Journal
CRYSTAL GROWTH & DESIGN
Volume 17, Issue 11, Pages 5898-5907Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.cgd.7b00997
Keywords
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Funding
- Helmholtz Association [VH-NG-815]
- Center for Actinide Science and Technology (CAST), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0016568]
- National Natural Science Foundation of China [21422704]
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A series of novel uranyl borates, K4Sr4[UO2)(13)(B2O5)(2)(BO3)(2)O-12], A(6)[(UO2)(12)(BO3)(8)O-3](H2O)(6) (A = Rb and Cs), and Rb-3[UO2)(3)(BO3)(2)O(OH)]-(H2O), were synthesized using conventional conditions. Among them, K4Sr4[(UO2)(13)(B2O5)(2)(BO3)(2)O-12] and A(6)[(UO2)(12)(BO3)(8)O-3](H2O)(6) were obtained through a high -temperature solid-state reaction method, whereas RE3[(UO2)(3)-(BO3)(2)O(OH)](H2O) was synthesized via a hydrothermal reaction. All compounds adopt novel two-dimensional (2D) layered structures in which basic building units (BBUs) consist of corner- or edge-sharing UOx (x = 6, 7 and 8) polyhedra linked with planar BO3 triangles or B2O5 dimers. K4Sr4[UO2)(13)(B2O5)(2)(BO3)(2)O-12] is the first mixed alkali-alkaline earth metal uranyl borate. This compound has the most complex 2D anion topology observed thus far in 2D uranyl borates. The fundamental building block (FBB) in this structure, [UO2)(13)(B2O5)(2)(BO3)(2)O-12](12-), consists of 3 UO8 hexagonal bipyramids and 10 UO7 pentagonal bipyramids connected with 2 BO3 triangles and 2 B2O5 dimers. The FBB of Rb-6[(UO2)(12)(BO3)(8)O-3](H-2)(6) is [UO2)(6)(BO3)(4)O-3](6-), comprised of five edg-sharing UO7 pentagonal bipyramids, one UO6 tetragonal bipyramid, and four BO3 triangles. The simplest FBB, [(UO2)(3)(BO3)(2)O-2](4-), occurs in Rb-3[(UO2)(3)(BO3)(2)O(OH)](H2O), where three UO7 pentagonal bipyramids are linked with two BO3 triangles via edge sharing. The aforementioned FBBs are further polymerized into the corresponding infinite uranyl borates layers. The synthetic methods, novel topologies, thermal stability, and spectroscopic properties of these compounds are reported herein.
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