Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state

被引：79

作者：

Silver, Mark A. ^{[1
]}

Cary, Samantha K. ^{[1
]}

Johnson, Jason A. ^{[2
]}

Baumbach, Ryan E. ^{[3
]}

Arico, Alexandra A. ^{[1
]}

Luckey, Morgan ^{[4
,5
]}

Urban, Matthew ^{[4
,5
]}

Wang, Jamie C. ^{[1
]}

Polinski, Matthew J. ^{[6
]}

Chemey, Alexander ^{[1
]}

Liu, Guokui ^{[7
]}

Chen, Kuan-Wen ^{[3
]}

Van Cleve, Shelley M. ^{[8
]}

Marsh, Matthew L. ^{[1
]}

Eaton, Teresa M. ^{[1
]}

de Burgt, Lambertus J. van ^{[1
]}

Gray, Ashley L. ^{[2
]}

Hobart, David E. ^{[1
]}

Hanson, Kenneth ^{[1
]}

Maron, Laurent ^{[9
]}

Gendron, Frederic ^{[10
]}

Autschbach, Jochen ^{[10
]}

Speldrich, Manfred ^{[11
]}

Koegerler, Paul ^{[11
]}

Yang, Ping ^{[12
]}

Braley, Jenifer ^{[4
,5
]}

Albrecht-Schmitt, Thomas E. ^{[1
]}

机构：

[1] Florida State Univ, Dept Chem & Biochem, Tallahassee, FL 32306 USA

[2] Florida State Univ, Environm Hlth & Safety, Tallahassee, FL 32306 USA

[3] Natl High Magnet Field Lab, Tallahassee, FL 32310 USA

[4] Colorado Sch Mines, Dept Chem & Geochem, Golden, CO 80401 USA

[5] Colorado Sch Mines, Dept Nucl Engn, Golden, CO 80401 USA

[6] Bloomsburg Univ Penn, Dept Chem & Biochem, Bloomsburg, PA 17815 USA

[7] Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA

[8] Oak Ridge Natl Lab, Nucl Mat Proc Grp, One Bethel Valley Rd, Oak Ridge, TN 37830 USA

[9] Inst Natl Sci Appl, Lab Phys & Chim Nanoobjets, F-31077 Toulouse 4, France

[10] SUNY Buffalo, Univ Buffalo, Dept Chem, Buffalo, NY 14260 USA

[11] Univ Aachen, Inst Anorgan Chem, Rheinisch Westfal Tech Hsch, D-52074 Aachen, Germany

[12] Los Alamos Natl Lab, Div Theory, Los Alamos, NM 87545 USA

来源：

SCIENCE | 2016年 / 353卷 / 6302期

基金：

欧洲研究理事会; 美国国家科学基金会;

关键词：

MOLECULAR-ORBITAL METHODS; VALENCE BASIS-SETS; TRIVALENT ACTINIDE; CRYSTAL-STRUCTURES; CALIFORNIUM; ENERGY; ELEMENT; COVALENCY; PLUTONIUM(III); SPECTRA;

D O I：

10.1126/science.aaf3762

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Berkelium is positioned at a crucial location in the actinide series between the inherently stable half-filled 5f(7) configuration of curium and the abrupt transition in chemical behavior created by the onset of a metastable divalent state that starts at californium. However, the mere 320-day half-life of berkelium's only available isotope, Bk-249, has hindered in-depth studies of the element's coordination chemistry. Herein, we report the synthesis and detailed solid-state and solution-phase characterization of a berkelium coordination complex, Bk(III)tris(dipicolinate), as well as a chemically distinct Bk(III) borate material for comparison. We demonstrate that berkelium's complexation is analogous to that of californium. However, from a range of spectroscopic techniques and quantum mechanical calculations, it is clear that spin-orbit coupling contributes significantly to berkelium's multiconfigurational ground state.

引用

页数：8

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