Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis

Abstract

The catalysts supported on LiAl₅O₈ (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N₂ adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H₂. Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl₅O₈ (spinel) was formed at 800°C, while LiAl₅O₈ (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO₂, also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl₂-PdCl₂/LiAl₅O₈ (spinel) with better electron transfer ability and low Pd²⁺ reduction temperature exhibited a better catalytic ability.

Key words： Wacker-type catalyst; dimethyl carbonate; methyl nitrite; spinel

References

1 Nuernberg G D B, Fajardo H V, Foletto E L, Hickel-Probst S M, Carreño N L V, Probst L F D, Barrault J. Methane conversion to hydrogen and nanotubes on Pt/Ni catalysts supported over spinel MgAl₂O₄. Catalysis Today, 2011, 176(1): 465–469

2 Widatallah H M, Johnson C, Berry F J, Jartych E, Gismelseed A M, Pekala M, Grabski J. On the synthesis and cation distribution of aluminum-substituted spinel-related lithium ferrite. Materials Letters, 2005, 59(8–9): 1105–1109

3 Valenzuela M A, Jacobs J P, Bosch P, Reijne S, Zapata B, Brongersma H H. The influence of the preparation method on the surface structure of ZnAl₂O₄. Applied Catalysis A, 1997, 148(2): 315–324

4 Grabowska H, Zawadzki M, Syper L. Catalytic method for N-methyl-4-pyridone synthesis in the presence of ZnAl₂O₄. Catalysis Letters, 2007, 121(1–2): 103–110

5 Yamamoto Y, Matsuzaki T, Tanaka S, Nishihira K, Ohdan K, Nakamura A, Okamoto Y. Catalysis and characterization of Pd/NaY for dimethyl carbonate synthesis from methyl nitrite and CO. Journal of the Chemical Society, Faraday Transactions, 1997, 93(20): 3721–3727

6 Anderson S L, Mizushima T, Udagawa Y. Growth/restructuring of palladium clusters induced by carbon monoxide adsorption. Journal of Physical Chemistry, 1991, 95(17): 6603–6610

7 Yamamoto Y, Matsuzaki T, Ohdan K, Okamoto Y. Structure and electronic state of PdCl₂-CuCl₂ catalysts supported on activated carbon. Journal of Catalysis, 1996, 161(2): 577–586

8 Manada N, Murakami M, Yamamoto Y, Kurafuji T. Preparation of dimethyl carbonate in the gas-phase reaction release of Cl-compound from PdCl₂ catalyst and effect of methyl chloroformate. Nippon Kagaku Kaishi, 1994, 1994(11): 985–991

9 Briggs D N, Bong G, Leong E, Oei K, Lestari G, Bell A T. Effects of support composition and pretreatment on the activity and selectivity of carbon-supported PdCu_nCl_x catalysts for the synthesis of diethyl carbonate. Journal of Catalysis, 2010, 276(2): 215–228

10 Jiang R, Wang Y, Zhao X, Wang S, Jin C, Zhang C. Characterization of catalyst in the synthesis of dimethyl carbonate by gas-phase oxidative carbonylation of methanol. Journal of Molecular Catalysis A Chemical, 2002, 185(1–2): 159–166

11 Yamamoto Y. Vapor phase carbonylation reactions using methyl nitrite over Pd catalysts. Catalysis Surveys from Asia, 2010, 14(3–4): 103–110

12 Ohdan K, Matsuzaki T, Hidaka M. US Patent, <patent>5688984-A</patent>, 1996–<month>11</month>–<day>27</day>

13 Curnutt G L. USPatent, <patent>5004827-A</patent>, 1991–04–02

14 Koyama T, Tonosaki M, Yamada N, Mori K. US Patent, <patent>5347031-A</patent>, 1993–<month>02</month>–<day>24</day>

15 Yang P, Cao Y, Dai W L, Deng J F, Fan K N. Effect of chemical treatment of activated carbon as a support for promoted dimethyl carbonate synthesis by vapor phase oxidative carbonylation of methanol over Wacker-type catalysts. Applied Catalysis A, 2003, 243(2): 323–331

16 Briggs D N, Lawrence K H, Bell A T. An investigation of carbon-supported CuCl₂/PdCl₂ catalysts for diethyl carbonate synthesis. Applied Catalysis A, 2009, 366(1): 71–83

17 Jiang R, Wang S, Zhao X, Wang Y, Zhang C. The effects of promoters on catalytic properties and deactivation–regeneration of the catalyst in the synthesis of dimethyl carbonate. Applied Catalysis A, 2003, 238(1): 131–139

18 Kutty T R N, Nayak M. Cationic distribution and its influence on the luminescent properties of Fe³⁺-doped LiAl₅O₈ prepared by wet chemical methods. Journal of Alloys and Compounds, 1998, 269(1–2): 75–87

19 Yang P, Cao Y, Hu J C, Dai W L, Fan K N. Mesoporous bimetallic PdCl₂-CuCl₂ catalysts for dimethyl carbonate synthesis by vapor phase oxidative carbonylation of methanol. Applied Catalysis A, 2003, 241(1–2): 363–373

20 Zhang Z, Ma X, Zhang P, Li Y, Wang S. Effect of treatment temperature on the crystal structure of activated carbon supported CuCl₂-PdCl₂ catalysts in the oxidative carbonylation of ethanol to diethyl carbonate. Journal of Molecular Catalysis A, Chemical, 2007, 266(1–2): 202–206

21 Liu T C, Chang C S. Vapor-phase oxidative carbonylation of ethanol over CuCl-PdCl₂/C catalyst. Applied Catalysis A, 2006, 304: 7277

22 Besenhard J O. Cycling behaviour and corrosion of Li-Al electrodes in organic electrolytes. Journal of Electroanalytical Chemistry, 1978, 94(1): 77–81

23 Hamon Y, Brousse T, Jousse F, Topart P, Buvat P, Schleich D M. Aluminum negative electrode in lithium ion batteries. Journal of Power Sources, 2001, 97–98: 185–187

24 Perentzis G, Horopanitis E E, Papadimitriou L. Effect of multivalent cation substitution on the capacity fading of lithium manganese spinel cathodes. Ionics, 2006, 12(4–5): 269–274

25 Neumair S C, Vanicek S, Kaindl R, Többens D M, Wurst K, Huppertz H. High-pressure synthesis and crystal structure of the lithium borate HP-LiB₃O₅. Journal of Solid State Chemistry, 2011, 184(9): 2490–2497