Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Autoren

  • Jan M. Welch
  • Danny Müller
  • Christian Knoll
  • Martin Wilkovitsch
  • Gerald Giester
  • Johannes Ofner
  • Bernhard Lendl
  • Peter Weinberger
  • Georg Steinhauser

Organisationseinheiten

Externe Organisationen

  • Technische Universität Wien (TUW)
  • Universität Wien
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Details

Titel in ÜbersetzungPikomolare Spuren von AmIII verursachen drastische Unterschiede in der Koordinationschemie von TbIII: ein Sprung über die “Gadoliniumecke”
OriginalspracheEnglisch
Seiten (von - bis)13264-13269
Seitenumfang6
FachzeitschriftAngewandte Chemie
Jahrgang56
Ausgabenummer43
Frühes Online-Datum26 Juli 2017
PublikationsstatusVeröffentlicht - 16 Okt. 2017

Abstract

The crystallization of terbium 5,5′-azobis[1H-tetrazol-1-ide] (ZT) in the presence of trace amounts (ca. 50 Bq, ca. 1.6 pmol) of americium results in 1) the accumulation of the americium tracer in the crystalline solid and 2) a material that adopts a different crystal structure to that formed in the absence of americium. Americium-doped [Tb(Am)(H2O)7ZT]2 ZT⋅10 H2O is isostructural to light lanthanide (Ce–Gd) 5,5′-azobis[1H-tetrazol-1-ide] compounds, rather than to the heavy lanthanide (Tb–Lu) 5,5′-azobis[1H-tetrazol-1-ide] (e.g., [Tb(H2O)8]2ZT3⋅6 H2O) derivatives. Traces of Am seem to force the Tb compound into a structure normally preferred by the lighter lanthanides, despite a 108-fold Tb excess. The americium-doped material was studied by single-crystal X-ray diffraction, vibrational spectroscopy, radiochemical neutron activation analysis, and scanning electron microcopy. In addition, the inclusion properties of terbium 5,5′-azobis[1H-tetrazol-1-ide] towards americium were quantified, and a model for the crystallization process is proposed.

ASJC Scopus Sachgebiete

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Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”. / Welch, Jan M.; Müller, Danny; Knoll, Christian et al.
in: Angewandte Chemie , Jahrgang 56, Nr. 43, 16.10.2017, S. 13264-13269.

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Welch, JM, Müller, D, Knoll, C, Wilkovitsch, M, Giester, G, Ofner, J, Lendl, B, Weinberger, P & Steinhauser, G 2017, 'Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”', Angewandte Chemie , Jg. 56, Nr. 43, S. 13264-13269. https://doi.org/10.1002/anie.201703971, https://doi.org/10.1002/ange.201703971
Welch, J. M., Müller, D., Knoll, C., Wilkovitsch, M., Giester, G., Ofner, J., Lendl, B., Weinberger, P., & Steinhauser, G. (2017). Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”. Angewandte Chemie , 56(43), 13264-13269. https://doi.org/10.1002/anie.201703971, https://doi.org/10.1002/ange.201703971
Welch JM, Müller D, Knoll C, Wilkovitsch M, Giester G, Ofner J et al. Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”. Angewandte Chemie . 2017 Okt 16;56(43):13264-13269. Epub 2017 Jul 26. doi: 10.1002/anie.201703971, 10.1002/ange.201703971
Welch, Jan M. ; Müller, Danny ; Knoll, Christian et al. / Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III) : A Break in the “Gadolinium Break”. in: Angewandte Chemie . 2017 ; Jahrgang 56, Nr. 43. S. 13264-13269.
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title = "Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III): A Break in the “Gadolinium Break”",
abstract = "The crystallization of terbium 5,5′-azobis[1H-tetrazol-1-ide] (ZT) in the presence of trace amounts (ca. 50 Bq, ca. 1.6 pmol) of americium results in 1) the accumulation of the americium tracer in the crystalline solid and 2) a material that adopts a different crystal structure to that formed in the absence of americium. Americium-doped [Tb(Am)(H2O)7ZT]2 ZT⋅10 H2O is isostructural to light lanthanide (Ce–Gd) 5,5′-azobis[1H-tetrazol-1-ide] compounds, rather than to the heavy lanthanide (Tb–Lu) 5,5′-azobis[1H-tetrazol-1-ide] (e.g., [Tb(H2O)8]2ZT3⋅6 H2O) derivatives. Traces of Am seem to force the Tb compound into a structure normally preferred by the lighter lanthanides, despite a 108-fold Tb excess. The americium-doped material was studied by single-crystal X-ray diffraction, vibrational spectroscopy, radiochemical neutron activation analysis, and scanning electron microcopy. In addition, the inclusion properties of terbium 5,5′-azobis[1H-tetrazol-1-ide] towards americium were quantified, and a model for the crystallization process is proposed.",
keywords = "actinides, energetic anions/ligands, gadolinium break, lanthanides, structural influence",
author = "Welch, {Jan M.} and Danny M{\"u}ller and Christian Knoll and Martin Wilkovitsch and Gerald Giester and Johannes Ofner and Bernhard Lendl and Peter Weinberger and Georg Steinhauser",
note = "Publisher Copyright: {\textcopyright} 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Copyright: Copyright 2017 Elsevier B.V., All rights reserved.",
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TY - JOUR

