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Athanassios K. Boudalis - One of the best experts on this subject based on the ideXlab platform.

  • aerobic feiii feii reduction in the presence of 2 4 6 tri 2 pyridyl 1 3 5 triazine and Benzilic Acid synthesis and characterization of a heptacoordinate feii nitrato complex
    European Journal of Inorganic Chemistry, 2008
    Co-Authors: Catherine P. Raptopoulou, Yiannis Sanakis, Athanassios K. Boudalis
    Abstract:

    The simultaneous presence of Benzilic Acid [Ph2C(OH)CO2H] and tptz [2,4,6-tri(2-pyridyl)-1,3,5-triazine] in FeIII-containing reaction mixtures leads to partial and/or quantitative metal reduction. In the presence of the oxidative NO3– ions in the reaction mixture, partial reduction of the metal leads to the isolation of a heptacoordinate FeII–nitrato complex, [FeII(tptz)(NO3)(MeOH)2](NO3) (1), along with a FeIII complex (2). In the presence of perchlorate ions in the reaction mixture, the quantitative reduction of FeIII leads to the isolation of a hexacoordinate FeII complex, [FeII(tptzH)2](ClO4)4 (3). Complexes 1 and 3 have been structurally characterized and possess a pentagonal-bipyramidal and a distorted octahedral coordination geometry, respectively. In both complexes, tptz behaves as a tridentate ligand, adopting the terpy-like coordination mode, and is coordinated through the triazine nitrogen atom and the two adjacent pyridine nitrogen atoms. One asymmetrically coordinated chelate, NO3–, and two MeOH molecules complete the pentagonal-bipyramidal geometry around FeII in 1. On the basis of analytical, spectroscopic (IR, Mossbauer) and magnetic susceptibility data from polycrystalline samples of 2, an oxido-bridged diferric structure is proposed [ΔEQ(78 K) = 1.79 mm s–1, JFe–Fe = –117 cm–1]. The Mossbauer spectra of the polycrystalline samples of 1 and 3 are consistent with high-spin and low-spin FeII, respectively, in anN/O coordination environment. Variable-temperature and variable-field magnetic measurements of 1 suggest significant zero-field splitting of the ferrous ions (D = 5.5 cm–1).(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)

  • Aerobic FeIII–FeII Reduction in the Presence of 2,4,6-Tri(2-pyridyl)-1,3,5-triazine and Benzilic Acid: Synthesis and Characterization of a Heptacoordinate FeII–Nitrato Complex
    European Journal of Inorganic Chemistry, 2008
    Co-Authors: Catherine P. Raptopoulou, Yiannis Sanakis, Athanassios K. Boudalis
    Abstract:

    The simultaneous presence of Benzilic Acid [Ph2C(OH)CO2H] and tptz [2,4,6-tri(2-pyridyl)-1,3,5-triazine] in FeIII-containing reaction mixtures leads to partial and/or quantitative metal reduction. In the presence of the oxidative NO3– ions in the reaction mixture, partial reduction of the metal leads to the isolation of a heptacoordinate FeII–nitrato complex, [FeII(tptz)(NO3)(MeOH)2](NO3) (1), along with a FeIII complex (2). In the presence of perchlorate ions in the reaction mixture, the quantitative reduction of FeIII leads to the isolation of a hexacoordinate FeII complex, [FeII(tptzH)2](ClO4)4 (3). Complexes 1 and 3 have been structurally characterized and possess a pentagonal-bipyramidal and a distorted octahedral coordination geometry, respectively. In both complexes, tptz behaves as a tridentate ligand, adopting the terpy-like coordination mode, and is coordinated through the triazine nitrogen atom and the two adjacent pyridine nitrogen atoms. One asymmetrically coordinated chelate, NO3–, and two MeOH molecules complete the pentagonal-bipyramidal geometry around FeII in 1. On the basis of analytical, spectroscopic (IR, Mossbauer) and magnetic susceptibility data from polycrystalline samples of 2, an oxido-bridged diferric structure is proposed [ΔEQ(78 K) = 1.79 mm s–1, JFe–Fe = –117 cm–1]. The Mossbauer spectra of the polycrystalline samples of 1 and 3 are consistent with high-spin and low-spin FeII, respectively, in anN/O coordination environment. Variable-temperature and variable-field magnetic measurements of 1 suggest significant zero-field splitting of the ferrous ions (D = 5.5 cm–1).(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)

Gayle K. Schulte - One of the best experts on this subject based on the ideXlab platform.

Hitoshi Takeshita - One of the best experts on this subject based on the ideXlab platform.

Kazuo Nagasawa - One of the best experts on this subject based on the ideXlab platform.

  • Enantioselective Total Synthesis of (+)-Stephadiamine through Bioinspired Aza-Benzilic Acid Type Rearrangement.
    Journal of the American Chemical Society, 2021
    Co-Authors: Minami Odagi, Taisei Matoba, Keisuke Hosoya, Kazuo Nagasawa
    Abstract:

    We report the first enantioselective total syntheses of the hasubanan alkaloid (-)-metaphanine and the norhasubanan alkaloid (+)-stephadiamine. Key features of these syntheses include diastereoselective oxidative phenolic coupling reaction and subsequent regioselective intramolecular aza-Michael reaction, which efficiently construct the hasubanan skeleton with the all-carbon quaternary stereogenic center at C13. Based on our hypothesis regarding the biosynthetic pathway of (+)-stephadiamine, we found that (-)-metaphanine is easily converted to (+)-stephadiamine via aza-Benzilic Acid type rearrangement reaction.

