Honeycomb-like S = 5/2 Spin–Lattices in Manganese(II) Vanadates
Abstract
We synthesized new complex manganese vanadate materials as high-quality single crystals in multi-millimeter lengths using a high-temperature, high-pressure hydrothermal method. We grew one compound, Mn5(VO4)2(OH)4, from Mn2O3 and V2O5 in 3 M CsOH at 580 °C and 1.5 kbar. Changing the mineralizer to 1 M CsOH/3MCsCl leads to the formation of another product, Mn6O(VO4)2(OH). Both compounds were structurally characterized by single-crystal X-ray diffraction (Mn5(VO4)2(OH)4: C2/m, Z = 2, a = 9.6568(9) Å, b = 9.5627(9) Å, c = 5.4139(6) Å, β = 98.529(8)°; Mn6O(VO4)2(OH): P21/m, Z = 2, a = 8.9363(12) Å, b = 6.4678(8) Å, c = 10.4478(13) Å, β = 99.798(3)°), revealing interesting low-dimensional transition-metal features. Mn5(VO4)2(OH)4 possesses complex honeycomb-type Mn–O layers, built from edge-sharing [MnO6] octahedra in the bc plane, with bridging vanadate groups connecting these layers along the a-axis. Mn6O(VO4)2(OH) presents a more complicated structure with both octahedral [MnO6] and trigonal bipyramidal [MnO5] units. A different pattern of planar honeycomb sheets are formed by edge-shared [MnO6] octahedra, and these sublattices are connected through edge-shared dimers of [MnO5] trigonal bipyramids to form corrugated sheets. Vanadate groups again condense the sheets into a three-dimensional framework. Infrared and Raman spectroscopies indicated the presence of OH groups and displayed characteristicmore »
- Authors:
-
- Clemson Univ., SC (United States). Dept. of Chemistry and Center for Optical Materials Science and Engineering Technologies
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1352765
- Grant/Contract Number:
- AC05-00OR22725; DMR-1410727
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 55; Journal Issue: 18; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Sanjeewa, Liurukara. D., McGuire, Michael A., McMillen, Colin D., Willett, Daniel, Chumanov, George, and Kolis, Joseph W. Honeycomb-like S = 5/2 Spin–Lattices in Manganese(II) Vanadates. United States: N. p., 2016.
Web. doi:10.1021/acs.inorgchem.6b01286.
Sanjeewa, Liurukara. D., McGuire, Michael A., McMillen, Colin D., Willett, Daniel, Chumanov, George, & Kolis, Joseph W. Honeycomb-like S = 5/2 Spin–Lattices in Manganese(II) Vanadates. United States. https://doi.org/10.1021/acs.inorgchem.6b01286
Sanjeewa, Liurukara. D., McGuire, Michael A., McMillen, Colin D., Willett, Daniel, Chumanov, George, and Kolis, Joseph W. Fri .
"Honeycomb-like S = 5/2 Spin–Lattices in Manganese(II) Vanadates". United States. https://doi.org/10.1021/acs.inorgchem.6b01286. https://www.osti.gov/servlets/purl/1352765.
@article{osti_1352765,
title = {Honeycomb-like S = 5/2 Spin–Lattices in Manganese(II) Vanadates},
author = {Sanjeewa, Liurukara. D. and McGuire, Michael A. and McMillen, Colin D. and Willett, Daniel and Chumanov, George and Kolis, Joseph W.},
abstractNote = {We synthesized new complex manganese vanadate materials as high-quality single crystals in multi-millimeter lengths using a high-temperature, high-pressure hydrothermal method. We grew one compound, Mn5(VO4)2(OH)4, from Mn2O3 and V2O5 in 3 M CsOH at 580 °C and 1.5 kbar. Changing the mineralizer to 1 M CsOH/3MCsCl leads to the formation of another product, Mn6O(VO4)2(OH). Both compounds were structurally characterized by single-crystal X-ray diffraction (Mn5(VO4)2(OH)4: C2/m, Z = 2, a = 9.6568(9) Å, b = 9.5627(9) Å, c = 5.4139(6) Å, β = 98.529(8)°; Mn6O(VO4)2(OH): P21/m, Z = 2, a = 8.9363(12) Å, b = 6.4678(8) Å, c = 10.4478(13) Å, β = 99.798(3)°), revealing interesting low-dimensional transition-metal features. Mn5(VO4)2(OH)4 possesses complex honeycomb-type Mn–O layers, built from edge-sharing [MnO6] octahedra in the bc plane, with bridging vanadate groups connecting these layers along the a-axis. Mn6O(VO4)2(OH) presents a more complicated structure with both octahedral [MnO6] and trigonal bipyramidal [MnO5] units. A different pattern of planar honeycomb sheets are formed by edge-shared [MnO6] octahedra, and these sublattices are connected through edge-shared dimers of [MnO5] trigonal bipyramids to form corrugated sheets. Vanadate groups again condense the sheets into a three-dimensional framework. Infrared and Raman spectroscopies indicated the presence of OH groups and displayed characteristic Raman scattering due to vanadate groups. Furthermore, temperature-dependent magnetic studies indicated Curie–Weiss behavior above 100 K with significant anti-ferromagnetic coupling for both compounds, with further complex magnetic behavior at lower temperatures. The data indicate canted anti-ferromagnetic order below 57 K in Mn5(VO4)2(OH)4 and below 45 K in Mn6O(VO4)2(OH). Members of another class of compounds, K2M3(VO4)2(OH)2 (M = Mn, Co), also containing a honeycomb-type sublattice, were also synthesized to allow a comparison of the structural features across all three structure types and to demonstrate extension to other transition metals.},
doi = {10.1021/acs.inorgchem.6b01286},
journal = {Inorganic Chemistry},
number = 18,
volume = 55,
place = {United States},
year = {2016},
month = {8}
}
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