Flux Synthesis of a Metal Carbide Hydride Using Anthracene As a Reactant

Engstrand, Tate O.; Cope, Emily M.; Vasquez, Guillermo; Haddock, Jo W.; Hertz, Mary B.; Wang, Xiaoping; Latturner, Susan E.

doi:10.1021/acs.inorgchem.0c01505

Flux Synthesis of a Metal Carbide Hydride Using Anthracene As a Reactant

Journal Article · Tue Aug 04 00:00:00 EDT 2020 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.0c01505· OSTI ID:1771895

Engstrand, Tate O. ^[1]; Cope, Emily M. ^[1]; Vasquez, Guillermo ^[1]; Haddock, Jo W. ^[1]; Hertz, Mary B. ^[1]; ^[2]; ^[1]

Florida State Univ., Tallahassee, FL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this study, La₁₅(FeC₆)₄H was synthesized from the reaction of iron and anthracene in La/Ni eutectic flux. Anthracene was the source of both the carbon and hydrogen in the product. The structure of this metal carbide hydride features hydride ions in tetrahedral interstitial sites surrounded by lanthanum ions, which was confirmed by single-crystal neutron diffraction studies. The trigonal planar FeC₆ units in which the central iron atom is coordinated by three ethylenide groups are similar to those found in La_3.67FeC₆, a previously reported compound that is formed in the absence of a hydride source. Magnetic susceptibility data confirm that the iron sites do not have magnetic moments. Density of states calculations indicate that La₁₅(FeC₆)₄H is metallic and is stabilized by the incorporation of hydride anions.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1771895

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 16 Vol. 59; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (41)

