Thermally stable manganese(III) peroxido complexes with hindered N3 tripodal ligands: Structures and their physicochemical properties

被引:5
作者
Fujisawa, Kiyoshi [1 ]
Sakuma, Syuhei [1 ]
Ikarugi, Riko [1 ]
Jose, Anex [2 ]
Solomon, Edward I. [2 ,3 ]
机构
[1] Ibaraki Univ, Dept Chem, Mito, Ibaraki 3108512, Japan
[2] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
[3] Stanford Univ, SLAC, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA
关键词
Mononuclear manganese(II) complexes; Manganese(III) complexes; Peroxido complexes; X-ray crystallography; Infrared spectroscopy; DFT calculations; I RIBONUCLEOTIDE REDUCTASES; SUPEROXIDE DISMUTASES; ELECTRONIC-STRUCTURE; METAL-COMPLEXES; BOND OXIDATION; WATER; IRON; REACTIVITY; CRYSTAL; BEARING;
D O I
10.1016/j.jinorgbio.2021.111597
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
Mononuclear manganese(III) peroxido complexes are candidates for the reaction intermediates in manganese containing proteins, such as manganese superoxide dismutase (Mn-SOD) etc. In this study, manganese(III) peroxido complexes [Mn(O-2)(L3)] and [Mn(O-2)(L10)] ligated by anionic N3 type ligands with sterically hindered substituents, hydrotris(3-tertiary butyl-5-isopropyl-1-pyrazolyl)borate (L3(-)) and hydrotris(3-adamantyl-5-isopropyl-1-pyrazolyl)borate (L10(-)), respectively, were structurally characterized. These complexes are the first examples of structurally characterized five-coordinate manganese(III) peroxido complexes. Their characteristic nu(O-O) and nu(Mn-O) stretchings were determined by using (H2O2)-O-18 for the first time. Theoretical calculations were performed to obtain further insight into their structural parameters. The decomposed products were obtained as [{Mn-III(mu-O)(L3)}(2)Mn-IV] and [Mn-III(OH){L10(O)}] from [Mn(O-2)(L3)] and [Mn(O-2)(L10)], respectively.
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页数:9
相关论文
共 68 条
[21]   A MONOMERIC SIDE-ON SUPEROXOCOPPER(II) COMPLEX - CU(O-2)(HB(3-TBU-5-IPRPZ)(3)) [J].
FUJISAWA, K ;
TANAKA, M ;
MOROOKA, Y ;
KITAJIMA, N .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (26) :12079-12080
[22]   The most hindered hydrotris(pyrazolyl)borate ligand, X-ray structure of chlorocopper(II) complex:: [Cu(Cl){HB(3-Ad-5-Pripz)3}] as compared with [Cu(Cl){HB(3-But-5-Pripz)3}] [J].
Fujisawa, K ;
Tada, N ;
Ishikawa, Y ;
Higashimura, H ;
Miyashita, Y ;
Okamoto, KI .
INORGANIC CHEMISTRY COMMUNICATIONS, 2004, 7 (02) :209-212
[23]   Mononuclear copper(II) hydroxo complex: Structural effect of a 3-position of tris(pyrazolyl)borates [J].
Fujisawa, K ;
Kobayashi, T ;
Fujita, K ;
Kitajima, N ;
Moro-oka, Y ;
Miyashita, Y ;
Yamada, Y ;
Okamoto, K .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 2000, 73 (08) :1797-1804
[24]   SECOND-SPHERE TUNING OF THE METAL ION REDUCTION POTENTIALS IN IRON AND MANGANESE SUPEROXIDE DISMUTASES [J].
Grove, Laurie E. ;
Brunold, Thomas C. .
COMMENTS ON INORGANIC CHEMISTRY, 2008, 29 (5-6) :134-168
[25]   Electron Paramagnetic Resonance Detection of Intermediates in the Enzymatic Cycle of an Extradiol Dioxygenase [J].
Gunderson, William A. ;
Zatsman, Anna I. ;
Emerson, Joseph P. ;
Farquhar, Erik R. ;
Que, Lawrence, Jr. ;
Lipscomb, John D. ;
Hendrich, Michael P. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (44) :14465-+
[26]  
Herschbach D.R., 1961, 9694 UCRL
[27]   Synthesis and characterization of the benzoylformato ferrous complexes with the hindered tris(pyrazolyl)borate ligand as a structural model for mononuclear non-heme iron enzymes [J].
Hikichi, S ;
Ogihara, T ;
Fujisawa, K ;
Kitajima, N ;
Akita, M ;
Morooka, Y .
INORGANIC CHEMISTRY, 1997, 36 (20) :4539-4547
[28]   Metal use in ribonucleotide reductase R2, di-iron, di-manganese and heterodinuclear-an intricate bioinorganic workaround to use different metals for the same reaction [J].
Hogbom, Martin .
METALLOMICS, 2011, 3 (02) :110-120
[29]   63Cu NMR study of copper(I) carbonyl complexes with various hydrotris(pyrazolyl)borates:: Correlation between 63Cu chemical shifts and CO stretching vibrations [J].
Imai, S ;
Fujisawa, K ;
Kobayashi, T ;
Shirasawa, N ;
Fujii, H ;
Yoshimura, T ;
Kitajima, N ;
Moro-oka, Y .
INORGANIC CHEMISTRY, 1998, 37 (12) :3066-3070
[30]   Probing the geometric and electronic structures of the low-temperature azide adduct and the product-inhibited form of oxidized manganese superoxide dismutase [J].
Jackson, TA ;
Karapetian, A ;
Miller, AF ;
Brunold, TC .
BIOCHEMISTRY, 2005, 44 (05) :1504-1520