Skip to main content Accessibility help
×
Home

The crystal structure of anthropogenic Pb2(OH)3(NO3), and a review of Pb-(O,OH) clusters and lead nitrates

  • U. Kolitsch (a1) and E. Tillmanns (a1)

Abstract

The previously unknown crystal structure of the basic lead nitrate Pb2(OH)3(NO3) has been determined using single-crystal X-ray diffraction data (Mo-Kα radiation, CCD area detector). The compound is orthorhombic, space group Immm, with a = 8.314(2), b = 8.545(2), c = 17.210(3) Å (R1 = 2.78% for 940 ‘observed’ reflections with Fo > 4σ(Fo)). The layered structure contains a previously unknown cuboid [Pb8(OH)12]4+ cluster and NO3 groups. The study used crystals formed by anthropogenic processes on a medieval mine dump, probably involving black gunpowder used in the blasting of ore. Pb2(OH)3(NO3) is associated with a second nitrate, Pb13O8(OH)6(NO3)4, which was previously designated as “Pb3O3(OH)4(NO3)2” or “Pb3(OH)5(NO3)”. It is rhombohedral, space group , with a = 10.263(1), c = 25.454(5) Å, and a structure solution is in complete agreement with an independent single-crystal study by Li et al. (2001). Probable hydrogen bonds in Pb2(OH)3(NO3) are indicated. Reported data on clusters and lead hydroxide and oxide nitrates are summarized and discussed critically. The probable conditions of formation of the studied samples are evaluated.

