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From the aerial parts of <i>Senecio dianthus</i>, four new eremophilenolides (<b>1</b>-<b>4</b>, resp.) and one new eremophilenolide alkaloid (<b>5</b>), of the relatively uncommon eremophilenoid-type sesquiterpenoid lactones, were isolated together with three known sesquiterpenoid lactones, 10<i>β</i>-hydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>6</b>), 8<i>β</i>,10<i>β</i>-dihydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>7</b>), and 10<i>α</i>-hydroxy-1-oxoeremophila-7(11),8(9)-dien-12,8-olide (<b>8</b>). On the basis of IR, MS, and NMR data, particularly 2D-NMR analyses, the structures of the new compounds were established as: 2<i>β</i>-(angeloyloxy)-10<i>β</i>-hydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>1</b>), 6<i>β</i>-(angeloyloxy)-10<i>β</i>-hydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>2</b>), 2<i>β</i>-(angeloyloxy)-8<i>β</i>,10<i>β</i>-dihydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>3</b>), 2<i>β</i>-(angeloyloxy)-8<i>α</i>-hydroxyeremophila-7(11),9(10)-dien-12,8<i>β</i>-olide (<b>4</b>), and 8<i>β</i>-amino-10<i>β</i>-hydroxyeremophil-7(11)-en-12,8<i>α</i>-olide (<b>5</b>). In addition, the relative configuration of <b>1</b> was corroborated by X-ray diffraction analysis.