- Email: [email protected]
Unprecedented 5,5-connected (47 · 63) (48 · 62) structural topology: A lead biphosphonate with double layered structure
Available online at www.sciencedirect.com
Inorganic Chemistry Communications 11 (2008) 604–607 www.elsevier.com/locate/inoche
Unprecedented 5,5-connected (47 63) (48 62) structural topology: A lead biphosphonate with double layered structure Shu-Fang Zhang a,c,*, Zhi Liu b, Xiao-Gang Yang a,c, Qing Yu a,c, Bao-Rong Hou a,* b
a Institute of Oceanology, Chinese Academy of Sciences, Nanhai Road, Qingdao 266071, China College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China c Graduate School of the Chinese Academy of Sciences, Beijing 100039, China
Received 16 January 2008; accepted 14 February 2008 Available online 21 February 2008
Abstract A new lead(II) phosphonate, Pb[(PO3)2C(OH)CH3] H2O (1) was hydrothermally synthesized and characterized by IR, elemental analysis, UV, TGA, SEM, and single crystal X-ray diffraction analysis. X-ray crystallographic study showed that complex 1 has a two-dimensional double layered hybrid structure containing interconnected 4- and 12-membered rings and shows an unusual (5,5)-connected (47 63) (48 62) topology. Ó 2008 Elsevier B.V. All rights reserved. Keywords: Lead phosphonate; Crystal structure; Layered structure; Topology
The search for novel microporous materials is very intense in materials chemistry recently [1–4]. This is mainly due to their extensive applications in the area of catalysis, separations, ion exchange as well as their potential applications in electro-optical and sensing applications [5,6]. Following the discovery of Flanigen’s first microporous aluminophosphates in 1982 [7], a great deal of attention has been paid to the synthesis of open-framework phosphate-based materials [8]. The metal phosphonates family of solids has proved a particularly rich source of new compounds [9]. Research on metal phosphonates has shown that most of the compounds have microporous or open-framework structures in which the metal centers are bridged by the phosphonate tetrahedra. Metal phosphonates with neutral layers are of great interest respect to intercalation reaction. Studies showed that the structure of a layer affects the ability to intercalate *
Corresponding authors. Address: Institute of Oceanology, Chinese Academy of Sciences, Nanhai Road, Qingdao 266071, China. Tel.: +86 532 82898742; fax: +86 532 82880498 (S.-F. Zhang). E-mail addresses: [email protected] (S.-F. Zhang), [email protected] (B.-R. Hou). 1387-7003/$ - see front matter Ó 2008 Elsevier B.V. All rights reserved. doi:10.1016/j.inoche.2008.02.020
guest molecules greatly. To build neutral layers with interesting structures, a variety of phosphonates of bifunctional or multifunctional units including other functional groups such as crown ether, amine and carboxylate groups have been employed [10–12]. To promote specific chemical reactions or to enhance particular physical properties, new types of layered materials are often desired. As far as the metal ions were concerned, although a lot of examples of transitional or rare earth metal phosphonates have been reported, reports on main group metal phosphonates are relatively rare [13]. Several lead phosphonates isolated by using a second ligand were reported by Clearfield group [2], Cheetham group [3], and Mao group [14]. Studies have shown that the presence of the lone pair electrons of Pb(II) affects the structures of the phosphonates formed greatly [15]. To synthesize metal phosphonates with diversified layered structures and unexpected functional properties different from those of the transitional metals, we have employed diphosphonate Hedp (Hedp = l-hydroxyethylidenediphosphonate) and lead(II) acetate as initial materials. In this work, we successfully obtained a new Pb(II) phosphonate Pb[(PO3)2C(OH)CH3] H2O (1). It is strikingly the rare example of
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607
metal phosphonates with two-dimensional double layered hybrid structure with interconnected 4-and 12-membered rings and showing an unusual (5,5)-connected (47 63) (48 62) topology. Herein, we report its synthesis, crystal structure, and characterization. The novel lead phosphonate Pb[(PO3)2C(OH)CH3] H2O 1, was prepared by employing mild hydrothermal method with Pb(CH3COO)2 and l-hydroxyethylidenediphosphonate, [CH3C(OH)(PO3H2)2] (L) heated at 170 °C for 5 days [16]. The formulation is supported by IR, elemental analysis and thermogravimetric analysis (TGA) results. The scanning electron microscopy (SEM) image in Fig. S1 shows the morphology of the block single crystals in compound 1. Single-crystal X-ray crystallography for 1 [17] reveals that the complex features a two-dimensional (2D) double layer. Fig. 1 shows the environment about Pb atom. Compared