The Metal Flux: A Preparative Tool for the Exploration of Intermetallic Compounds Kanatzidis, Mercouri G.; Pöttgen, Rainer; Jeitschko, Wolfgang Angewandte Chemie International Edition, Vol. 44, Issue 43 https://doi.org/10.1002/anie.200462170	journal	November 2005
Planar Fe6 Cluster Units in the Crystal Structure of RE15Fe8C25 (RE=Y, Dy, Ho, Er) Davaasuren, Bambar; Borrmann, Horst; Dashjav, Enkhtsetseg Angewandte Chemie International Edition, Vol. 49, Issue 33 https://doi.org/10.1002/anie.201002338	journal	July 2010
Two Germanide Hydride Phases Grown in Calcium-Rich Flux: Use of Interstitial Elements for Discovery of New Phases Lang, David A.; Latturner, Susan E. European Journal of Inorganic Chemistry, Vol. 2011, Issue 26 https://doi.org/10.1002/ejic.201100325	journal	July 2011
Neutron Instruments for Research in Coordination Chemistry: Neutron Instruments for Research in Coordination Chemistry Xue, Zi-Ling; Ramirez-Cuesta, Anibal J.; Brown, Craig M. European Journal of Inorganic Chemistry, Vol. 2019, Issue 8 https://doi.org/10.1002/ejic.201801076	journal	January 2019
Structure and Bonding of La ₂ NiBi: Structure and Bonding of La ₂ NiBi Ott, Claudia; Baumgartner, Max; Schäfer, Konrad Zeitschrift für anorganische und allgemeine Chemie, Vol. 645, Issue 3 https://doi.org/10.1002/zaac.201800237	journal	September 2018
Tin‐rich Phases RE ₂ Au ₃ Sn ₆ with RE = La, Ce, Pr, Nd, Sm – Synthesis, Structure, Magnetic Properties, and ¹¹⁹ Sn Mössbauer Spectra Engelbert, Simon; Janka, Oliver; Klenner, Steffen Zeitschrift für anorganische und allgemeine Chemie, Vol. 646, Issue 18 https://doi.org/10.1002/zaac.201900329	journal	January 2020
Investigations on the LaCo5H and CeCo5H systems Kuijpers, F. A. Journal of the Less Common Metals, Vol. 27, Issue 1 https://doi.org/10.1016/0022-5088(72)90101-4	journal	April 1972
An X-Ray investigation of the phase relationships in the system LaH2LaH3 Boroch, E.; Conder, K.; Ru-Xiu, Cai Journal of the Less Common Metals, Vol. 156, Issue 1-2 https://doi.org/10.1016/0022-5088(89)90424-4	journal	December 1989
Magnetic structure of ternary rare earth carbides of the type R2Fe17C Haije, W. G.; Jacobs, T. H.; Buschow, K. H. J. Journal of the Less Common Metals, Vol. 163, Issue 2 https://doi.org/10.1016/0022-5088(90)90602-G	journal	October 1990
Organometallic structural units in solid state ternary transition metal carbides Bruce King, R. Journal of Organometallic Chemistry, Vol. 536-537 https://doi.org/10.1016/S0022-328X(96)06718-6	journal	May 1997
High-performance Pr2Fe14C-type magnets prepared by melt spinning Zhang, Wen-Yong; Du, Hong-Lin; Jiang, Jian-Sheng Journal of Magnetism and Magnetic Materials, Vol. 257, Issue 2-3 https://doi.org/10.1016/S0304-8853(02)01283-0	journal	February 2003
Properties of intermetallic compounds suitable for hydrogen storage applications Dantzer, P. Materials Science and Engineering: A, Vol. 329-331 https://doi.org/10.1016/S0921-5093(01)01590-8	journal	June 2002
Critical review on the elastic properties of transition metal carbides, nitrides and carbonitrides Kral, C.; Lengauer, W.; Rafaja, D. Journal of Alloys and Compounds, Vol. 265, Issue 1-2 https://doi.org/10.1016/S0925-8388(97)00297-1	journal	January 1998
Hydrogen stabilization. Leon-Escamilla, E. Alejandro; Corbett, John D. Journal of Alloys and Compounds, Vol. 265, Issue 1-2 https://doi.org/10.1016/S0925-8388(97)00320-4	journal	January 1998
Repulsive carbon–deuterium interactions in zirconium and titanium carbodeuterides Guzik, Matylda N.; Hauback, Bjørn C.; Yvon, Klaus Journal of Alloys and Compounds, Vol. 461, Issue 1-2 https://doi.org/10.1016/j.jallcom.2007.07.085	journal	August 2008
Direct observation of crystallographic and chemical changes during dehydrogenation of oxygen contaminated La2C3H1.5 Kienle, L.; García García, F. J.; Duppel, V. Journal of Solid State Chemistry, Vol. 179, Issue 4 https://doi.org/10.1016/j.jssc.2005.12.019	journal	April 2006
Reinvestigation and superstructure of La3.67[Fe(C2)3] Davaasuren, Bambar; Dashjav, Enkhtsetseg; Kreiner, Guido Journal of Solid State Chemistry, Vol. 182, Issue 6 https://doi.org/10.1016/j.jssc.2009.01.040	journal	June 2009
Structural relationships between new carbide La14Sn(MnC6)3 and fully ordered La11(MnC6)3 Zaikina, Julia V.; Zhou, Haidong; Latturner, Susan E. Journal of Solid State Chemistry, Vol. 183, Issue 12 https://doi.org/10.1016/j.jssc.2010.10.004	journal	December 2010
Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments Arnold, O.; Bilheux, J. C.; Borreguero, J. M. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764 https://doi.org/10.1016/j.nima.2014.07.029	journal	November 2014
Clusters, Assemble: Growth of Intermetallic Compounds from Metal Flux Reactions Latturner, Susan E. Accounts of Chemical Research, Vol. 51, Issue 1 https://doi.org/10.1021/acs.accounts.7b00483	journal	December 2017
