High-temperature, high-pressure hydrothermal synthesis, characterization, and structural relationships of layered uranyl arsenates

Hsin Kuan Liu; Eswaran Ramachandran; Yi Hsin Chen; Wen Jung Chang; Kwang Hwa Lii

doi:10.1021/ic501091g

High-temperature, high-pressure hydrothermal synthesis, characterization, and structural relationships of layered uranyl arsenates

Hsin Kuan Liu, Eswaran Ramachandran, Yi Hsin Chen, Wen Jung Chang, Kwang Hwa Lii

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

12 Scopus citations

Abstract

Five new uranyl arsenates, Na₁₄[(UO₂) ₅(AsO₄)₈]·2H₂O (1), K ₆[(UO₂)₅O₅(AsO₄) ₂] (2a), K₄[(UO₂)₃O ₂(AsO₄)₂] (2b), Rb₄[(UO ₂)₃O₂(AsO₄)₂] (3), and Cs₆[(UO₂)₅O₂(AsO₄) ₄] (4), were synthesized by high-temperature, high-pressure hydrothermal reactions at about 560°C and 1440 bar and were characterized by single-crystal X-ray diffraction, thermogravimetric analysis, and photoluminescence spectroscopy. Crystal data for compound 1: triclinic, P1̄, a = 7.0005(3) Å, b = 12.1324(4) Å, c = 13.7428(5) Å, α = 64.175(2)°, β = 89.092(2)°, γ = 85.548(2)°, V = 1047.26(7) Å³, Z = 1, R1 = 0.0185; compound 2a: monoclinic, P2₁/c, a = 6.8615(3) Å, b = 24.702(1) Å, c = 7.1269(3) Å, β = 98.749(2)°, V = 1193.89(9) Å³, Z = 2, R1 = 0.0225; compound 2b: monoclinic, P2₁/c, a = 6.7852(3) Å, b = 17.3640(8) Å, c = 7.1151(3) Å, β = 98.801(3)°, V = 828.42(6) Å³, Z = 2, R1 = 0.0269; compound 3: monoclinic, P2₁/m, a = 6.9783(3) Å, b = 17.4513(8) Å, c = 7.0867(3) Å, β = 90.808(3)°, V = 862.94(7) Å³, Z = 2, R1 = 0.0269; compound 4: triclinic, P1̄, a = 7.7628(3) Å, b = 9.3324(4) Å, c = 11.9336(4) Å, α = 75.611(2)°, β = 73.136(2)°, γ = 86.329(2)°, V = 801.37(5) Å³, Z = 1, R1 = 0.0336. The five compounds have layer structures consisting of uranyl square, pentagonal, and hexagonal bipyramids as well as AsO₄ tetrahedra. Compound 1 contains chains of discrete uranyl square and pentagonal bipyramids, 2a contains three-polyhedron-wide ribbons of edge- and corner-sharing uranyl square and pentagonal bipyramids, 2b and 3 contain dimers of edge-shairing pentagonal bipyramids that share edges with hexagonal bipyramids to form chains, and 4 contains one-polyhedron-wide zigzag chains of edge-sharing uranyl polyhedra. The double sheet structure of 1 is new, but the chain topology has been observed in an organically templated uranyl sulfate. Compound 2b is a new geometrical isomer of the phosphuranylite group. The sheet anion topologies of 2a and 4 can be obtained by splitting the β-U ₃O₈-type sheet into complex chains and connecting the chains by arsenates.

Original language	English
Pages (from-to)	9065-9072
Number of pages	8
Journal	Inorganic Chemistry
Volume	53
Issue number	17
DOIs	https://doi.org/10.1021/ic501091g
State	Published - 2 Sep 2014

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10.1021/ic501091g

CSD 1031818: Experimental Crystal Structure Determination
Liu, H.-K. (Creator), Ramachandran, E. (Creator), Chen, Y.-H. (Creator), Chang, W.-J. (Creator) & Lii, K.-H. (Creator), The Cambridge Structural Database, 2014
DOI: 10.25505/fiz.icsd.cc13mpgw, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc13mpgw&sid=DataCite
Dataset
CSD 1031821: Experimental Crystal Structure Determination
Liu, H.-K. (Creator), Ramachandran, E. (Creator), Chen, Y.-H. (Creator), Chang, W.-J. (Creator) & Lii, K.-H. (Creator), The Cambridge Structural Database, 2014
DOI: 10.25505/fiz.icsd.cc13mpkz, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc13mpkz&sid=DataCite
Dataset
CSD 1031820: Experimental Crystal Structure Determination
Liu, H.-K. (Creator), Ramachandran, E. (Creator), Chen, Y.-H. (Creator), Chang, W.-J. (Creator) & Lii, K.-H. (Creator), The Cambridge Structural Database, 2014
DOI: 10.25505/fiz.icsd.cc13mpjy, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc13mpjy&sid=DataCite
Dataset