with common five or six-coordination in other lead phosphonates reported by the literature [18,19], Pb(1) atom adopts a relatively rare coordination model, which is four-coordinated by phosphonate oxygen atoms from three ligands. The coordination geometry around Pb(1) can be described as a tetrahedron. The Pb– O distances (Table S1) are in the range of 2.352(6)– ˚ , these distances are comparable to those 2.529(7) A reported in other lead(II) phosphonates [20–23]. The diphosphonate anion is tetradentate with four phosphonate oxygen atoms (O(1), O(3), O(4),O(6)) bridging with three Pb(1) atoms, and the other two phosphonate oxygen atoms (O(2), O(5)) are non-coordinated. Scheme 1 shows the formula of the Hedp and its coordination model in compound 1. The cross-linkage of Pb(II) ions by diphosphonate ligands leads to a two-dimensional (2D) hybrid double layer along bc-plane (Fig. 2). One interesting aspect of this lead phosphonate is that it contains 12- and 4-membered rings in the layer. The 12-membered ring was formed by
Fig. 1. Thermal ellipsoid plot (50% probability) and atom labeling scheme for asymmetric unit of compound 1. Atom labels with ‘‘i” refer to symmetry generated atoms.
605
Scheme 1. The molecular formula of the Hedp and its coordination model in compound 1.
Fig. 2. View of the 2D layer with 4- and 12-membered rings propagate along bc-plane: Pb (black), O (white), C (light-grey) and PO4 (light-grey).
six diphosphonate ligands connecting six lead atoms alternately. Similar to that in the 12-membered ring, two diphosphonate ligands connect two lead atoms to form the 4-membered ring. Each 12-membered ring is surrounded by six other 12-membered rings and two 4-membered rings, while each 4-membered ring is surrounded by four 12-membered rings. This structural feature is quite different from other lead phosphonates observed previously, most of which contain no ring or small rings. In the view of topology, the 2D architecture can be best rationalized to the (5,5)-connected (47 63) (48 62) network if we simplified the diphosphonate Hedp and Pb(II) ions as 5-connected nodes (Fig. 3). The unprecedented topological net with 5,5-connected node is rarely observed in coordination polymers up to now. To the best of our knowledge, this framework has never been described so far in the chemistry of phosphate-based materials. The adjacent layers are stacked in an AAAA sequence along the a-axis, as shown in Fig. 4. The lattice water molecule O(1W) is located above the plane of the 12-MR. There are only inter-molecular H-bonds with O. . .O ˚ (Table S2) and no H(O4. . .O7) at a distance of 2.701 A bonds between adjacent layers. In the IR spectrum of compound 1 (Fig. S2), the broadband at 3378 and 3164 cm 1 can be assigned to the O–H
606
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607
Fig. 5. Absorption spectra of C(OH)CH3] H2O (solid line). Fig. 3. Schematic representation of the 5, 5-connected (47 63) (48 62) topology in 1.
L
(dotted
line)
and Pb[(PO3)2-
In summary, by hydrothermal reactions of lead(II) acetate with diphosphonate Hedp, a new two-dimensional lead phosphonate hybrid was obtained. The diphosphonate Hedp ligand in compound 1 acts as a multidentate metal linker, which connects Pb atoms to form a double layered structure with 4- and 12-membered rings. It is noteworthy that compound with neutral layers characterized by weak interlayer interactions may accommodate large guest molecules by free adjustment of interlayer separation. It is believed that the successful synthesis of this compound provides the possibility for preparing other new types of microporous materials that may find widespread application in intercalation reactions. Acknowledgement
Fig. 4. View of the packing of the layers along the [001] direction: Pb (black), O (white), C (light-grey) and PO4 (light-grey).
stretching vibrations. The strong band at 1637 cm 1 is characteristic band to the d(H–OH). The bands from 900 to 1200 cm 1 are due to the stretching vibrations of the tetrahedral CPO3 group [24,25]. Absorption spectra of [CH3C(OH)(PO3H2)2] (L) and Pb[(PO3)2C(OH)CH3] H2O are presented in Fig. 5. The UV spectrum of the free ligand L displays one strong absorption band at 206 nm. Upon combination with lead ion, the band centered at 206 nm Einstein shifts to 219 nm, which may be attributable to conformational changes of the ligand induced by the metal. The TGA curve (Fig. S3) shows 1 is thermally stable up to 150 °C. Subsequently, decomposition occurs in two steps with a total weight loss of 17.55% until 700 °C. The initial weight loss of 4.12% between 160 °C and 240 °C can be assigned to the release of the lattice water molecules (calcd 4.19%). The second step with a sharp weight loss of 13.43% between 400 °C and 700 °C can be assigned to the combustion of phosphonate ligands.
