메뉴 건너뛰기
European Journal of Inorganic Chemistry
Volumn , Issue 22, 2008, Pages 3423-3427
Self-assembled two-dimensional water-soluble dipicolinate Cu/Na coordination polymer: Structural features and catalytic activity for the mild peroxidative oxidation of cycloalkanes in acid-free medium
Author keywords

C H activation; Homogeneous catalysis; N,O ligands; Self assembly; Supramolecular chemistry
Indexed keywords

ACTIVATION ANALYSIS; CATALYSIS; CATALYST ACTIVITY; CATALYTIC OXIDATION; CHEMICAL ACTIVATION; COPPER COMPOUNDS; CRYSTAL STRUCTURE; HYDROGEN BONDS; KETONES; MOLECULES; ORGANOMETALLICS; SINGLE CRYSTALS; SODIUM HYDROXIDE; SUPRAMOLECULAR CHEMISTRY; X RAY DIFFRACTION ANALYSIS;
EID: 53249145452     PISSN: 14341948     EISSN: 10990682     Source Type: Journal    
DOI: 10.1002/ejic.200800355     Document Type: Article
Times cited : (97)
References (46)
  • 2
    • 85153318976 scopus 로고    scopus 로고
    • See the Cambridge Structural Database (CSD, version 5.28, Jan. 2008): F. H. Allen, Acta Crystallogr., Sect. B 2002, 58, 380.
    • See the Cambridge Structural Database (CSD, version 5.28, Jan. 2008): F. H. Allen, Acta Crystallogr., Sect. B 2002, 58, 380.
  • 28
    • 85153173921 scopus 로고    scopus 로고
    • Synthesis of [Cu(μ-dipic)2{Na2(μ-H 2O)4}]n·2nH2O (1, To an aqueous solution (10.0 mL) containing Cu(NO3) 2·2.5H2O (1.00 mmol, 233 mg) and HNO3 (1.00 mmol, the acid was added to avoid spontaneous hydrolysis of the metal salt] were added dropwise triethanolamine (1.00 mmol, 130 μL) and an aqueous solution (4.0 mL) of NaOH (160 mg, 4.00 mmol, and solid H2dipic 84 mg, 0.50 mmol, in this order and with continuous stirring in air at ambient temperature. The resulting clear blue solution was stirred overnight, then passed through a filter, concentrated under reduced pressure to one half of its and kept in a beaker in air at ambient temperature. Light blue X-ray quality crystals were formed in 2-3 weeks from a deep blue oily solution, then collected, gently wiped with a filter paper and dried in air to furnish compound
    • [9]
  • 30
    • 85153211207 scopus 로고    scopus 로고
    • X-ray crystal structure determination: X-ray data were collected with an Enraf-Nonius CAD4 diffractometer equipped with graphite monochromator and by using Mo-Kα radiation (λ, 0.71073 Å, The structure was solved by direct methods with the SHELXS-97 program.[11] A semiempirical absorption correction was applied.[12] The structure was refined with the SHELXL-97 program.[11] All hydrogen atoms were located. Crystal data for 1: C14H18CuN 2Na2O14, M, 547.82, monoclinic, space group P2/c, a, 9.7626(12) Å, b, 7.9756(10) Å, c, 12.9066(13) Å, V, 1004.9(2) Å3, Z, 2, Dc, 1.811 gcm-3, F000, 558, μ, 1.210 mm-1, T, 293 K, 2026 reflections collected, 1624 reflections with I > 2σI, Rint, 0.0217
    • 2 = 0.0736. CCDC-683529 contains the supplementary crystallographic data for 1. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif.
  • 34
    • 85153272608 scopus 로고    scopus 로고
    • 2O)] fragments.
    • 2O)] fragments.
  • 40
    • 85153176817 scopus 로고    scopus 로고
    • Peroxidative oxidation of cyclohexane and cyclopentane: The catalyst precursor 1 (5.0 mg, 9.2 μmol, used as a solid, was mixed with the cycloalkane (1.25 mmol, CH3NO2 (internal standard for GC analysis, 0.50 mL of its 1.4 M solution in MeCN, acetonitrile (4.20 mL) and H2O2 (2.50 mmol, 50% in H2O, 0.17 mL, in this order. The resulting reaction mixtures were vigorously stirred in thermostatted (50°C) Pyrex cylindrical vessels for 5 h at atmospheric air pressure. The product analysis was performed as follows: a sample was taken from the reaction mixture, treated with an excess of solid PPh3 (for prior reduction[17] of cycloalkyl hydroperoxides that are the main primary products) and then analyzed by GC by using a Fisons Instruments GC 8000 series gas chromatograph with a DB-624 (J&W) capillary column and the Jasco-Borwin v.1.50 software, revealing the formation of the following mixt
    • 2NH (2.50 mmol of each in a separate batch), displaying an almost complete suppression of catalytic activity of 1 (only traces of products, below 0.3% were observed).
  • 41
    • 0037120663 scopus 로고    scopus 로고
    • and references cited therein
    • G. B. Shul'pin, J. Mol. Catal. A 2002, 189, 39, and references cited therein.
    • (2002) J. Mol. Catal. A , vol.189 , pp. 39
    • Shul'pin, G.B.1
  • 42
    • 85153259086 scopus 로고    scopus 로고
    • This activity has been achieved by using slightly different (relative to those described[16, reaction parameters, i.e, catalyst precursor 1 (3.0 mg, 5.5 μmol, cyclohexane (10.0 mmol, acetonitrile (3.80 mL) and H2O2 10.0 mmol, 50% in H2O, 0.68 mL
    • 2O, 0.68 mL).
  • 43
    • 85153212689 scopus 로고    scopus 로고
    • II (I = 3/2) with g = 2.22 and A = 130 G (with poorly resolved hyperfine coupling) were observed for both solid (298 K) and solution (100 K) samples of 1. A broad signal (g = 2.16) without hyperfine coupling was obtained for a solid sample at 100 K.
    • II (I = 3/2) with g = 2.22 and A = 130 G (with poorly resolved hyperfine coupling) were observed for both solid (298 K) and solution (100 K) samples of 1. A broad signal (g = 2.16) without hyperfine coupling was obtained for a solid sample at 100 K.
  • 46
    • 85153296004 scopus 로고    scopus 로고
    • 3, reveal no activity in the oxidation of cyclohexane (i.e. only traces of products, below 0.2% of the total yield, have been detected). Moreover, the activity of 1 is not promoted to any extent by the addition of potassium or sodium carbonate.
    • 3, reveal no activity in the oxidation of cyclohexane (i.e. only traces of products, below 0.2% of the total yield, have been detected). Moreover, the activity of 1 is not promoted to any extent by the addition of potassium or sodium carbonate.

* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.