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@article{8956d53a7c93420bab65118361737704,

title = "High-temperature, high-pressure hydrothermal synthesis, characterization, and structural relationships of layered uranyl arsenates",

abstract = "Five new uranyl arsenates, Na14[(UO2) 5(AsO4)8]·2H2O (1), K 6[(UO2)5O5(AsO4) 2] (2a), K4[(UO2)3O 2(AsO4)2] (2b), Rb4[(UO 2)3O2(AsO4)2] (3), and Cs6[(UO2)5O2(AsO4) 4] (4), were synthesized by high-temperature, high-pressure hydrothermal reactions at about 560°C and 1440 bar and were characterized by single-crystal X-ray diffraction, thermogravimetric analysis, and photoluminescence spectroscopy. Crystal data for compound 1: triclinic, P{\=1}, a = 7.0005(3) {\AA}, b = 12.1324(4) {\AA}, c = 13.7428(5) {\AA}, α = 64.175(2)°, β = 89.092(2)°, γ = 85.548(2)°, V = 1047.26(7) {\AA}3, Z = 1, R1 = 0.0185; compound 2a: monoclinic, P21/c, a = 6.8615(3) {\AA}, b = 24.702(1) {\AA}, c = 7.1269(3) {\AA}, β = 98.749(2)°, V = 1193.89(9) {\AA}3, Z = 2, R1 = 0.0225; compound 2b: monoclinic, P21/c, a = 6.7852(3) {\AA}, b = 17.3640(8) {\AA}, c = 7.1151(3) {\AA}, β = 98.801(3)°, V = 828.42(6) {\AA}3, Z = 2, R1 = 0.0269; compound 3: monoclinic, P21/m, a = 6.9783(3) {\AA}, b = 17.4513(8) {\AA}, c = 7.0867(3) {\AA}, β = 90.808(3)°, V = 862.94(7) {\AA}3, Z = 2, R1 = 0.0269; compound 4: triclinic, P{\=1}, a = 7.7628(3) {\AA}, b = 9.3324(4) {\AA}, c = 11.9336(4) {\AA}, α = 75.611(2)°, β = 73.136(2)°, γ = 86.329(2)°, V = 801.37(5) {\AA}3, Z = 1, R1 = 0.0336. The five compounds have layer structures consisting of uranyl square, pentagonal, and hexagonal bipyramids as well as AsO4 tetrahedra. Compound 1 contains chains of discrete uranyl square and pentagonal bipyramids, 2a contains three-polyhedron-wide ribbons of edge- and corner-sharing uranyl square and pentagonal bipyramids, 2b and 3 contain dimers of edge-shairing pentagonal bipyramids that share edges with hexagonal bipyramids to form chains, and 4 contains one-polyhedron-wide zigzag chains of edge-sharing uranyl polyhedra. The double sheet structure of 1 is new, but the chain topology has been observed in an organically templated uranyl sulfate. Compound 2b is a new geometrical isomer of the phosphuranylite group. The sheet anion topologies of 2a and 4 can be obtained by splitting the β-U 3O8-type sheet into complex chains and connecting the chains by arsenates.",

author = "Liu, {Hsin Kuan} and Eswaran Ramachandran and Chen, {Yi Hsin} and Chang, {Wen Jung} and Lii, {Kwang Hwa}",

year = "2014",

month = sep,

day = "2",

doi = "10.1021/ic501091g",

language = "???core.languages.en_GB???",

volume = "53",

pages = "9065--9072",

journal = "Inorganic Chemistry",

issn = "0020-1669",

number = "17",

}

TY - JOUR

T1 - High-temperature, high-pressure hydrothermal synthesis, characterization, and structural relationships of layered uranyl arsenates

