Synthesis and characterization of a three-dimensional open-framework lead(II) carboxyethylphosphonate, Pb3(O2CCH2CH2PO3)2

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S. Ayyappan, G. Diaz de Delgado, A. K. Cheetham, G. Férey and C. N. R. Rao


Abstract

The hydrothermal synthesis and single crystal XRD characterization of a three-dimensional open-framework lead(II) carboxyethylphosphonate, Pb3(O2CCH2CH2PO3)2, is described; the structure contains PbO3, PbO4 and PbO5 polyhedra, each with stereochemically active lone pairs of electrons, and exhibits several types of channels.


References

  1. C. T. Kresge, M. E. Leonowicz, W. J. Roth, J. C. Vartuli and J. S. Beck, Nature (London), 1992, 359, 710 CrossRef CAS.
  2. R. J. P. Corriu, D. Leclercq, P. H. Mutin, L. Sarlin and A. Vioux, J. Mater. Chem., 1998, 8, 1827 RSC.
  3. S. Drumel, P. Janvier, P. Barboux, M. Bujoli-Doeuff and B. Bujoli, Inorg. Chem., 1995, 34, 148 CrossRef CAS.
  4. A. Clearfield, Curr. Opin. Solid State Mater. Sci., 1996, 1, 266 CrossRef CAS.
  5. C. T. Seip, G. E. Granroth, M. W. Meisel and D. R. Talham, J. Am. Chem. Soc., 1997, 119, 7084 CrossRef CAS.
  6. P. Gendraud, L. Bigey, C. Gueho, M. E. de Roy and J. P. Besse, Chem. Mater., 1997, 9, 539 CrossRef CAS.
  7. P. J. Zapf, D. J. Rose, R. C. Haushalter and J. Zubieta, J. Solid State Chem., 1997, 132, 438 CrossRef CAS.
  8. B. Adair, S. Natarajan and A. K. Cheetham, J. Mater. Chem., 1998, 8, 1477 RSC.
  9. F. Serpaggi and G. Férey, Inorg. Chem., in the press Search PubMed.
  10. A. Distler and S. C. Sevov, Chem. Commun., 1998, 959 RSC.
  11. E. M. Sabbar, M. E. de Roy, A. Ennaqadi, C. Gueho and J. P. Besse, Chem. Mater., 1998, 10, 3856 CrossRef.
  12. G. B. Hix and K. D. M. Harris, J. Mater. Chem., 1998, 8, 579 RSC.
  13. F. Fredoueil, D. Massiot, D. M. Poojary, M. Bujoli-Doeuff, A. Cleareld and B. Bujoli, Chem. Commun., 1998, 175 RSC.
  14. D. A. Burwell and M. E. Thompson, Chem. Mater., 1991, 3, 14 CrossRef CAS.
  15. J.-P. Silvestre, N. El Messbahi, R. Rochdaoui, N. Q. Dao, M.-R. Lee and A. Neuman, Acta Crystallogr., Sect. C, 1990, 46, 986 CrossRef.
  16. D. M. Poojary, B. Zhang, A. Cabeza, M. A. G. Aranda, S. Bruque and A. Cleareld, J. Mater. Chem., 1996, 6, 639 RSC.
  17. In a typical experiment, 1.655 g of lead nitrate and 0.77 g of 2-carboxyethylphosphonic acid were mixed with water in the ratio 1:1:55. The pH of the above solution was raised to 6, using 10 N NaOH. The starting mixtures were stirred to attain homogeneity, transferred to a 23 ml (fill-factor = 40%) PTFE bottle, then sealed in a stainless steel autoclave (Parr, USA) and heated at 150 °C for 48 h under autogenous pressure. The resulting product, which mainly contained crystals, was filtered and washed thoroughly with deionized water. The powder X-ray diffraction (XRD) pattern of the powdered crystals indicated that the product was a new material. Thermogravimetric analysis (TGA) was carried out in static air in the range between 25 and 900 °C. The results indicate that a sharp weight loss of 9.5%(calc. 9.9%) at around 400 °C corresponds to the loss of carbon, hydrogen and some oxygen. The powder XRD of the decomposed product at 400 °C conrms the presence of α-Pb3(PO4)2(JCPDS: 25-1394).
  18. A suitable single crystal (0.01 × 0.2 × 0.1 mm) was carefully selected under a polarizing microscope. Single crystal structure determination by X-ray diffraction was performed on a Siemens Smart-CCD diffractometer equipped with a normal focus, 2.4 kW sealed tube X-ray source (Mo-Kα radiation, λ= 0.71073 Å) operating at 40 Kv and 40 mA. A hemisphere of intensity data was collected at room temperature in 1321 frames with ω scans (width of 0.30° and exposure time of 10 s per frame). The final unit cell constants were determined by a least squares fit of 1368 reections in the range 3° < 2θ < 46.5°. Crystal data for Pb3(O2CCH2CH2PO3)2: monoclinic, space group P21/c, a= 9.0559(10), b= 14.5584(17), c= 10.7154(12)Å, β= 111.19 (1)°, V= 1317.2(3)Å3, Z= 4, M= 923.63, µ= 38.5 mm–1. Total data 10042 reections; observed data 1368 relections; R(int)= 0.116. Final RF= 0.0446, wR2= 0.1046, S= 0.938, for 190 parameters. CCDC reference number 186/1569.
  19. G. M. Sheldrick, SHELXS-86, Program for Crystal Structure Determination, University of Göttingen, 1986; Acta Crystallogr., Sect. A, 1990, 35, 467 Search PubMed; G. M. Sheldrick, SADABS User Guide, University of Göttingen, 1995 Search PubMed; G. M. Sheldrick, SHELXL-93, A program for crystal structure determination, University of Göttingen, Germany, 1993.
  20. D. Massiot, S. Drumel, P. Janvier, M. Bujoli-Doeuff and B. Bujoli, Chem. Mater., 1997, 9, 6 CrossRef CAS.
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