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Oxonitridosilicate chlorides-synthesis, single-crystal X-ray and neutron powder diffraction, chemical analysis and properties of Ln(4) Si4O3+N-x(7-x) Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2

Oxonitridosilicate chlorides-synthesis, single-crystal X-ray and neutron powder diffraction, chemical analysis and properties of Ln(4) Si4O3+N-x(7-x) Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2
Oxonitridosilicate chlorides-synthesis, single-crystal X-ray and neutron powder diffraction, chemical analysis and properties of Ln(4) Si4O3+N-x(7-x) Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2
The isotypic oxonitridosilicate chlorides Ln(4)[Si4O3+xN7-x]Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2 were obtained by the reaction of the respective rare-earth metals, their oxides and chlorides with "Si(NH)(2)" in a radiofrequency furnace at temperatures around 1800 degrees C, using CsCl as a flux. The crystal structures were determined by single-crystal X-ray diffraction (P2(1)3, no. 198, Z = 4, Cc: a = 10.4461(12)pm, R1 = 0.0524; Pr: a = 10.3720(12)pm, R1 = 0.0415; Nd: a = 10.3618(12) pm, R1 = 0.0257) and found to be isotypic with Ce-4[Si4O4N6]O. In order to characterize the incorporation of chlorine into the structure, the crystallographic site occupation factors of O, N and Cl were determined by neutron powder diffraction. Furthermore, these results were substantiated by the chemical analyses for Pr-4[Si4O3+xN7-x]Cl1-xOx and electron microprobe analyses for all of the synthesized oxonitridosilicate chlorides. Temperature-dependent magnetic Susceptibility measurements of the cerium and the praseodymium compound indicate Curie-Weiss behavior with experimentally determined magnetic moments of 2.15(5) mu(B)/Ce and 3.50(5) mu(B)/Pr, respectively. No magnetic ordering could be detected down to 2 K. The 4f(I) of cerium has been confirmed by XAS measurements.
cerium, praseodymium, neodymium, chloride, oxonitridosilicate, crystal structure, neutron diffraction, magnetism, x-ray spectroscopy, lightelement electron probe microanalyseselectron-microprobe analysis, magnetic-properties, nitridosilicates, silicates, oxygen
0022-4596
976-988
Lieb, Alexandra
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Weller, Mark T.
5be42713-fd58-4dc6-bc7a-86a801e201bc
Henry, Paul F.
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Niewa, Rainer
56701609-6da1-4226-8bd0-5450ae128c5d
Pöttgen, Rainer
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Hoffmann, Rolf-Dieter
b152a640-e0ff-4f0d-af75-4131df3f33e3
Höfer, Heidi E.
755d4661-fdc0-42e7-8b51-cddb1e2a9437
Schnick, Wolfgang
a2c9466f-33fc-4736-bcac-8950f8f2dbda
Lieb, Alexandra
bf550f75-1843-4433-8efa-5de8ef0a8888
Weller, Mark T.
5be42713-fd58-4dc6-bc7a-86a801e201bc
Henry, Paul F.
6ab0d6ca-bb2c-4286-9fad-1a5894dd8b75
Niewa, Rainer
56701609-6da1-4226-8bd0-5450ae128c5d
Pöttgen, Rainer
2ef0dba9-eecb-460c-a5c7-6a69f1020b44
Hoffmann, Rolf-Dieter
b152a640-e0ff-4f0d-af75-4131df3f33e3
Höfer, Heidi E.
755d4661-fdc0-42e7-8b51-cddb1e2a9437
Schnick, Wolfgang
a2c9466f-33fc-4736-bcac-8950f8f2dbda

Lieb, Alexandra, Weller, Mark T., Henry, Paul F., Niewa, Rainer, Pöttgen, Rainer, Hoffmann, Rolf-Dieter, Höfer, Heidi E. and Schnick, Wolfgang (2005) Oxonitridosilicate chlorides-synthesis, single-crystal X-ray and neutron powder diffraction, chemical analysis and properties of Ln(4) Si4O3+N-x(7-x) Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2. Journal of Solid State Chemistry, 178 (4), 976-988. (doi:10.1016/j.jssc.2004.10.022).

Record type: Article

Abstract

The isotypic oxonitridosilicate chlorides Ln(4)[Si4O3+xN7-x]Cl1-xOx with Ln = Ce, Pr, Nd and x approximate to 0.2 were obtained by the reaction of the respective rare-earth metals, their oxides and chlorides with "Si(NH)(2)" in a radiofrequency furnace at temperatures around 1800 degrees C, using CsCl as a flux. The crystal structures were determined by single-crystal X-ray diffraction (P2(1)3, no. 198, Z = 4, Cc: a = 10.4461(12)pm, R1 = 0.0524; Pr: a = 10.3720(12)pm, R1 = 0.0415; Nd: a = 10.3618(12) pm, R1 = 0.0257) and found to be isotypic with Ce-4[Si4O4N6]O. In order to characterize the incorporation of chlorine into the structure, the crystallographic site occupation factors of O, N and Cl were determined by neutron powder diffraction. Furthermore, these results were substantiated by the chemical analyses for Pr-4[Si4O3+xN7-x]Cl1-xOx and electron microprobe analyses for all of the synthesized oxonitridosilicate chlorides. Temperature-dependent magnetic Susceptibility measurements of the cerium and the praseodymium compound indicate Curie-Weiss behavior with experimentally determined magnetic moments of 2.15(5) mu(B)/Ce and 3.50(5) mu(B)/Pr, respectively. No magnetic ordering could be detected down to 2 K. The 4f(I) of cerium has been confirmed by XAS measurements.

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Published date: 1 April 2005
Keywords: cerium, praseodymium, neodymium, chloride, oxonitridosilicate, crystal structure, neutron diffraction, magnetism, x-ray spectroscopy, lightelement electron probe microanalyseselectron-microprobe analysis, magnetic-properties, nitridosilicates, silicates, oxygen

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Local EPrints ID: 20850
URI: http://eprints.soton.ac.uk/id/eprint/20850
ISSN: 0022-4596
PURE UUID: 17684055-fb60-4c79-be7c-fbc4b1d4a83d

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Date deposited: 03 Mar 2006
Last modified: 15 Jul 2019 19:25

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Contributors

Author: Alexandra Lieb
Author: Mark T. Weller
Author: Paul F. Henry
Author: Rainer Niewa
Author: Rainer Pöttgen
Author: Rolf-Dieter Hoffmann
Author: Heidi E. Höfer
Author: Wolfgang Schnick

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