Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Structural and Electronic Properties of Fluoride Complexes of Nb V , Ta V , and Pa V : The Influence of Relativistic Effects on Group V Elements

Journal Article · · European Journal of Inorganic Chemistry
 [1];  [1];  [2]
  1. Chemical Sciences and Engineering Division Argonne National Laboratory 60439 Argonne IL USA
  2. Univ. Lille CNRS UMR 8523 ‐ PhLAM ‐ Physique des Lasers Atomes et Molécules 59000 Lille France

Aqueous fluorido complexes of niobium and tantalum were studied by using synchrotron‐based extended X‐ray absorption spectroscopy (EXAFS) as model systems for comparison of the structural and coordination chemistry of the group V metals Nb, Ta, and their pseudo‐homologue Pa V . The EXAFS measurements indicate differences in the coordination chemistry of Nb and Ta in these systems that were not intuitively based on their similar charge and ionic radii. The Ta speciation is dominated by six‐ and seven‐coordinate fluorido complexes, while the chemical speciation of Nb under the same conditions is dominated by its hydrolyzed oxyfluoride complexes. Quantum chemical computations were performed to more fully describe these observations, and these results are compared to our earlier study on the fluorido complexes of protactinium. Computations performed with and without the inclusion of scalar relativistic effects reveal that the differences in chemistry among the group V elements and their pseudo‐homologue protactinium are due to the increasing influence of relativistic effects as Z increases from niobium to protactinium.

Sponsoring Organization:
USDOE
Grant/Contract Number:
NONE; AC02-06CH11357
OSTI ID:
1401710
Journal Information:
European Journal of Inorganic Chemistry, Journal Name: European Journal of Inorganic Chemistry Journal Issue: 35 Vol. 2016; ISSN 1434-1948
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

References (56)