Pr ₆₂ Fe ₂₁ M ₁₆ C ₃₂ Versus Pr ₂₁ Fe ₈ M ₇ ^′ C ₁₂ (M = Si, P; M′ = Si, Ge, Sn): Competing Intermetallic Carbides Grown from a Pr/Ni Flux Engstrand, Tate O.; Latturner, Susan E. Inorganic Chemistry, Vol. 58, Issue 1 https://doi.org/10.1021/acs.inorgchem.8b02741	journal	December 2018
Structural, chemical, and physical properties of rare-earth metal rhodium carbides LnRhC2 (Ln = La, Ce, Pr, Nd, Sm) Hoffmann, Rolf Dieter; Jeitschko, Wolfgang; Boonk, Ludger Chemistry of Materials, Vol. 1, Issue 6 https://doi.org/10.1021/cm00006a007	journal	November 1989
Ca ₅₄ In ₁₃ B _{4– x} H _{23+ x} : A Complex Metal Subhydride Featuring Ionic and Metallic Regions Blankenship, Trevor V.; Chen, Banghao; Latturner, Susan E. Chemistry of Materials, Vol. 26, Issue 10 https://doi.org/10.1021/cm5007982	journal	May 2014
Rare Earth-Hydrogen Systems. I. Structural and Thermodynamic Properties Korst, William L.; Warf, James C. Inorganic Chemistry, Vol. 5, Issue 10 https://doi.org/10.1021/ic50044a018	journal	October 1966
Synthesis, Crystal Structure, and Magnetic Properties of Novel Intermetallic Compounds R ₂ Co ₂ SiC (R = Pr, Nd) Zhou, Sixuan; Mishra, Trinath; Wang, Man Inorganic Chemistry, Vol. 53, Issue 12 https://doi.org/10.1021/ic5005984	journal	May 2014
Preparation and some properties of ytterbium carbide hydrides Haschke, John M. Inorganic Chemistry, Vol. 14, Issue 4 https://doi.org/10.1021/ic50146a016	journal	April 1975
Ca ₁₂ InC _{13– x} and Ba ₁₂ InC ₁₈ H ₄ : Alkaline-Earth Indium Allenylides Synthesized in AE/Li Flux (AE = Ca, Ba) Blankenship, Trevor V.; Dickman, Matthew J.; van de Burgt, Lambertus J. Inorganic Chemistry, Vol. 54, Issue 3 https://doi.org/10.1021/ic502315m	journal	November 2014
The Structure of Ethylene from Infrared Spectra ¹ Allen, Harry C.; Plyler, Earle K. Journal of the American Chemical Society, Vol. 80, Issue 11 https://doi.org/10.1021/ja01544a021	journal	June 1958
Ca ₂ LiC ₃ H: A New Complex Carbide Hydride Phase Grown in Metal Flux Lang, David A.; Zaikina, Julia V.; Lovingood, Derek D. Journal of the American Chemical Society, Vol. 132, Issue 49 https://doi.org/10.1021/ja107436n	journal	December 2010
A Tale of Two Metals: New Cerium Iron Borocarbide Intermetallics Grown from Rare-Earth/Transition Metal Eutectic Fluxes Tucker, Patricia C.; Nyffeler, Jason; Chen, Banghao Journal of the American Chemical Society, Vol. 134, Issue 29 https://doi.org/10.1021/ja303370j	journal	July 2012
Gd ₁₃ Fe ₁₀ C ₁₃ : Indications of Fe–Fe Multiple Bonding Emerging from Chemical Frustration Hadler, Amelia B.; Fredrickson, Daniel C. Journal of the American Chemical Society, Vol. 134, Issue 25 https://doi.org/10.1021/ja3034944	journal	June 2012
Spin Glass Behavior of Isolated, Geometrically Frustrated Tetrahedra of Iron Atoms in the Intermetallic La ₂₁ Fe ₈ Sn ₇ C ₁₂ Benbow, Evan M.; Dalal, Naresh S.; Latturner, Susan E. Journal of the American Chemical Society, Vol. 131, Issue 9 https://doi.org/10.1021/ja809084n	journal	March 2009
Linear methods in band theory Andersen, O. Krogh Physical Review B, Vol. 12, Issue 8 https://doi.org/10.1103/PhysRevB.12.3060	journal	October 1975
Improved tetrahedron method for Brillouin-zone integrations Blöchl, Peter E.; Jepsen, O.; Andersen, O. K. Physical Review B, Vol. 49, Issue 23 https://doi.org/10.1103/PhysRevB.49.16223	journal	June 1994
Evidence for Superconductivity above 260 K in Lanthanum Superhydride at Megabar Pressures Somayazulu, Maddury; Ahart, Muhtar; Mishra, Ajay K. Physical Review Letters, Vol. 122, Issue 2 https://doi.org/10.1103/PhysRevLett.122.027001	journal	January 2019
CrystalPlan : an experiment-planning tool for crystallography Zikovsky, Janik; Peterson, Peter F.; Wang, Xiaoping P. Journal of Applied Crystallography, Vol. 44, Issue 2 https://doi.org/10.1107/S0021889811007102	journal	March 2011
Integration of neutron time-of-flight single-crystal Bragg peaks in reciprocal space Schultz, Arthur J.; Jørgensen, Mads Ry Vogel; Wang, Xiaoping Journal of Applied Crystallography, Vol. 47, Issue 3 https://doi.org/10.1107/S1600576714006372	journal	May 2014
Crystal structure refinement with SHELXL Sheldrick, George M. Acta Crystallographica Section C Structural Chemistry, Vol. 71, Issue 1, p. 3-8 https://doi.org/10.1107/S2053229614024218	journal	January 2015
Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon Upham, D. Chester; Agarwal, Vishal; Khechfe, Alexander Science, Vol. 358, Issue 6365 https://doi.org/10.1126/science.aao5023	journal	November 2017
Metallic Hydrides I: Hydrogen Storage and Other Gas-Phase Applications Bowman, Robert C.; Fultz, Brent MRS Bulletin, Vol. 27, Issue 9 https://doi.org/10.1557/mrs2002.223	journal	September 2002
Hydrogenation Properties of LnAl2 (Ln = La, Eu, Yb), LaGa2, LaSi2 and the Crystal Structure of LaGa2H0.71(2) Werwein, Anton; Benndorf, Christopher; Bertmer, Marko Crystals, Vol. 9, Issue 4 https://doi.org/10.3390/cryst9040193	journal	April 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Flux Synthesis of a Metal Carbide Hydride Using Anthracene As a Reactant

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