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The crystal structure of ianthinite, a mixed-valence uranium oxide hydrate

Conference ·
OSTI ID:572273
 [1];  [2];  [3]; ;  [4]
  1. Univ. of Illinois, Urbana, IL (United States). Dept. of Geology
  2. Argonne National Lab., IL (United States). Chemical Technology Div.
  3. Univ. of Manitoba, Winnipeg, Manitoba (Canada). Dept. of Geological Sciences
  4. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Earth and Planetary Sciences

Ianthinite, [U{sup 4+}{sub 2}(UO{sub 2}){sub 4}O{sub 6}(OH){sub 4}(H{sub 2}O){sub 4}](H{sub 2}O){sub 5}, is the only known uranyl oxide hydrate mineral that contains U{sup 4+}, and it has been proposed that ianthinite may be an important Pu{sup 4+}-bearing phase during the oxidative dissolution of spent nuclear fuel. The crystal structure of ianthinite, orthorhombic, a 7.178(2), b 11.473(2), c 30.39(1) {angstrom}, V 2502.7 {angstrom}{sup 3}, Z = 4, space group P2{sub 1}cn, has been solved by direct methods and refined by least-squares methods to an R index of 9.7% and a wR index of 12.6% using 888 unique observed [{vert_bar}F{vert_bar} {ge} 5{sigma} {vert_bar}F{vert_bar}] reflections. The structure contains both U{sup 6+} and U{sup 4+}. The U{sup 6+} cations are present as roughly linear uranyl ions (Ur) that are in turn coordinated by five O{sup 2{minus}} and OH{sup {minus}} located at the equatorial positions of pentagonal bipyramids. The U{sup 4+} cations are coordinated by O{sup 2{minus}}, OH{sup {minus}} and H{sub 2}O in a distorted octahedral arrangement. The Ur{phi}{sub 5} and U{sup 4+}{phi}{sub 6}({phi}: O{sup 2{minus}}, OH{sup {minus}}, H{sub 2}O) polyhedra link by sharing edges to form two symmetrically distinct sheets at z {approx} 0.0 and z {approx}0.25 that are parallel to (001). There are five symmetrically distinct H{sub 2}O groups between the sheets of U{phi}{sub n} polyhedra, and the sheets of U{phi}{sub n} polyhedra are linked together only by hydrogen bonding to the intersheet H{sub 2}O groups. The crystal-chemical requirements of U{sup 4+} and Pu{sup 4+} are very similar, indicating that extensive Pu{sup 4+} {leftrightarrow} U{sup 4+} substitution can occur within the structure of ianthinite.

Sponsoring Organization:
Natural Sciences and Engineering Research Council of Canada, Ottawa, ON (Canada); USDOE, Washington, DC (United States)
DOE Contract Number:
FG03-95ER14540
OSTI ID:
572273
Report Number(s):
CONF-961202--
Country of Publication:
United States
Language:
English

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