4

Summary

4 (four) is a number, numeral and digit. It is the natural number following 3 and preceding 5. It is a square number, the smallest semiprime and composite number, and is considered unlucky in many East Asian cultures. Evolution of the Hindu-Arabic digit Brahmic numerals represented 1, 2, and 3 with as many lines. 4 was simplified by joining its four lines into a cross that looks like the modern plus sign. The Shunga would add a horizontal line on top of the digit, and the Kshatrapa and Pallava evolved the digit to a point where the speed of writing was a secondary concern. The Arabs' 4 still had the early concept of the cross, but for the sake of efficiency, was made in one stroke by connecting the "western" end to the "northern" end; the "eastern" end was finished off with a curve. The Europeans dropped the finishing curve and gradually made the digit less cursive, ending up with a digit very close to the original Brahmin cross. While the shape of the character for the di

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Background: Angipoietin-1 activation of the tyrosine kinase receptor Tek expressed mainly on endothelial cells leads to survival and stabilization of endothelial cells. Studies have shown that Angiopoietin-1 counteracts permeability induced by a number of stimuli. Here, we test the hypothesis that loss of Angiopoietin-1/Tek signaling in the vasculature would increase metastasis. Methods: Angiopoietin-1 was deleted in mice just before birth using floxed Angiopoietin-1 and Tek mice crossed to doxycycline-inducible bitransgenic ROSA-rtTA/tetO-Cre mice. By crossing Angiopoietin-1 knockout mice to the MMTV-PyMT autochthonous mouse breast cancer model, we investigated primary tumor growth and metastasis to the lung. Furthermore, we utilized B16F10 melanoma cells subcutaneous and experimental lung metastasis models in Angiopoietin-1 and Tek knockout mice. Results: We found that primary tumor growth in MMTV-PyMT mice was unaffected, while metastasis to the lung was significantly increased in Angiopoietin-1 knockout MMTV-PyMT mice. In addition, angiopoietin-1 deficient mice exhibited a significant increase in lung metastasis of B16F10 melanoma cells, compared to wild type mice 3 weeks after injection. Additional experiments showed that this was likely an early event due to increased attachment or extravasation of tumor cells, since seeding of tumor cells was significantly increased 4 and 24 h post tail vein injection. Finally, using inducible Tek knockout mice, we showed a significant increase in tumor cell seeding to the lung, suggesting that Angiopoietin-1/Tek signaling is important for vascular integrity to limit metastasis. Conclusions: This study show that loss of the Angiopoietin-1/Tek vascular growth factor system leads to increased metastasis without affecting primary tumor growth.

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Metathesis of a U(V) imido complex: a route to a terminal U(V) sulfide

Marta Falcone, Rory Patrick Kelly, Marinella Mazzanti, Rosario Scopelliti

Herein, we report the synthesis and characterisation of the first terminal uranium(V) sulfide and a related UV trithiocarbonate complex supported by sterically demanding tris(tert-butoxy)siloxide ligands. The reaction of the potassium-bound UV imido complex, [U(NAd){OSi(OtBu)3}4K] (4), with CS2 led to the isolation of perthiodicarbonate [K(18c6)]2[C2S6] (6), with concomitant formation of the UIV complex, [U{OSi(OtBu)3}4], and S[double bond, length as m-dash]C[double bond, length as m-dash]NAd. In contrast, the reaction of the UV imido complex, [K(2.2.2-cryptand)][U(NAd){OSi(OtBu)3}4] (5), with one or two equivalents of CS2 afforded the trithiocarbonate complex, [K(2.2.2-cryptand)][U(CS3){OSi(OtBu)3}4] (7), which was isolated in 57% yield, with concomitant elimination of the admantyl thiocyanate product, S[double bond, length as m-dash]C[double bond, length as m-dash]NAd. Complex 7 is likely formed by fast nucleophilic addition of a UV terminal sulfide intermediate, resulting from the slow metathesis reaction of the imido complex with CS2, to a second CS2 molecule. The addition of a solution of H2S in thf (1.3 eq.) to 4 afforded the first isolable UV terminal sulfide complex, [K(2.2.2-cryptand)][US{OSi(OtBu)3}4] (8), in 41% yield. Based on DFT calculations, triple-bond character with a strong covalent interaction is suggested for the U–S bond in complex 7.

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Trifluoromethoxy Substituted Anilines: Metalation as the Key Step for Structural Elaboration

Trifluoromethoxy-substituted anilines undergo hydrogen/lithium permutation ("metalation") with optional site selectivity depending on the N-protective group employed. N-tert-Butoxycarbonyl-2- and -4-(trifluoromethoxy)aniline react with tert-BuLi at the nitrogen-adjacent 6- and 2-position affording, after electrophilic trapping, the corresponding substituted anilines I (R1 = F3CO, R2 = H, R3 = HO2C; R1 = H, R2 = F3CO, R3 = Me, CHO, HO2C, HOCH2CH2). In contrast, deprotonation of the N,N-bis(trimethylsilyl)-substituted 4-(trifluoromethoxy)aniline occurs at the oxygen-neighboring 3-position. Sec-BuLi attacks 3-trifluoromethoxy-N-(trimethylsilyl)aniline at the 2-position, but 3-trifluoromethoxy-N,N-bis(trimethylsilyl)aniline at the 4-position to provide the corresponding acids II (R4 = HO2C, R5 = H; R4 = H, R5 = HO2C), resp., after carboxylation. The synthesis of two new benzodiazepines III (R6 = F3CO, R7 = H, R8 = F; R6 = Cl, R7 = HO, R8 = F3CO) illustrates the preparative potential of the aniline functionalization mediated by organometallic reagents. [on SciFinder (R)]

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