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Title: Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium

Abstract

Advancing our understanding of the minor actinides (Am, Cm) versus lanthanides is key for developing advanced nuclear-fuel cycles. Here in this paper, we describe the preparation of (NBu 4)Am[S 2P( tBu 2C 12H 6)] 4 and two isomorphous lanthanide complexes, namely one with a similar ionic radius (i.e., Nd III) and an isoelectronic one (Eu III). The results include the first measurement of an Am-S bond length, with a mean value of 2.921(9) Å, by single-crystal X-ray diffraction. Comparison with the Eu III and Nd III complexes revealed subtle electronic differences between the complexes of Am III and the lanthanides.

Authors:
 [1];  [2];  [3];  [1];  [3]; ORCiD logo [1];  [1];  [1];  [4];  [1];  [5]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Illinois, Urbana-Champaign, IL (United States)
  3. Univ. of Illinois, Urbana-Champaign, IL (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); California State Polytechnic Univ., Pomona, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Nuclear Physics (NP) (SC-26); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5); National Science Foundation (NSF)
OSTI Identifier:
1435060
Alternate Identifier(s):
OSTI ID: 1401877; OSTI ID: 1441291
Report Number(s):
LA-UR-16-24625
Journal ID: ISSN 1433-7851; ark:/13030/qt3zq898qx; TRN: US1803074
Grant/Contract Number:  
AC02-05CH11231; AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 41; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; actinides; americium; lanthanides; radiochemistry; X-ray diffraction; Inorganic and Physical Chemistry

Citation Formats

Cross, Justin N., Macor, Joseph A., Bertke, Jeffery A., Ferrier, Maryline G., Girolami, Gregory S., Kozimor, Stosh A., Maassen, Joel R., Scott, Brian L., Shuh, David K., Stein, Benjamin W., and Stieber, S. Chantal E.. Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium. United States: N. p., 2016. Web. doi:10.1002/anie.201606367.
Cross, Justin N., Macor, Joseph A., Bertke, Jeffery A., Ferrier, Maryline G., Girolami, Gregory S., Kozimor, Stosh A., Maassen, Joel R., Scott, Brian L., Shuh, David K., Stein, Benjamin W., & Stieber, S. Chantal E.. Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium. United States. doi:10.1002/anie.201606367.
Cross, Justin N., Macor, Joseph A., Bertke, Jeffery A., Ferrier, Maryline G., Girolami, Gregory S., Kozimor, Stosh A., Maassen, Joel R., Scott, Brian L., Shuh, David K., Stein, Benjamin W., and Stieber, S. Chantal E.. Thu . "Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium". United States. doi:10.1002/anie.201606367. https://www.osti.gov/servlets/purl/1435060.
@article{osti_1435060,
title = {Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium},
author = {Cross, Justin N. and Macor, Joseph A. and Bertke, Jeffery A. and Ferrier, Maryline G. and Girolami, Gregory S. and Kozimor, Stosh A. and Maassen, Joel R. and Scott, Brian L. and Shuh, David K. and Stein, Benjamin W. and Stieber, S. Chantal E.},
abstractNote = {Advancing our understanding of the minor actinides (Am, Cm) versus lanthanides is key for developing advanced nuclear-fuel cycles. Here in this paper, we describe the preparation of (NBu4)Am[S2P(tBu2C12H6)]4 and two isomorphous lanthanide complexes, namely one with a similar ionic radius (i.e., NdIII) and an isoelectronic one (EuIII). The results include the first measurement of an Am-S bond length, with a mean value of 2.921(9) Å, by single-crystal X-ray diffraction. Comparison with the EuIII and NdIII complexes revealed subtle electronic differences between the complexes of AmIII and the lanthanides.},
doi = {10.1002/anie.201606367},
journal = {Angewandte Chemie (International Edition)},
number = 41,
volume = 55,
place = {United States},
year = {Thu Sep 15 00:00:00 EDT 2016},
month = {Thu Sep 15 00:00:00 EDT 2016}
}

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Works referenced in this record:

Plutonium(IV) Sequestration: Structural and Thermodynamic Evaluation of the Extraordinarily Stable Cerium(IV) Hydroxypyridinonate Complexes1
journal, September 2000

  • Xu, Jide; Radkov, Emil; Ziegler, Marco
  • Inorganic Chemistry, Vol. 39, Issue 18, p. 4156-4164
  • DOI: 10.1021/ic000063i