Copyright

Corresponding author

References

Hide All
Abakumov, A.M., Shpanchenko, R.V. and Antipov, E.V. (1998) Synthesis and structure of the double oxide Pb6Re6O19. Zeitschrift für Anorganische und Allgemeine Chemie, 624, 750—753
Arbatskii, A.P., Benson, V.V. and Bol’shakova, E.V. (1995) Compositions and solubility products of lead nitrate hydroxides and hydroxide. Russian Journal of Physical Chemistry, 69, 1730—1732
Baes, C.F., Jr. and Mesmer, R.E. (1976) The Hydrolysis of Cations. Wiley-Interscience, New York.
Behm, H. (1983) Hexalead chloride triorthoborate oxide, Pb4O[Pb2(BO3)3Cl]. Acta Crystallographica, C39, 1317—1319
Bengtsson, L. and Holmberg, B. (1990) Cationic lead(II) hydroxide complexes in molten alkali-metal nitrate. Journal of the Chemical Society, Faraday Transactions, 86, 351—359
Brese, N.E. and O’Keeffe, M. (1991) Bond-valence parameters for solids. Acta Crystallographica, B47, 192—197
Brooker, M.H., Sunder, S., Taylor, P. and Lopata, V.J. (1983) Infrared and Raman spectra and X-ray diffraction studies of solid lead(II) carbonates. Canadian Journal of Chemistry, 61, 494—502
Brusset, H., Martin, J.J.P. and Peltier, C. (1967) Lead oxide nitrate hydrates. Bulletin de la Societe Chimique de France, 1967, 1127—1133(in French).
Cooper, M.A., Hawthorne, F.C., Merlino, S., Pasero, M. and Perchiazzi, N. (1999) Stereoactive lone-pair behavior of Pb in the crystal structure of bideauxite: Pb2+ 2Ag+Cl3F(OH). The Canadian Mineralogist, 37, 915—921
Cram, A.G. and Davies, M.B. (1976) A Raman and IR spectrophotometric study of some basic lead nitrate compounds and their thermal decomposition products. Journal of Inorganic and Nuclear Chemistry, 38, 1111—1117
Cruywagen, J.J. and van de Water, R.F. (1993) The hydrolysis of lead(II). A potentiometric and en-thalpimetric study. Talanta, 40, 1091—1095
Donaldson, J.D., Grimes, S.M., Johnston, S.R. and Abrahams, I. (1995) Characterisation of the tin(II) hydroxide cation [Sn3(OH)4]2+, and the crystal structure of tritin(II) tetrahydroxide dinitrate. Journal of the Chemical Society, Dalton Transactions, 1995, 2273—2276
Eiden-Assmann, S., Schneider, A.M., Behrens, P., Wiebcke, M., Engelhardt, G. and Felsche, J. (2000) Lead hydro sodalite [Pb2(OH)(H2O)3]2[Al3Si3O12]2: synthesis and structure determination by combining X-ray Rietveld refinement, 1H MAS NMR FTIR and XANES spectroscopy. Chemistry - A European Journal , 6, 292—297
Frostemark, F., Bengtsson, L.A. and Holmberg, B. (1994) Formation and structure of mono- and di-lead hydroxide and fluoride complexes in molten NH4NO3-1.5H2O at 50°C. Journal of the Chemical Society, Faraday Transactions, 90, 2531—2539
Garcia-Clavel, M.E., Martinez-Lope, M.J., Casais-Alvarez, M.T. and Kilany, A. (1985) Thermoanalytical and structural study of lead trioxynitrates. Pp. 547-551 in: Thermal Analysis, Proceedings ICTA, 8th, Vol. 1 (Blazek, A., editor).
Garcia-Clavel, M.E., Martinez-Lope, M.J., Casais-Alvarez, M.T. and Kilany, A. (1986a) Obtention, thermal behavior and structural study of the dioxynitrates of lead. Thermochimica Acta , 105, 111—116
Garcia-Clavel, M.E., Martinez-Lope, M.J., Casais-Alvarez, M.T. and Kilany, A. (1986b) Study of the degradation in open atmosphere of the hydrated dioxynitrate of lead. Thermochimica Acta , 108, 29—32
Garcia-Clavel, M.E., Martinez-Lope, M.J., Casais-Alvarez, M.T. and Kilany, A. (1986c) Thermoanalytical study of lead monohydroxynitrate. Thermochimica Acta, 98, 205—212
Graf, H.-W. (1991) Die Grube “Neue Hoffnung” zu Bleialf/Eifel. Lapis, 16 (2), 1318 (in German).