This work was financially supported by the Knowledge Innovation Program of the Chinese Academy of Sciences (KZCX2-YW-210). Appendix A. Supplementary material CCDC 655907 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif. Supplementary data associated with this article can be found, in the online version, at doi:10.1016/j.inoche.2008.02.020. References [1] C.V. Krishnamohan Sharma, A. Clearfield, J. Am. Chem. Soc. 122 (2000) 4394. [2] S. Konar, N. Bhuvanesh, A. Clearfield, J. Am. Chem. Soc. 128 (2006) 9604. [3] A.K. Cheetham, G. Ferey, T. Loiseau, Angew. Chem. Int. Ed. 38 (1999) 3268. [4] R. Murugavel, M.P. Singh, Inorg. Chem. 45 (2006) 9154. [5] S.D. Alexandratos, X.P. Zhu, Inorg. Chem. 46 (2007) 2139.
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607 [6] J. Zhu, X. Bu, P. Feng, G.D. Stucky, J. Am. Chem. Soc. 122 (2000) 11563. [7] S.T. Wilson, B.M. Lok, C.A. Messina, T.R. Cannan, E.M. Flanigen, J. Am. Chem. Soc. 4 (1982) 1146. [8] A.K. Cheetham, G. Fe´rey, T. Loiseau, Angew. Chem. Int. Ed. 38 (1999) 3268. [9] (a) V. Soghomonian, Q. Chen, R.C. Haushalter, J. Zubieta, Angew. Chem. Int. Ed. 34 (1995) 223; (b) U. Costantino, M. Nocchetti, R. Vivani, J. Am. Chem. Soc. 124 (2002) 8428; (c) S.O.H. Gutschke, D.J. Price, A.K. Powell, P.T. Wood, Angew. Chem. Int. Ed. 38 (1999) 1088. [10] S. Ayyappan, G.D. Delgado, A.K. Cheetham, G. Fe´rey, C.N.R. Rao, J. Chem. Soc. Dalton Trans. 17 (1999) 2905. [11] A. Distler, S.C. Sevov, Chem. Commun. 9 (1998) 959. [12] S.J. Hartman, E. Todorov, C. Cruz, S.C. Sevov, Chem. Commun. 13 (2000) 1213. [13] A. Subbiah, D. Pyle, A. Rowland, J. Huang, R.A. Narayanan, P. Thiyagarajan, J. Zon´, A. Clearfield, J. Am. Chem. Soc. 127 (2005) 10826. [14] J.-L. Song, J.-G. Mao, Y.-Q. Sun, H.-Y. Zeng, R.K. Kremer, A. Clearfield, J. Solid State Chem. 177 (2004) 633. [15] A. Cabeza, M.A.G. Aranda, M. Martinez-Lara, S. Bruque, J. Sanz, Acta Crystallogr. B52 (1996) 982. [16] All chemicals used during the course of this work were of reagent grade and used without further purification. Preparation of 1: typically, 0.20 g of Pb(CH3COO)2 was dissolved in 10 mL H2O. To this solution, 0.2 mL l-hydroxyethylidenediphosphonate, [CH3C(OH)(PO3H2)2] was added dropwise under constant stirring. The resulting mixture, with pH value of about 2, was sealed in a Teflon-lined steel autoclave and heated at 170 °C for 5 days. After cooling to room temperature, colorless block crystals were obtained by filtration, washed with distilled water and dried in air (52% yield based on Pb). Elemental analysis for complex 1, C2H6O8P2Pb, Found: C, 5.60; H,
[17]
[18] [19]
[20] [21] [22] [23] [24] [25]
607
1.46; P, 14.62%. Anal. Calc.: C, 5.62; H, 1.41; P, 14.50%. IR (KBr, cm 1): 3378(s) and 3164(s) for m(O–H), 1637(s) for d(H–OH), 900– 1200(vs) for m(C–PO3). Crystal structure determination by X-ray diffraction was performed on a Siemens SMART CCD diffractometer with graphite-monochro˚ ) radiation at room temperature. An mated Mo Ka (k = 0.71073 A empirical absorption correction was applied using the SADABS program [18]. The structure was solved by direct methods using SHELXS-97 [19]. The lead and phosphorus atoms were first located, and the oxygen and carbon atoms were found in the successive difference Fourier maps. The hydrogen atoms attached to the water molecules were not located. The refinements were performed against all full matrix least-squares analysis with anisotropic thermal parameters for all non-hydrogen atoms. Crystal data for 1: Monoclinic, ˚ , b = 8.280(2) A ˚ , c = 10.285(2) A ˚, b= P2(1)/c, a = 10.850(2) A ˚ 3, Z = 4. Dc = 3.240 g/cm3, l = 19.781 109.75(3)°, V = 869.6(3) A mm 1, F(0 0 0) = 764, GooF = 1.035, R1 = 0.0473, wR2 = 0.0483 for 1531 unique reflections and 114 parameters. G.M. Sheldrick, A Program for the Siemens Area Detector Absorption Correction, University of Go¨ttingen, 1997. G.M. Sheldrick, SHELXS97 Program for Solution of Crystal Structures, University of Go¨ttingen, Go¨ttingen, Germany, 1997; G.M. Sheldrick, SHELXL97 Program for Solution of Crystal Structures, University of Go¨ttingen, Germany, 1997. L. Lin, T.-J. Zhang, Y.-T. Fan, D.-G. Ding, H.-W. Hou, J. Mol. Struct. 837 (2007) 107. A. Cabeza, M.A.G. Aranda, S. Bruque, J. Mater. Chem. 9 (1999) 571. N. Stock, G.D. Stucky, A.K. Cheetham, Chem. Commun. (2000) 2277. J.-G. Mao, Z. Wang, A. Clearfield, Inorg. Chem. 41 (2002) 6106. J.-G. Mao, Z. Wang, A. Clearfield, J. Chem. Soc. Dalton Trans. (2002) 4541. Z.-Y. Du, S.-M. Ying, J.-G. Mao, J. Mol. Struct. 788 (2006) 218.
Inorganic Chemistry Communications 11 (2008) 604–607 www.elsevier.com/locate/inoche
Unprecedented 5,5-connected (47 63) (48 62) structural topology: A lead biphosphonate with double layered structure Shu-Fang Zhang a,c,*, Zhi Liu b, Xiao-Gang Yang a,c, Qing Yu a,c, Bao-Rong Hou a,* b
a Institute of Oceanology, Chinese Academy of Sciences, Nanhai Road, Qingdao 266071, China College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China c Graduate School of the Chinese Academy of Sciences, Beijing 100039, China
Received 16 January 2008; accepted 14 February 2008 Available online 21 February 2008
Abstract A new lead(II) phosphonate, Pb[(PO3)2C(OH)CH3] H2O (1) was hydrothermally synthesized and characterized by IR, elemental analysis, UV, TGA, SEM, and single crystal X-ray diffraction analysis. X-ray crystallographic study showed that complex 1 has a two-dimensional double layered hybrid structure containing interconnected 4- and 12-membered rings and shows an unusual (5,5)-connected (47 63) (48 62) topology. Ó 2008 Elsevier B.V. All rights reserved. Keywords: Lead phosphonate; Crystal structure; Layered structure; Topology
The search for novel microporous materials is very intense in materials chemistry recently [1–4]. This is mainly due to their extensive applications in the area of catalysis, separations, ion exchange as well as their potential applications in electro-optical and sensing applications [5,6]. Following the discovery of Flanigen’s first microporous aluminophosphates in 1982 [7], a great deal of attention has been paid to the synthesis of open-framework phosphate-based materials [8]. The metal phosphonates family of solids has proved a particularly rich source of new compounds [9]. Research on metal phosphonates has shown that most of the compounds have microporous or open-framework structures in which the metal centers are bridged by the phosphonate tetrahedra. Metal phosphonates with neutral layers are of great interest respect to intercalation reaction. Studies showed that the structure of a layer affects the ability to intercalate *
Corresponding authors. Address: Institute of Oceanology, Chinese Academy of Sciences, Nanhai Road, Qingdao 266071, China. Tel.: +86 532 82898742; fax: +86 532 82880498 (S.-F. Zhang). E-mail addresses: [email protected] (S.-F. Zhang), [email protected] (B.-R. Hou). 1387-7003/$ - see front matter Ó 2008 Elsevier B.V. All rights reserved. doi:10.1016/j.inoche.2008.02.020