  • enantioselective total synthesis of stephadiamine through bioinspired aza Benzilic Acid type rearrangement
    Journal of the American Chemical Society, 2021
    Co-Authors: Minami Odagi, Taisei Matoba, Keisuke Hosoya, Kazuo Nagasawa
    Abstract:

    We report the first enantioselective total syntheses of the hasubanan alkaloid (-)-metaphanine and the norhasubanan alkaloid (+)-stephadiamine. Key features of these syntheses include diastereoselective oxidative phenolic coupling reaction and subsequent regioselective intramolecular aza-Michael reaction, which efficiently construct the hasubanan skeleton with the all-carbon quaternary stereogenic center at C13. Based on our hypothesis regarding the biosynthetic pathway of (+)-stephadiamine, we found that (-)-metaphanine is easily converted to (+)-stephadiamine via aza-Benzilic Acid type rearrangement reaction.

Catherine P. Raptopoulou - One of the best experts on this subject based on the ideXlab platform.

  • aerobic feiii feii reduction in the presence of 2 4 6 tri 2 pyridyl 1 3 5 triazine and Benzilic Acid synthesis and characterization of a heptacoordinate feii nitrato complex
    European Journal of Inorganic Chemistry, 2008
    Co-Authors: Catherine P. Raptopoulou, Yiannis Sanakis, Athanassios K. Boudalis
    Abstract:

    The simultaneous presence of Benzilic Acid [Ph2C(OH)CO2H] and tptz [2,4,6-tri(2-pyridyl)-1,3,5-triazine] in FeIII-containing reaction mixtures leads to partial and/or quantitative metal reduction. In the presence of the oxidative NO3– ions in the reaction mixture, partial reduction of the metal leads to the isolation of a heptacoordinate FeII–nitrato complex, [FeII(tptz)(NO3)(MeOH)2](NO3) (1), along with a FeIII complex (2). In the presence of perchlorate ions in the reaction mixture, the quantitative reduction of FeIII leads to the isolation of a hexacoordinate FeII complex, [FeII(tptzH)2](ClO4)4 (3). Complexes 1 and 3 have been structurally characterized and possess a pentagonal-bipyramidal and a distorted octahedral coordination geometry, respectively. In both complexes, tptz behaves as a tridentate ligand, adopting the terpy-like coordination mode, and is coordinated through the triazine nitrogen atom and the two adjacent pyridine nitrogen atoms. One asymmetrically coordinated chelate, NO3–, and two MeOH molecules complete the pentagonal-bipyramidal geometry around FeII in 1. On the basis of analytical, spectroscopic (IR, Mossbauer) and magnetic susceptibility data from polycrystalline samples of 2, an oxido-bridged diferric structure is proposed [ΔEQ(78 K) = 1.79 mm s–1, JFe–Fe = –117 cm–1]. The Mossbauer spectra of the polycrystalline samples of 1 and 3 are consistent with high-spin and low-spin FeII, respectively, in anN/O coordination environment. Variable-temperature and variable-field magnetic measurements of 1 suggest significant zero-field splitting of the ferrous ions (D = 5.5 cm–1).(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)

  • Aerobic FeIII–FeII Reduction in the Presence of 2,4,6-Tri(2-pyridyl)-1,3,5-triazine and Benzilic Acid: Synthesis and Characterization of a Heptacoordinate FeII–Nitrato Complex
    European Journal of Inorganic Chemistry, 2008
    Co-Authors: Catherine P. Raptopoulou, Yiannis Sanakis, Athanassios K. Boudalis
    Abstract:

    The simultaneous presence of Benzilic Acid [Ph2C(OH)CO2H] and tptz [2,4,6-tri(2-pyridyl)-1,3,5-triazine] in FeIII-containing reaction mixtures leads to partial and/or quantitative metal reduction. In the presence of the oxidative NO3– ions in the reaction mixture, partial reduction of the metal leads to the isolation of a heptacoordinate FeII–nitrato complex, [FeII(tptz)(NO3)(MeOH)2](NO3) (1), along with a FeIII complex (2). In the presence of perchlorate ions in the reaction mixture, the quantitative reduction of FeIII leads to the isolation of a hexacoordinate FeII complex, [FeII(tptzH)2](ClO4)4 (3). Complexes 1 and 3 have been structurally characterized and possess a pentagonal-bipyramidal and a distorted octahedral coordination geometry, respectively. In both complexes, tptz behaves as a tridentate ligand, adopting the terpy-like coordination mode, and is coordinated through the triazine nitrogen atom and the two adjacent pyridine nitrogen atoms. One asymmetrically coordinated chelate, NO3–, and two MeOH molecules complete the pentagonal-bipyramidal geometry around FeII in 1. On the basis of analytical, spectroscopic (IR, Mossbauer) and magnetic susceptibility data from polycrystalline samples of 2, an oxido-bridged diferric structure is proposed [ΔEQ(78 K) = 1.79 mm s–1, JFe–Fe = –117 cm–1]. The Mossbauer spectra of the polycrystalline samples of 1 and 3 are consistent with high-spin and low-spin FeII, respectively, in anN/O coordination environment. Variable-temperature and variable-field magnetic measurements of 1 suggest significant zero-field splitting of the ferrous ions (D = 5.5 cm–1).(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)