Grimes, S.M., Johnston, S.R. and Abrahams, I. (1995) Characterisation of the predominant low-pH lead(II)- hydroxo cation, [Pb4(OH)4]4+; crystal structure of [Pb4(OH)4][NO3]4 and the implications of basic salt formation on the transport of lead in the aqueous environment. Journal of the Chemical Society, Dalton Transactions , 1995, 2081—2086
Gyunner, E.A., Tsareva, A.I., Bakina, N.B. and Vel’mozhnyi, I.S. (1978) Reaction of lead nitrate with some bases in aqueous solutions. Ukrainskii Khimicheskii Zhurnal (Russian edition), 44, 348—352(in Russian).
Haag-Bruhl, C., Fuess, H., Lightfoot, P. and Cheetham, A.K. (1988) Preparation and structure of lead oxide hydroxide perrhenate hydrate (Pb6O(OH)6 (ReO4)4H2O). Acta Crystallographica, C44, 8—11
Hill, R.J. (1985) Structure of Pb3O2(OH)2 by Rietveld analysis of neutron powder diffraction data. Acta Crystallographica , C41, 998—1003
Hong, S.-H. and Olin, A. (1973) Crystal structure of [Pb4(OH)4]3(CO3)(ClO4)106H2O. Acta Chemica Scandinavica, 27, 2309—2320
Hong, S.-H. and Olin, A. (1974) Crystal structure of [Pb4(OH)4](ClO4)4(H2O)2. Acta Chemica Scandinavica, A28, 233—238
Hyde, B.G. and Andersson, S. (1989) Inorganic Crystal Structures . Wiley Interscience, New York, 302 pp.
Johansson, G. and Olin, A. (1968) Structures of the dominating hydrolysis products of lead(II) in solution. Acta Chemica Scandinavica , 22, 3197—3201
Keller, H.L. (1982) Darstellung und Kristallstruktur von TlPb8O4Br9. Zeitschrift für Anorganische und Allgemeine Chemie, 491, 191—198(in German).
Keller, H.L. (1983) Eine neuartige Blei-Sauerstoff- Baugruppe: (Pb8O4)8+. Angewandte Chemie, 95, 318—319(in German).
Kolitsch, U. (1997) Neufunde von Mineralien aus einigen Vorkommen der Vogesen, Frankreich: Triembach, Bluttenberg und Val d’Ajol. Aufschluss, 48, 65—91(in German).
Kolitsch, U. (2000) Eine durch Betoneinwirkung entstandene Paragenese von Blei-Verbindungen aus der Grube Clara im mittleren Schwarzwald. Erzgraber, 14, 48—53(in German).
Kolitsch, U. and Giester, G. (2000) Elyite, Pb4Cu(SO4)O2(OH)4H2O: crystal structure and new data. American Mineralogist, 85, 1816—1821
Krivovichev, S.V. and Brown, I.D. (2001) Are the compressive effects of encapsulation an artifact of the bond valence parameters? Zeitschrift für Kristallographie, 216, 245—247
Krivovichev, S.V. and Bums, P.C. (2000a) Crystal chemistry of basic lead carbonates. I. Crystal structure of synthetic shannonite, Pb2O(CO3). Mineralogical Magazine, 64, 1063 — 1068.
Krivovichev, S.V. and Burns, P.C. (2000b) Crystal chemistry of basic lead carbonates. II. Crystal structure of synthetic “plumbonacrite”. Mineralogical Magazine, 64, 1069—1075
Krivovichev, S.V. and Burns, P.C. (2000c) Crystal chemistry of basic lead carbonates. III. Crystal structures of Pb3O2(CO3) and NaPb2(OH)(CO3)2 . Mineralogical Magazine, 64, 1077—1088
Krivovichev, S.V. and Filatov, S.K. (1999a) Metal arrays in structural units based on anion-centered metal tetrahedra. Acta Crystallographica, B55, 664—676
Krivovichev, S.V. and Filatov, S.K. (1999b) Structural principles for minerals and inorganic compounds containing anion-centered tetrahedra. American Mineralogist, 84, 1099—1106
Krivovichev, S.V., Filatov, S.K. and Semenova, T.F. (1998) Types of cationic complexes based on oxocentred tetrahedra [OM4] in the crystal structures of inorganic compounds. Russian Chemical Reviews, 67, 137—155