guest molecules greatly. To build neutral layers with interesting structures, a variety of phosphonates of bifunctional or multifunctional units including other functional groups such as crown ether, amine and carboxylate groups have been employed [10–12]. To promote specific chemical reactions or to enhance particular physical properties, new types of layered materials are often desired. As far as the metal ions were concerned, although a lot of examples of transitional or rare earth metal phosphonates have been reported, reports on main group metal phosphonates are relatively rare [13]. Several lead phosphonates isolated by using a second ligand were reported by Clearfield group [2], Cheetham group [3], and Mao group [14]. Studies have shown that the presence of the lone pair electrons of Pb(II) affects the structures of the phosphonates formed greatly [15]. To synthesize metal phosphonates with diversified layered structures and unexpected functional properties different from those of the transitional metals, we have employed diphosphonate Hedp (Hedp = l-hydroxyethylidenediphosphonate) and lead(II) acetate as initial materials. In this work, we successfully obtained a new Pb(II) phosphonate Pb[(PO3)2C(OH)CH3] H2O (1). It is strikingly the rare example of
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607
metal phosphonates with two-dimensional double layered hybrid structure with interconnected 4-and 12-membered rings and showing an unusual (5,5)-connected (47 63) (48 62) topology. Herein, we report its synthesis, crystal structure, and characterization. The novel lead phosphonate Pb[(PO3)2C(OH)CH3] H2O 1, was prepared by employing mild hydrothermal method with Pb(CH3COO)2 and l-hydroxyethylidenediphosphonate, [CH3C(OH)(PO3H2)2] (L) heated at 170 °C for 5 days [16]. The formulation is supported by IR, elemental analysis and thermogravimetric analysis (TGA) results. The scanning electron microscopy (SEM) image in Fig. S1 shows the morphology of the block single crystals in compound 1. Single-crystal X-ray crystallography for 1 [17] reveals that the complex features a two-dimensional (2D) double layer. Fig. 1 shows the environment about Pb atom. Compared with common five or six-coordination in other lead phosphonates reported by the literature [18,19], Pb(1) atom adopts a relatively rare coordination model, which is four-coordinated by phosphonate oxygen atoms from three ligands. The coordination geometry around Pb(1) can be described as a tetrahedron. The Pb– O distances (Table S1) are in the range of 2.352(6)– ˚ , these distances are comparable to those 2.529(7) A reported in other lead(II) phosphonates [20–23]. The diphosphonate anion is tetradentate with four phosphonate oxygen atoms (O(1), O(3), O(4),O(6)) bridging with three Pb(1) atoms, and the other two phosphonate oxygen atoms (O(2), O(5)) are non-coordinated. Scheme 1 shows the formula of the Hedp and its coordination model in compound 1. The cross-linkage of Pb(II) ions by diphosphonate ligands leads to a two-dimensional (2D) hybrid double layer along bc-plane (Fig. 2). One interesting aspect of this lead phosphonate is that it contains 12- and 4-membered rings in the layer. The 12-membered ring was formed by
Fig. 1. Thermal ellipsoid plot (50% probability) and atom labeling scheme for asymmetric unit of compound 1. Atom labels with ‘‘i” refer to symmetry generated atoms.
605
Scheme 1. The molecular formula of the Hedp and its coordination model in compound 1.
Fig. 2. View of the 2D layer with 4- and 12-membered rings propagate along bc-plane: Pb (black), O (white), C (light-grey) and PO4 (light-grey).
