Synthesis and characterization of gold-containing oxides of K2NiF4 or Nd2CuO4 structure type
Abstract
In this work, different materials of Nd2CuO4 and K2NiF4 Ruddlesden-Popper structure have been prepared by solid-state reaction in air and high temperatures. The powders of mixed oxides, of general formula La2Li0.5M0.5 − xAu x O4 (M = Cu, Ni), were prepared from [Au(NH3)4](NO3)3 as gold source. The stoichiometric proportions of the all reagents (including La2O3, NiCO3, CuO) were grounded with a LiOH excess as mineralizer, pressed to form into pellets and heated in static air at temperatures between 750 and 850 °C for several hours. Structural characterization of the synthesized oxides using X-ray diffraction (XRD) are presented. La2Li0.5Au0.5O4, La2Li0.5Cu0.5O4, and La2Li0.5Ni0.5O4, three previously known oxides, were obtained. As expected, La2Li0.5Ni0.5O4 and La2Li0.5Cu0.5O4 consist of an ordered K2NiF4 Ruddlesden-Popper structure, while the La2Li0.5Au0.5O4 compound exhibits a Nd2CuO4 type structure. On the other hand, the preparation of the new proposed group La2Li0.5M0.5 − xAuxO4 (x = 0.0125–0.5) containing gold and nickel/copper simultaneously, under the studied conditions, was not possible. The experimental results revealed that the host structures are intolerant with respect to M (Cu or Ni) and Au cation double substitution. The difficulty to obtain the new phases is discussed regarding the exceptional instability displayed by the trivalent state of gold ion (Au3+) and the soft interactions of this specie with the lithium cation. Finally, the monophasic oxides, more interesting in terms of catalytic activity, were analyzed by temperature-programmed reduction (TPR-H2).
Keywords
Mixed oxide Gold SynthesisNotes
Acknowledgements
The authors are grateful to UIS’ Microscopy and Xray Laboratory (Parque Tecnológico Guatiguará) for the technical support. The Universidad Industrial de Santander is also acknowledged for supporting and funding this work (internal project VIE 5195 and movilidad program 2018).
References
- 1.Haruta M, Kobayashi T, Sano H, Yamada N (1987) Novel gold catalysts for the oxidation of carbon monoxide at a temperature far below 0 °C. Chem Lett 405:405–408CrossRefGoogle Scholar
- 2.Haruta M (2004) Gold as a novel catalyst in the 21st century: preparation, working mechanism and applications. Gold Bull 37:27–36CrossRefGoogle Scholar
- 3.Hashmi ASK, Hutchings GJ (2006) Gold catalysis. Angew Chem Int Ed 45:7896–7936CrossRefGoogle Scholar
- 4.Prati L, Villa A (2012) The art of manufacturing gold catalysts. Catalysts 2:24–37CrossRefGoogle Scholar
- 5.Hashmi ASK (2000) New and selective transition metal catalyzed reactions of allenes. Angew Chem Int Ed 39:2285–2288CrossRefGoogle Scholar
- 6.Hashmi ASK (2000) Highly selective gold-catalyzed arene synthesis. J Am Chem Soc 122:11553–11554CrossRefGoogle Scholar
- 7.Hashmi ASK (2007) Gold-catalyzed organic reactions. Chem Rev 107:3180–3211CrossRefGoogle Scholar
- 8.Pflästerer D, Hashmi ASK (2016) Gold catalysis in total synthesis—recent achievements. Chem Soc Rev 45:1331–1367CrossRefGoogle Scholar
- 9.Cotton SA (1997) Silver and gold. In: Chemistry of precious metals, 1st edn. Chapman & Hall, London, pp 273–283CrossRefGoogle Scholar
- 10.Shi H, Asahi R, Stampf C (2007) Properties of the gold oxides Au2O3 and Au2O: first-principles investigation. Phys Rev B 75:205125CrossRefGoogle Scholar
- 11.Kurzman JA, Ouyang X, Im WB, Li J, Hu J, Scott SL, Seshadri R (2010) La4LiAuO8 and La2BaPdO5: comparing two highly stable d 8 square-planar oxides. Inorg Chem 49:4670–4680CrossRefGoogle Scholar
- 12.Etourneau J, Portier J (1992) The role of the inductive effect in solid state chemistry: how the chemist can use it to modify both the structural and the physical properties of the materials. J Alloys Compd 188:1–7CrossRefGoogle Scholar
