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Improved high-performance La0.7Sr0.3MxFe1-xO3 (M = Cu, Cr, Ni) perovskite catalysts for ortho-para hydrogen spin conversion

  • Choi, Jeong-Gil (Department of Chemical Engineering and Advances Materials, Hannam University) ;
  • Choi, Euiji (Applied Chemistry, Department of Materials Science and Engineering, Kyushu University) ;
  • Kweon, Soon-Cheol (Green City Technology Institute, Korea Institute of Science and Technology) ;
  • Oh, In-Hwan (Green City Technology Institute, Korea Institute of Science and Technology)
  • Received : 2017.12.04
  • Accepted : 2017.12.28
  • Published : 2018.02.28

Abstract

The improved high-performance Fe-based perovskite-type oxides ($La_{0.7}Sr_{0.3}M_xFe_{1-x}O_3$, M = Cu, Cr, Ni) were synthesized by a citrate method and characterized by SEM, EDS, XRD and NMR spectroscopy analyses. The characterization analyses revealed that the stoichiometric amounts of lattice oxygen were existed in all of perovskite samples except for a nickel-doped perovskite. Fe-based perovskites exhibited a surprising result for ortho-para $H_2$ spin conversion reaction, indicating two orders of magnitude higher conversions and conversion rates than commercial $Fe_2O_3$. It was considered that this conversion difference might be attributed to the presence of oxygen vacancies in Fe-based perovskites prepared in this study.

Keywords

References

  1. J. Zhang, T.S. Fisher, P.V. Ramachandran, J.P. Gore and I. Mudawar, "A review of heat transfer issues in hydrogen storage technologies", J. Heat Transfer. 127 (2005) 1391.
  2. K. Makoshi, M. Rami and E. Ilisca, "Dipolar and contact processes in $H_2$ o-p conversion on ionic surfaces", J. Physics: Condensed Matter. 5 (1993) 7325.
  3. M. Rami, K. Makoshi and E. Illisca, "Physisorption and ortho-para conversion of molecular hydrogen on solid surfaces", Appl. Surf. Sci. 68 (1993) 197.
  4. S.K. Dickinson Jr., "The chemical structure of solids", AF CRL-70-0727, National Technical Information Center (1970).
  5. B. Michael and S. McIntosh, "Kinetics of ortho-para conversion of hydrogen", J. Catal. 255 (2008) 313.
  6. F. Dhainaut, S. Pietrzyk and P. Granger, "Kinetic investigation of the NO reduction by $H_2$ over noble metal based catalysts", Catal. Today 119 (2007) 94.
  7. S.Q. Chen and Y. Liu, "$LaFe_yNi_{1-y}O_3$ supported nickel catalysts used for steam reforming of ethanol", Int'l. J. of Hydrogen Energy 34 (2009) 4735.
  8. M.M. Natile, F. Poletto, A. Galenda, A. Glisenti, T. Montini, L. De Rogatis and P. Fornasiero, "$La_2Cu_{0.8}Co_{0.2}O_{4+}$ by Pechini method", Chem. Mat'ls 20 (2008) 2314.
  9. E. Arendt, A. Maione, A. Klisnska, O. Sanz, M. Montes, S. Suarez, J. Blanco and P. Ruiz, "High-efficiency $CeWO_x$ catalyst for the selective catalytic reduction of $NO_x$ with $NH_3$", Appl. Catal. A: General 339 (2008) 1.
  10. D.H. Prasad, S.Y. Park, E.O. Oh, H. Ji, H.R. Kim, K.J. Yoon, J.W. Son and J.H. Lee, "Synthesis of nano-crystalline $La_{1-x}Sr_xCoO_{3-{\delta}}$ perovskite oxides by EDTA-citrate complexing process and its catalytic activity for soot oxidation", Appl. Catal. A; General 447 (2012) 100.
  11. C.H. Kim, G. Qi, K. Dahlberg and W. Li, "Strontiumdoped perovskites rival platinum catalysts for treating $NO_x$ in simulated diesel exhaust", Science 327 (2010) 1624.
  12. J. Suntivich, K.J. May, H.A. Gasteiger, J.B. Goodenough and Y. Shao-Horn, "A perovskite oxide optimized for oxygen evolution catalysis from molecular orbital principles", Science 334 (2011) 1383.
  13. J. Faye, A. Baylet, M. Trentesaux, S. Royer, F. Dumeignil, D. Duprez, S. Valange and J.M. Tatibouet, "Influence of lanthanum stoichiometry in $La_{1-x}FeO_{3-{\delta}}$ perovskites on their structure and catalytic performance in $CH_4$ total oxidation", Applied Catalysis B: Environment 126 (2012) 134.
  14. A. Gamliel, H. Allouche-Arnon, R. Nalbandian, C.M. Barzily, J.M. Gomori and R. Katz-Brull, "An apparatus for production of isotopically and spin-enriched hydrogen for induced polarization studies", Appl. Magnet. Reson. 39 (2010) 329.
  15. E. Sartori, M, Ruzzi, R.G. Lawler and N.J. Turro, "Demonstration of a chemical transformation inside a fullerene. The reversible conversion of the allotropes of $H_2@C_{60}$", JACS 130 (2008) 12752.
  16. J.G. Vitillo, L. Regli, S. Chavan, G. Ricchiardi, G. Spoto, P.D.C. Dietzel, S. Bordiga and A. Zecchina, "Role of exposed metal sites in hydrogen storage in MOFs", JACS 130 (2008) 8386.
  17. E. Baron and P.W. Selwood, "Parahydrogen conversion and magnetocatalytic effects over yttria and lutetia", J. Catal. 28 (1973) 422.
  18. C.F. Ng and P.W. Selwood, "Magnetic effects on the ortho-para hydrogen conversion over ${\alpha}-Cr_2O_3$, CoO, and MnO", J. Catal. 43 (1976) 252.
  19. J.G. Choi, R.L. Curl and L.T. Thompson, "Molybdenum nitride catalysts: I. Influence of the synthesis factors on structural properties", J. Catal. 146 (1994) 218.
  20. G.A. Somorjai and J. Carrazza, "Structure sensitivity of catalytic reactions", Ind. Eng. Chem. Fund. 25 (1986) 63.
  21. M. Boudart, "Catalysis by supported metals", Princeton Univ. Press 1992: chap. 5.
  22. J.G. Choi, J.R. Brenner, C.W. Colling, K. Demczy, J.L. Dunning and L.T. Thompson, "Synthesis and characterization of molybdenum nitride hydrodenitrogenation catalysts", Catal. Today 15 (1992) 201.
  23. J.G. Choi, J.R. Brenner and L.T. Thompson. "Pyridine hydrodenitrogenation over molybdenum carbide catalysts", J. Catal. 154 (1995) 33.