
the concomitant delivery of NLG919 inhibits the activation of indoleamine
2,3-dioxygenase 1 (IDO-1) to reverse the immunosuppressive tumor microenvironment.
Ultimately, the photodynamic sensitized immunotherapy with iPSs efficiently
inhibit the primary and distant tumor growth with a low system toxicity,
which would shed light on the development of self-delivery nanomedicine
for clinical transformation in tumor precision therapy.
Green and efficient synthesis of titanium‐containing molecular sieves is limited by the quantity of environmentally unfriendly additives and complicated synthesis procedures required. Oligomerization of Ti monomers into anatase TiO2 is the typical outcome of such procedures because of a mismatch between hydrolysis rates of Si and Ti precursors. We report a simple and generic additive‐free route for the synthesis of Ti‐containing molecular sieves (MFI, MEL, and BEA). This approach successfully reverses the formation of Ti oligomers to match hydrolysis rates of Ti and Si species with the assistance of hydroxyl free radicals generated in situ from ultraviolet irradiation. Moreover, fantastic catalytic performance for propene epoxidation with H2 and O2 was observed. Compared with the conventional hydrothermal method, this approach opens up new opportunities for high‐efficiency, environmentally benign, and facile production of pure titanium‐containing molecular sieves.
Chimeric antigen receptor T (CART) cells targeting CD19 have shown promising results in the treatment of chronic lymphocytic leukemia (CLL). However, efficacy seems to be inferior compared to diffuse large B-cell lymphoma or acute lymphoblastic leukemia. Impaired T-cell fitness of CLL patients may be involved in treatment failure. Less-differentiated naïve-like T cells play an important role in CART expansion and long-term persistence in vivo. These cells are sparse in CLL patients. Therefore, optimization of CART cell production protocols enriching less differentiated T cell subsets may overcome treatment resistance. The B-cell receptor inhibitor ibrutinib targeting Bruton's tyrosine kinase (BTK) is approved for the treatment of CLL. Besides BTK, ibrutinib additionally inhibits interleukin-2-inducible T-cell kinase (ITK) which is involved in T-cell differentiation. To evaluate the effect of ibrutinib on CART cell production, peripheral blood mononuclear cells from nine healthy donors and eight CLL patients were used to generate CART cells. T-cell expansion and phenotype, expression of homing and exhaustion makers as well as functionality of CART cells were evaluated. CART cell generation in the presence of ibrutinib resulted in increased cell viability and expansion of CLL patient-derived CART cells. Furthermore, ibrutinib enriched CART cells with less-differentiated naïve-like phenotype and decreased expression of exhaustion markers including PD-1, TIM-3 and LAG-3. In addition, ibrutinib increased the cytokine release capacity of CLL patient-derived CART cells. In summary, BTK/ITK inhibition with ibrutinib during CART cell culture can improve yield and function of CLL patient-derived CART cell products.
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