Krivovichev, S.V., Li, Y. and Burns, P.C. (2001) Crystal chemistry of lead oxide hydroxide nitrates. III. The crystal structure of Pb3O2(OH)(NO3). Journal of Solid State Chemistry, 158, 78—81
Kwestroo, W., Langereis, C. and van Hal, H.A.M. (1967) Basic lead nitrates. Journal of Inorganic and Nuclear Chemistry, 29, 33—38
Li, Y., Krivovichev, S.V. and Burns, P.C. (2000) Crystal chemistry of lead oxide hydroxide nitrates. I. The crystal structure of [Pb6O4](OH)(NO3)(CO3). Journal of Solid State Chemistry, 153, 365—370
Li, Y., Krivovichev, S.V. and Burns, P.C. (2001) Crystal chemistry of lead oxide hydroxide nitrates. II. The crystal structure of Pb13O8(OH)6(NO3)4. Journal of Solid State Chemistry, 158, 74—77.
Lundgren, G., Wernfors, G. and Yamaguchi, T. (1982) The structure of ditin(II) oxide sulfate. Acta Crystallographica, B38, 2357—2361
Lutz, H.D. and Jung, C. (1997) Lattice vibration spectra. Part XCII. High-pressure Raman spectroscopic studies on laurionite-type Pb(OD)Cl, Pb(OD)Br, Pb(OD)I, and Sr(OD)I, pressure dependence of the directionality of lone pairs. European Journal of Solid State and Inorganic Chemistry , 34, 1179—1185
Lutz, H.D., Beckenkamp, K. and Peter, S. (1995) Laurionite-type M(OH)X (M = Ba, Pb; X = Cl, Br, I) and Sr(OH)I. An IR and Raman spectroscopic study. Spectrochimica Acta, 51A, 755—767.
Lutz, H.D., Beckenkamp, K., Kellersohn, T., Moeller, H. and Peter, S. (1996) Neutron and X-ray structure determination of laurionite-type Pb{O(H,D)}X, with X = Cl, Br, and I, hydrogen bonds to lead(II) ions as a hydrogen-bond acceptor. Journal of Solid State Chemistry , 124, 155—161
Martin, J.J.P., Martin-Lefevre, C., Repelin, Y. and Husson, E. (1972a) Lead oxynitrates. Thermal analysis of hydrated lead heptoxytrinitrate. Bulletin de la Societe Chimique de France , 1972, 3341—3342 (in French).
Martin, J.J.P., Martin-Lefevre, C. and Despagne, B. (1972b) Lead oxynitrates. Thermal analysis of hydrated lead pentoxynitrate. Bulletin de la Societe Chimique de France, 1972, 2573—2574(in French).
Michell, E.W.J. (1974) Basic lead nitrates. I. Compounds formed by reaction of orthorhombic lead monoxide with cold aqueous lead nitrate. Journal of Applied Chemical Biotechnology , 24, 571—581
Moore, E.P., Chen, H.Y., Brixner, L.H. and Foris, C.M. (1982) The crystal structure of Pb8Bi2(PO4)6O2 . Materials Research Bulletin , 17, 653—660
Nardin, G., Randaccio, L. and Zangrando, E. (1995) Lead clustering in a zeolite X. Zeolites, 15, 684—688
Narita, E., Okayasu, H. and Naito, H. (1984) The formation and solubility of various lead(II) compounds prepared by the hydrolysis of lead(II) nitrate. Bulletin of the Chemical Society of Japan , 57, 309—310
Newkirk, A.E. and Hughes, V.B. (1970) Identification of the “lead(II) hydroxide” of Robin and Theolier. Inorganic Chemistry, 9, 401—404
O’Keeffe, M. and Hyde, B.G. (1985) An alternative approach to non-molecular crystal structures with emphasis on the arrangements of cations. Structure and Bonding, 61, 77—144
Olin, A. and Soderquist, R. (1972) Crystal structure of β-lead hydroxide oxide perchlorate hydrate (β-[Pb6O(OH)6](CIO4)4-H2O). Acta Chemica Scandinavica , 26, 3505—3514
Otwinowski, Z. and Minor, W. (1997) Processing of X-ray diffraction data collected in oscillation mode. Methods in Enzymology, 276, 307—326
Pauley, J.L. and Testerman, M.K. (1954) Basic salts of lead nitrate formed in aqueous media. Journal of the American Chemical Society , 76, 4220—4222
Pyykko, P. (1997) Strong closed-shell interactions in inorganic chemistry. Chemical Reviews , 97, 597—636