- 13.Abbattista F, Vallino M, Mazza D (1985) Preparation and crystallographic characteristics of the new phase La2Au0.5Li0.5O4. J Less-Common Met 110:391–396CrossRefGoogle Scholar
- 14.Warda SA, Pietzuch W, Berghöfer G, Kesper U, Massa W, Reinen DZ (1998) Ordered K2NiF4 structure of the solids La2Li1/2M1/2O4 (M(III) = Co, Ni, Cu) and the bonding properties of the MO6 polyhedra in various compounds of this type. J Solid State Chem 138:18–31CrossRefGoogle Scholar
- 15.Thalinger R, Gocyla M, Heggen M, Dunin-Borkowski R, Grünbacher M, Stöger-Pollach M, Schmidmair D, Klötzer B, Penner S (2016) Ni–perovskite interaction and its structural and catalytic consequences in methane steam reforming and methanation reactions. J Catal 337:26–35CrossRefGoogle Scholar
- 16.Corma A, García H (2008) Supported gold nanoparticles as catalysts for organic reactions. Chem Soc Rev 37:2096–2126CrossRefGoogle Scholar
- 17.Zhang Y, Cui X, Shi F, Deng Y (2012) Nano-gold catalysis in fine chemical synthesis. Chem Rev 112(4):2467–2505CrossRefGoogle Scholar
- 18.Wang H, Fan W, He Y, Wang J, Kondo JN, Tatsumi T (2013) Selective oxidation of alcohols to aldehydes/ketones over copper oxide-supported gold catalysts. J Catal 299:10–19CrossRefGoogle Scholar
- 19.Skibsted LH, Bjerrum J (1974) Studies on gold complexes. I. Robustness, stability and acid dissociation of tetramminegold(III) ion. Acta Chem Scand A28:740–746CrossRefGoogle Scholar
- 20.Rodríguez-Carvajal J (1993) Recent advances in magnetic structure determination by neutron powder diffraction. Phys B Condens Matter 192-1:55–69CrossRefGoogle Scholar
- 21.Rodríguez-Carvajal J (2001) Recent developments of the program FullProf. Commission on powder diffraction (IUCr). Newsletter 26:12–19Google Scholar
- 22.Steinhauser G, Evers J, Jakob S, Klapötke TM, Oehlinger G (2008) A review on fulminating gold (Knallgold). Gold Bull 41(4):305–317CrossRefGoogle Scholar
- 23.Manfait M, Alix AJP, Kappenstein C (1981) Raman and infrared studies of the square planar tetrammine gold(III) and its deuterate. Inorg Chim Acta 50:147–152CrossRefGoogle Scholar
- 24.Weishaupt M, Strähle J (1976) Crystal structure and vibrational spectrum of tetraamminegold- (III)-nitrate. Z Naturforsch 31:554–558CrossRefGoogle Scholar
- 25.Li GB, Yang JQ, Fan YX, Tian SJ, Zheng CG (1998) Phase equilibria of the system La2O3-NiO-Li2O at 700, 800, and 900 °C. J Solid State Chem 141-2:457–461CrossRefGoogle Scholar
- 26.Demazeau G, Parent C, Pouchard M, Hagenmuller P (1972) Sur deux nouvelles phases oxygenées du cuivre trivalent: LaCuO3 et La2Li0.50Cu0.50O4. Mater Res Bull 7(9):913–920CrossRefGoogle Scholar
- 27.Pietzuch W, Warda SA, Massa W, Reinen D (2000) Die Kristallstruktur von La2Li1/2Au1/2O4 und bindungschemische aspekte. Z Anorg Allg Chem 626:113–117CrossRefGoogle Scholar
- 28.Laguna A (2008) Modern supramolecular gold chemistry: gold-metal interactions and applications. Jhon Wiley-& Sons, New York, pp 41–48CrossRefGoogle Scholar
- 29.Hu Z, Kaindl G, Warda SA, Reinen D, de Groot FMF, Müller BG (1998) On the electronic structure of Cu(III) and Ni(III) in La2Li1/2Cu1/2O4, Nd2Li1/2Ni1/2O4, and Cs2KCuF6. Chem Phys 232:63–74CrossRefGoogle Scholar
- 30.Haines RI, McAuley A (1981) Synthesis and reactions of nickel(III) complexes. Coord Chem Rev 39:77–119CrossRefGoogle Scholar
- 31.Guo C, Zhang J, Zhang X (2008) Comparative study of LaNiO3 and La2NiO4 catalysts for partial oxidation of methane. React Kinet Catal Lett 95:89–97CrossRefGoogle Scholar
- 32.Kurzman JA, Moffitt SL, Llobet A, Seshadri R (2011) Neutron diffraction study of La4LiAuO8: understanding Au3+ in an oxide environment. J Solid State Chem 184(6):1439–1444CrossRefGoogle Scholar