six diphosphonate ligands connecting six lead atoms alternately. Similar to that in the 12-membered ring, two diphosphonate ligands connect two lead atoms to form the 4-membered ring. Each 12-membered ring is surrounded by six other 12-membered rings and two 4-membered rings, while each 4-membered ring is surrounded by four 12-membered rings. This structural feature is quite different from other lead phosphonates observed previously, most of which contain no ring or small rings. In the view of topology, the 2D architecture can be best rationalized to the (5,5)-connected (47 63) (48 62) network if we simplified the diphosphonate Hedp and Pb(II) ions as 5-connected nodes (Fig. 3). The unprecedented topological net with 5,5-connected node is rarely observed in coordination polymers up to now. To the best of our knowledge, this framework has never been described so far in the chemistry of phosphate-based materials. The adjacent layers are stacked in an AAAA sequence along the a-axis, as shown in Fig. 4. The lattice water molecule O(1W) is located above the plane of the 12-MR. There are only inter-molecular H-bonds with O. . .O ˚ (Table S2) and no H(O4. . .O7) at a distance of 2.701 A bonds between adjacent layers. In the IR spectrum of compound 1 (Fig. S2), the broadband at 3378 and 3164 cm 1 can be assigned to the O–H
606
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607
Fig. 5. Absorption spectra of C(OH)CH3] H2O (solid line). Fig. 3. Schematic representation of the 5, 5-connected (47 63) (48 62) topology in 1.
L
(dotted
line)
and Pb[(PO3)2-
In summary, by hydrothermal reactions of lead(II) acetate with diphosphonate Hedp, a new two-dimensional lead phosphonate hybrid was obtained. The diphosphonate Hedp ligand in compound 1 acts as a multidentate metal linker, which connects Pb atoms to form a double layered structure with 4- and 12-membered rings. It is noteworthy that compound with neutral layers characterized by weak interlayer interactions may accommodate large guest molecules by free adjustment of interlayer separation. It is believed that the successful synthesis of this compound provides the possibility for preparing other new types of microporous materials that may find widespread application in intercalation reactions. Acknowledgement
Fig. 4. View of the packing of the layers along the [001] direction: Pb (black), O (white), C (light-grey) and PO4 (light-grey).
stretching vibrations. The strong band at 1637 cm 1 is characteristic band to the d(H–OH). The bands from 900 to 1200 cm 1 are due to the stretching vibrations of the tetrahedral CPO3 group [24,25]. Absorption spectra of [CH3C(OH)(PO3H2)2] (L) and Pb[(PO3)2C(OH)CH3] H2O are presented in Fig. 5. The UV spectrum of the free ligand L displays one strong absorption band at 206 nm. Upon combination with lead ion, the band centered at 206 nm Einstein shifts to 219 nm, which may be attributable to conformational changes of the ligand induced by the metal. The TGA curve (Fig. S3) shows 1 is thermally stable up to 150 °C. Subsequently, decomposition occurs in two steps with a total weight loss of 17.55% until 700 °C. The initial weight loss of 4.12% between 160 °C and 240 °C can be assigned to the release of the lattice water molecules (calcd 4.19%). The second step with a sharp weight loss of 13.43% between 400 °C and 700 °C can be assigned to the combustion of phosphonate ligands.
This work was financially supported by the Knowledge Innovation Program of the Chinese Academy of Sciences (KZCX2-YW-210). Appendix A. Supplementary material CCDC 655907 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif. Supplementary data associated with this article can be found, in the online version, at doi:10.1016/j.inoche.2008.02.020. References [1] C.V. Krishnamohan Sharma, A. Clearfield, J. Am. Chem. Soc. 122 (2000) 4394. [2] S. Konar, N. Bhuvanesh, A. Clearfield, J. Am. Chem. Soc. 128 (2006) 9604. [3] A.K. Cheetham, G. Ferey, T. Loiseau, Angew. Chem. Int. Ed. 38 (1999) 3268. [4] R. Murugavel, M.P. Singh, Inorg. Chem. 45 (2006) 9154. [5] S.D. Alexandratos, X.P. Zhu, Inorg. Chem. 46 (2007) 2139.