Ronay, C. and Seff, K. (1993) Lead oxide hydroxide clusters in lead hydroxide oxide (Pb9O(OH)4)-A, zeolite A exchanged with Pb2+ at pH 6.0. Zeolites, 13, 97—101
Rouse, R.C. and Peacor, D.R. (1994) Maricopaite, an unusual lead calcium zeolite with an interrupted mordenite-like framework and intrachannel Pb4 tetrahedral clusters. American Mineralogist, 79, 175—184
Schlomann, C. and Steen, H. (1990) Neue Mineralfunde aus dem Bergbaugebiet von Badenweiler im SUdschwarzwald. Lapis, 15(12), 1320; 50 (in German).
Shape Software (1999) ATOMS for Windows and Macintosh V5.0.4. Kingsport, TN 37663, USA.
Sheldrick, G.M. (1997a) SHELXS-97, a program for the solution of crystal structures. University of Gottingen, Germany.
Sheldrick, G.M. (1997b) SHELXL-97, a program for crystal structure refinement. University of Gottingen, Germany.
Spek, A.L. (2001) PLATON, a multipurpose crystallographic tool . Utrecht University, Utrecht, The Netherlands.
Spiro, T.G., Templeton, D.H. and Zalkin, A. (1969) Crystal structure of a hexanuclear basic lead(II) perchlorate hydrate: Pb6O(OH)6(CIO4)4'H2O. Inorganic Chemistry, 8, 856—861
Sterns, M., Parise, J.B. and Howard, C.J. (1986) Refinement of the structure of trilead(II) uranate(VI) from neutron powder diffraction data. Acta Crystallographica, C42, 1275—1277
Stieglitz, H. and Metz, W. (1989) Die Mineralien der Grube Churfiirst Ernst in Bönkhausen. Lapis, 14(2), 2227, 33, 42 (in German).
Sugiyama, S., Nakanishi, T., Ishimura, T., Moriga, T., Hayashi, H., Shigemoto, N. and Moffat, J.B. (1999) Preparation, characterization, and thermal stability of lead hydroxyapatite. Journal of Solid State Chemistry, 143, 296—302
Tsai, P. and Cooney, R.P. (1976) Raman spectra of polynuclearhydroxo-compounds oflead(II) chloride. Journal of the Chemical Society, Dalton Transactions, 1976, 1631—1634
Uchida, M., Minakata, N. and Okuwaki, A. (1997) Recovery of ammonia and nitrate ion from ammonium nitrate in wastewater by steam distillation adding lead(II) oxide. Hydrometallurgy , 45, 239—247
Walenta, K. (1998) Neue Mineralfunde aus dem Schwarzwald. 7. Folge, 2. Teil. Lapis, 23(12), 43-48 (in German).
Werner, J.P. and Müller-Buschbaum, H. (1997) Elektroneutrale Pb4O4-Heterokubaneinheiten in den Aluminatsodalithen Ln4[Al12O24](Pb4O4)2 (Ln = Nd, Sm). Zeitschrift für Naturforschung, B52, 449—452(in German).
Wittern, A. (1994) Sekundärmineralien durch Feuersetzen in Oberschulenberg, Bönkhausen, Bleialf und Badenweiler. Aufschluss, 45, 36—42(in German).
Yeom, Y.H., Kim, Y. and Seff, K. (1997) Crystal structure of zeolite X exchanged with Pb(II) at pH 6.0 and dehydrated: (Pb4+)14(Pb2+)18(Pb4O4)8 Si100Al92O384. Journal of Physical Chemistry, B101, 5314—5318
Yeom, Y.H., Kim, Y. and Seff, K. (1999) Crystal structure of Pb2+ 44Pb4+ 5Tl+ 18O 2- 17-Si100Al92O384, zeolite X exchanged with Pb2+ and Tl+ and dehydrated, containing Pb4〇4(Pb2+,Pb4+mixed)4 clusters. Microporous and Mesoporous Materials, 28, 103—112

Keywords

Type Description Title
UNKNOWN
Supplementary materials

Kolitsch and Tillmanns supplementary material
Table 5

 Unknown (160 KB)
160 KB

The crystal structure of anthropogenic Pb2(OH)3(NO3), and a review of Pb-(O,OH) clusters and lead nitrates

  • U. Kolitsch (a1) and E. Tillmanns (a1)

Metrics

Full text views

Total number of HTML views: 0
Total number of PDF views: 0 *
Loading metrics...

Abstract views

Total abstract views: 0 *
Loading metrics...

* Views captured on Cambridge Core between <date>. This data will be updated every 24 hours.

Usage data cannot currently be displayed