T1 - Picomolar Traces of Americium(III) Introduce Drastic Changes in the Structural Chemistry of Terbium(III)

T2 - A Break in the “Gadolinium Break”

AU - Welch, Jan M.

AU - Müller, Danny

AU - Knoll, Christian

AU - Wilkovitsch, Martin

AU - Giester, Gerald

AU - Ofner, Johannes

AU - Lendl, Bernhard

AU - Weinberger, Peter

AU - Steinhauser, Georg

N1 - Publisher Copyright: © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Copyright: Copyright 2017 Elsevier B.V., All rights reserved.

PY - 2017/10/16

Y1 - 2017/10/16

N2 - The crystallization of terbium 5,5′-azobis[1H-tetrazol-1-ide] (ZT) in the presence of trace amounts (ca. 50 Bq, ca. 1.6 pmol) of americium results in 1) the accumulation of the americium tracer in the crystalline solid and 2) a material that adopts a different crystal structure to that formed in the absence of americium. Americium-doped [Tb(Am)(H2O)7ZT]2 ZT⋅10 H2O is isostructural to light lanthanide (Ce–Gd) 5,5′-azobis[1H-tetrazol-1-ide] compounds, rather than to the heavy lanthanide (Tb–Lu) 5,5′-azobis[1H-tetrazol-1-ide] (e.g., [Tb(H2O)8]2ZT3⋅6 H2O) derivatives. Traces of Am seem to force the Tb compound into a structure normally preferred by the lighter lanthanides, despite a 108-fold Tb excess. The americium-doped material was studied by single-crystal X-ray diffraction, vibrational spectroscopy, radiochemical neutron activation analysis, and scanning electron microcopy. In addition, the inclusion properties of terbium 5,5′-azobis[1H-tetrazol-1-ide] towards americium were quantified, and a model for the crystallization process is proposed.

AB - The crystallization of terbium 5,5′-azobis[1H-tetrazol-1-ide] (ZT) in the presence of trace amounts (ca. 50 Bq, ca. 1.6 pmol) of americium results in 1) the accumulation of the americium tracer in the crystalline solid and 2) a material that adopts a different crystal structure to that formed in the absence of americium. Americium-doped [Tb(Am)(H2O)7ZT]2 ZT⋅10 H2O is isostructural to light lanthanide (Ce–Gd) 5,5′-azobis[1H-tetrazol-1-ide] compounds, rather than to the heavy lanthanide (Tb–Lu) 5,5′-azobis[1H-tetrazol-1-ide] (e.g., [Tb(H2O)8]2ZT3⋅6 H2O) derivatives. Traces of Am seem to force the Tb compound into a structure normally preferred by the lighter lanthanides, despite a 108-fold Tb excess. The americium-doped material was studied by single-crystal X-ray diffraction, vibrational spectroscopy, radiochemical neutron activation analysis, and scanning electron microcopy. In addition, the inclusion properties of terbium 5,5′-azobis[1H-tetrazol-1-ide] towards americium were quantified, and a model for the crystallization process is proposed.

KW - actinides

KW - energetic anions/ligands

KW - gadolinium break

KW - lanthanides

KW - structural influence

UR - http://www.scopus.com/inward/record.url?scp=85031101766&partnerID=8YFLogxK

U2 - 10.1002/anie.201703971

DO - 10.1002/anie.201703971

M3 - Article

C2 - 28745419

AN - SCOPUS:85031101766

VL - 56

SP - 13264

EP - 13269

JO - Angewandte Chemie

JF - Angewandte Chemie

SN - 1433-7851

IS - 43

ER -