S.-F. Zhang et al. / Inorganic Chemistry Communications 11 (2008) 604–607 [6] J. Zhu, X. Bu, P. Feng, G.D. Stucky, J. Am. Chem. Soc. 122 (2000) 11563. [7] S.T. Wilson, B.M. Lok, C.A. Messina, T.R. Cannan, E.M. Flanigen, J. Am. Chem. Soc. 4 (1982) 1146. [8] A.K. Cheetham, G. Fe´rey, T. Loiseau, Angew. Chem. Int. Ed. 38 (1999) 3268. [9] (a) V. Soghomonian, Q. Chen, R.C. Haushalter, J. Zubieta, Angew. Chem. Int. Ed. 34 (1995) 223; (b) U. Costantino, M. Nocchetti, R. Vivani, J. Am. Chem. Soc. 124 (2002) 8428; (c) S.O.H. Gutschke, D.J. Price, A.K. Powell, P.T. Wood, Angew. Chem. Int. Ed. 38 (1999) 1088. [10] S. Ayyappan, G.D. Delgado, A.K. Cheetham, G. Fe´rey, C.N.R. Rao, J. Chem. Soc. Dalton Trans. 17 (1999) 2905. [11] A. Distler, S.C. Sevov, Chem. Commun. 9 (1998) 959. [12] S.J. Hartman, E. Todorov, C. Cruz, S.C. Sevov, Chem. Commun. 13 (2000) 1213. [13] A. Subbiah, D. Pyle, A. Rowland, J. Huang, R.A. Narayanan, P. Thiyagarajan, J. Zon´, A. Clearfield, J. Am. Chem. Soc. 127 (2005) 10826. [14] J.-L. Song, J.-G. Mao, Y.-Q. Sun, H.-Y. Zeng, R.K. Kremer, A. Clearfield, J. Solid State Chem. 177 (2004) 633. [15] A. Cabeza, M.A.G. Aranda, M. Martinez-Lara, S. Bruque, J. Sanz, Acta Crystallogr. B52 (1996) 982. [16] All chemicals used during the course of this work were of reagent grade and used without further purification. Preparation of 1: typically, 0.20 g of Pb(CH3COO)2 was dissolved in 10 mL H2O. To this solution, 0.2 mL l-hydroxyethylidenediphosphonate, [CH3C(OH)(PO3H2)2] was added dropwise under constant stirring. The resulting mixture, with pH value of about 2, was sealed in a Teflon-lined steel autoclave and heated at 170 °C for 5 days. After cooling to room temperature, colorless block crystals were obtained by filtration, washed with distilled water and dried in air (52% yield based on Pb). Elemental analysis for complex 1, C2H6O8P2Pb, Found: C, 5.60; H,
[17]
[18] [19]
[20] [21] [22] [23] [24] [25]
607
1.46; P, 14.62%. Anal. Calc.: C, 5.62; H, 1.41; P, 14.50%. IR (KBr, cm 1): 3378(s) and 3164(s) for m(O–H), 1637(s) for d(H–OH), 900– 1200(vs) for m(C–PO3). Crystal structure determination by X-ray diffraction was performed on a Siemens SMART CCD diffractometer with graphite-monochro˚ ) radiation at room temperature. An mated Mo Ka (k = 0.71073 A empirical absorption correction was applied using the SADABS program [18]. The structure was solved by direct methods using SHELXS-97 [19]. The lead and phosphorus atoms were first located, and the oxygen and carbon atoms were found in the successive difference Fourier maps. The hydrogen atoms attached to the water molecules were not located. The refinements were performed against all full matrix least-squares analysis with anisotropic thermal parameters for all non-hydrogen atoms. Crystal data for 1: Monoclinic, ˚ , b = 8.280(2) A ˚ , c = 10.285(2) A ˚, b= P2(1)/c, a = 10.850(2) A ˚ 3, Z = 4. Dc = 3.240 g/cm3, l = 19.781 109.75(3)°, V = 869.6(3) A mm 1, F(0 0 0) = 764, GooF = 1.035, R1 = 0.0473, wR2 = 0.0483 for 1531 unique reflections and 114 parameters. G.M. Sheldrick, A Program for the Siemens Area Detector Absorption Correction, University of Go¨ttingen, 1997. G.M. Sheldrick, SHELXS97 Program for Solution of Crystal Structures, University of Go¨ttingen, Go¨ttingen, Germany, 1997; G.M. Sheldrick, SHELXL97 Program for Solution of Crystal Structures, University of Go¨ttingen, Germany, 1997. L. Lin, T.-J. Zhang, Y.-T. Fan, D.-G. Ding, H.-W. Hou, J. Mol. Struct. 837 (2007) 107. A. Cabeza, M.A.G. Aranda, S. Bruque, J. Mater. Chem. 9 (1999) 571. N. Stock, G.D. Stucky, A.K. Cheetham, Chem. Commun. (2000) 2277. J.-G. Mao, Z. Wang, A. Clearfield, Inorg. Chem. 41 (2002) 6106. J.-G. Mao, Z. Wang, A. Clearfield, J. Chem. Soc. Dalton Trans. (2002) 4541. Z.-Y. Du, S.-M. Ying, J.-G. Mao, J. Mol. Struct. 788 (2006) 218.