Optimized Slater-type basis sets for the elements 1-118 journal May 2003
Chemistry with ADF journal January 2001
Uranyl photophysics book January 1982
Electronic structure and bonding in actinyl ions book January 2006
Effect of electron correlation on the Pa atom energy levels and electron coupling journal February 2011
Towards an order- journal January 1998
Solubility of B-Nb2O5 and the Hydrolysis of Niobium(V) in Aqueous Solution as a Function of Temperature and Ionic Strength journal February 2010
Crystal Chemistry of Tantalum and Niobium Fluoride Compounds book January 2004
Trans-effects in octahedral transition metal complexes journal June 2000
BESSRC-CAT bending magnet beamline at the advanced photon source
  • Beno, Mark A.; Engbretson, Mark; Jennings, Guy
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 467-468 https://doi.org/10.1016/S0168-9002(01)00465-X
journal July 2001
A fast and robust algorithm for Bader decomposition of charge density journal June 2006
An experimental study of the solubility and speciation of niobium in fluoride-bearing aqueous solutions at elevated temperature journal June 2015
Segmented contraction scheme for small-core actinide pseudopotential basis sets journal March 2004
Elucidating Protactinium Hydrolysis: The Relative Stabilities of PaO 2 (H 2 O) + and PaO(OH) 2 + journal July 2015
Reliable Potential Energy Surfaces for the Reactions of H 2 O with ThO 2 , PaO 2 + , UO 2 2+ , and UO 2 + journal November 2015
The electronic structure of actinide-containing molecules: a challenge to applied quantum chemistry journal July 1991
Relativistic effects in structural chemistry journal May 1988
Auxiliary Basis Sets for Density-Fitted MP2 Calculations: Correlation-Consistent Basis Sets for the 4d Elements journal January 2009
M−F Interatomic Distances and Effective Volumes of Second and Third Transition Series MF 6 - and MF 6 2- Anions journal June 2000
Analysis of the 5f1 .fwdarw. 6d1 transitions in hexahaloprotactinate(2-) (halo = chloro, bromo) and protactinium(4+)/thorium tetrabromide journal September 1988
REX calculations. 12. Iteration parameters for the 5f-element organometallics of thorium-neptunium. Geometries of thorium dioxide and uranyl ion revisited journal May 1989
First Structural Characterization of a Protactinium(V) Single Oxo Bond in Aqueous Media journal December 2005
Structural and Spectroscopic Studies of Fluoroprotactinates journal January 2014
Identification of Complex Ions of Niobium(V) in Hydrofluoric Acid Solutions by Raman and Infrared Spectroscopy journal August 1963
A Study by Raman Spectroscopy of Complex Ions Formed by Tantalum (V) in the System Ta (V)-HF-NH 4 F-H 2 O journal March 1966
Fluorine-19 nuclear magnetic resonance and Raman spectral studies of tantalum(V)-fluoride ion complexes in anhydrous hydrogen fluoride solutions journal September 1970
EXAFS Study of the Speciation of Protactinium(V) in Aqueous Hydrofluoric Acid Solutions journal November 2014
Local site symmetry of dispersed molybdenum oxide catalysts: XANES at the Mo L2,3-edges journal June 1993
THE FORMATION CONSTANTS OF THE TANTALUM FLUORIDE SYSTEM. I. POTENTIOMETRIC AND ANION EXCHANGE STUDIES—EVIDENCE FOR SPECIES OF COÖRDINATION NUMBER NINE 1,2 journal January 1962
Theoretical x-ray absorption fine structure standards journal July 1991
Covalency hinders AnO 2 (H 2 O) + → AnO(OH) 2 + isomerisation (An = Pa–Pu) journal January 2016
On the hydrolysis of niobium( V ) and tantalum( V ) in 3 mol dm –3 KCl at 25 °C. Part 1. Construction of a thermodynamic model for Nb V journal January 1994
COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient journal January 1993
On the inverse trans influence. Density functional studies of [MOX5]n– (M = Pa, n = 2; M = U, n = 1; M = Np, n = 0; X = F, Cl or Br) journal February 2002
Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy journal January 2005
Efficient use of the correlation consistent basis sets in resolution of the identity MP2 calculations journal February 2002
Comparative assessment of a new nonempirical density functional: Molecules and hydrogen-bonded complexes journal December 2003
A Variation of the F-Test for Determining Statistical Relevance of Particular Parameters in EXAFS Fits
  • Downward, L.; Booth, C. H.; Lukens, W. W.
  • X-RAY ABSORPTION FINE STRUCTURE - XAFS13: 13th International Conference, AIP Conference Proceedings https://doi.org/10.1063/1.2644450
conference January 2007
Energy-consistent relativistic pseudopotentials and correlation consistent basis sets for the 4d elements Y–Pd journal March 2007
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Relativistic effects in physics and chemistry of element 105. I. Periodicities in properties of group 5 elements. Electronic structure of the pentachlorides journal June 1992
Relativistic effects in physics and chemistry of element 105. III. Electronic structure of hahnium oxyhalides as analogs of group 5 elements oxyhalides journal July 1992
Relativistic effects in physics and chemistry of element 105. IV. Their influence on the electronic structure and related properties journal December 1993
Energy‐adjusted pseudopotentials for the actinides. Parameter sets and test calculations for thorium and thorium monoxide journal May 1994
Towards a first principles prediction of p K a : COSMO-RS and the cluster-continuum approach journal February 2010
An X-ray, NMR, infrared and Raman study of K 2 TaF 7 journal February 1983
Atoms in Molecules book December 1990
Extended x-ray-absorption fine-structure amplitudes—Wave-function relaxation and chemical effects journal January 1978
Theoretical approaches to x-ray absorption fine structure journal July 2000
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal September 1976
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
Relativistic Effects in Chemistry: More Common Than You Thought journal May 2012
Solution Chemistry of Element 105 Part I: Hydrolysis of Group 5 Cations: Nb, Ta, Ha and Pa journal February 1998
Solution Chemistry of Element 105 Part II: Hydrolysis and Complex Formation of Nb, Ta, Ha and Pa in HCl Solutions journal February 1998
Solution Chemistry of Element 105. Part III: Hydrolysis and Complex Formation of Nb, Ta, Db and Pa in HF and HBr Solutions journal January 1999
Structure of early actinides(V) in acidic solutions journal January 2009

Similar Records

Classification of fluorides and oxyfluorides of niobium(V) and tantalum(V) with alkali metals
Journal Article · Tue Dec 31 23:00:00 EST 1985 · J. Struct. Chem. (Engl. Transl.); (United States) · OSTI ID:6369634

EXAFS Study of the Speciation of Protactinium(V) in Aqueous Hydrofluoric Acid Solutions
Journal Article · Sun Nov 30 23:00:00 EST 2014 · Inorganic Chemistry · OSTI ID:1394037

Oxidation of several corrosion-resistant metals in HF-DMF
Journal Article · Thu Feb 19 23:00:00 EST 1987 · Bull. Acad. Sci. USSR, Div. Chem. Sci. (Engl. Transl.); (United States) · OSTI ID:6417961

Related Subjects