AU - Liu, Hsin Kuan

AU - Ramachandran, Eswaran

AU - Chen, Yi Hsin

AU - Chang, Wen Jung

AU - Lii, Kwang Hwa

PY - 2014/9/2

Y1 - 2014/9/2

N2 - Five new uranyl arsenates, Na14[(UO2) 5(AsO4)8]·2H2O (1), K 6[(UO2)5O5(AsO4) 2] (2a), K4[(UO2)3O 2(AsO4)2] (2b), Rb4[(UO 2)3O2(AsO4)2] (3), and Cs6[(UO2)5O2(AsO4) 4] (4), were synthesized by high-temperature, high-pressure hydrothermal reactions at about 560°C and 1440 bar and were characterized by single-crystal X-ray diffraction, thermogravimetric analysis, and photoluminescence spectroscopy. Crystal data for compound 1: triclinic, P1̄, a = 7.0005(3) Å, b = 12.1324(4) Å, c = 13.7428(5) Å, α = 64.175(2)°, β = 89.092(2)°, γ = 85.548(2)°, V = 1047.26(7) Å3, Z = 1, R1 = 0.0185; compound 2a: monoclinic, P21/c, a = 6.8615(3) Å, b = 24.702(1) Å, c = 7.1269(3) Å, β = 98.749(2)°, V = 1193.89(9) Å3, Z = 2, R1 = 0.0225; compound 2b: monoclinic, P21/c, a = 6.7852(3) Å, b = 17.3640(8) Å, c = 7.1151(3) Å, β = 98.801(3)°, V = 828.42(6) Å3, Z = 2, R1 = 0.0269; compound 3: monoclinic, P21/m, a = 6.9783(3) Å, b = 17.4513(8) Å, c = 7.0867(3) Å, β = 90.808(3)°, V = 862.94(7) Å3, Z = 2, R1 = 0.0269; compound 4: triclinic, P1̄, a = 7.7628(3) Å, b = 9.3324(4) Å, c = 11.9336(4) Å, α = 75.611(2)°, β = 73.136(2)°, γ = 86.329(2)°, V = 801.37(5) Å3, Z = 1, R1 = 0.0336. The five compounds have layer structures consisting of uranyl square, pentagonal, and hexagonal bipyramids as well as AsO4 tetrahedra. Compound 1 contains chains of discrete uranyl square and pentagonal bipyramids, 2a contains three-polyhedron-wide ribbons of edge- and corner-sharing uranyl square and pentagonal bipyramids, 2b and 3 contain dimers of edge-shairing pentagonal bipyramids that share edges with hexagonal bipyramids to form chains, and 4 contains one-polyhedron-wide zigzag chains of edge-sharing uranyl polyhedra. The double sheet structure of 1 is new, but the chain topology has been observed in an organically templated uranyl sulfate. Compound 2b is a new geometrical isomer of the phosphuranylite group. The sheet anion topologies of 2a and 4 can be obtained by splitting the β-U 3O8-type sheet into complex chains and connecting the chains by arsenates.

AB - Five new uranyl arsenates, Na14[(UO2) 5(AsO4)8]·2H2O (1), K 6[(UO2)5O5(AsO4) 2] (2a), K4[(UO2)3O 2(AsO4)2] (2b), Rb4[(UO 2)3O2(AsO4)2] (3), and Cs6[(UO2)5O2(AsO4) 4] (4), were synthesized by high-temperature, high-pressure hydrothermal reactions at about 560°C and 1440 bar and were characterized by single-crystal X-ray diffraction, thermogravimetric analysis, and photoluminescence spectroscopy. Crystal data for compound 1: triclinic, P1̄, a = 7.0005(3) Å, b = 12.1324(4) Å, c = 13.7428(5) Å, α = 64.175(2)°, β = 89.092(2)°, γ = 85.548(2)°, V = 1047.26(7) Å3, Z = 1, R1 = 0.0185; compound 2a: monoclinic, P21/c, a = 6.8615(3) Å, b = 24.702(1) Å, c = 7.1269(3) Å, β = 98.749(2)°, V = 1193.89(9) Å3, Z = 2, R1 = 0.0225; compound 2b: monoclinic, P21/c, a = 6.7852(3) Å, b = 17.3640(8) Å, c = 7.1151(3) Å, β = 98.801(3)°, V = 828.42(6) Å3, Z = 2, R1 = 0.0269; compound 3: monoclinic, P21/m, a = 6.9783(3) Å, b = 17.4513(8) Å, c = 7.0867(3) Å, β = 90.808(3)°, V = 862.94(7) Å3, Z = 2, R1 = 0.0269; compound 4: triclinic, P1̄, a = 7.7628(3) Å, b = 9.3324(4) Å, c = 11.9336(4) Å, α = 75.611(2)°, β = 73.136(2)°, γ = 86.329(2)°, V = 801.37(5) Å3, Z = 1, R1 = 0.0336. The five compounds have layer structures consisting of uranyl square, pentagonal, and hexagonal bipyramids as well as AsO4 tetrahedra. Compound 1 contains chains of discrete uranyl square and pentagonal bipyramids, 2a contains three-polyhedron-wide ribbons of edge- and corner-sharing uranyl square and pentagonal bipyramids, 2b and 3 contain dimers of edge-shairing pentagonal bipyramids that share edges with hexagonal bipyramids to form chains, and 4 contains one-polyhedron-wide zigzag chains of edge-sharing uranyl polyhedra. The double sheet structure of 1 is new, but the chain topology has been observed in an organically templated uranyl sulfate. Compound 2b is a new geometrical isomer of the phosphuranylite group. The sheet anion topologies of 2a and 4 can be obtained by splitting the β-U 3O8-type sheet into complex chains and connecting the chains by arsenates.

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U2 - 10.1021/ic501091g

DO - 10.1021/ic501091g

M3 - 期刊論文

AN - SCOPUS:84906858441

SN - 0020-1669

VL - 53

SP - 9065

EP - 9072

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 17

ER -

High-temperature, high-pressure hydrothermal synthesis, characterization, and structural relationships of layered uranyl arsenates

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Datasets

CSD 1031818: Experimental Crystal Structure Determination

CSD 1031821: Experimental Crystal Structure Determination

CSD 1031820: Experimental Crystal Structure Determination

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