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Chapman, Stephanie; Brookes, Catherine; Bowker, Michael; Gibson, Emma K.; Wells, Peter P. (2016)
Publisher: Royal Society of Chemistry
Languages: English
Types: Article
Subjects: QD
The performance of Mo-enriched, bulk ferric molybdate, employed commercially for the industrially important reaction of the selective oxidation of methanol to formaldehyde, is limited by a low surface area, typically 5-8 m(2) g(-1). Recent advances in the understanding of the iron molybdate catalyst have focused on the study of MoOx@Fe2O3 (MoOx shell, Fe2O3 core) systems, where only a few overlayers of Mo are present on the surface. This method of preparing MoOx@Fe2O3 catalysts was shown to support an iron molybdate surface of higher surface area than the industrially-favoured bulk phase. In this research, a MoOx@Fe2O3 catalyst of even higher surface area was stabilised by modifying a haematite support containing 5 wt% Al dopant. The addition of Al was an important factor for stabilising the haematite surface area and resulted in an iron molybdate surface area of ?35 m(2) g(-1), around a 5 fold increase on the bulk catalyst. XPS confirmed Mo surface-enrichment, whilst Mo XANES resolved an amorphous MoOx surface monolayer supported on a sublayer of Fe2(MoO4)3 that became increasingly extensive with initial Mo surface loading. The high surface area MoOx@Fe2O3 catalyst proved amenable to bulk characterisation techniques; contributions from Fe2(MoO4)3 were detectable by Raman, XAFS, ATR-IR and XRD spectroscopies. The temperature-programmed pulsed flow reaction of methanol showed that this novel, high surface area catalyst (3ML-HSA) outperformed the undoped analogue (3ML-ISA), and a peak yield of 94% formaldehyde was obtained at ?40 °C below that for the bulk Fe2(MoO4)3 phase. This work demonstrates how core-shell, multi-component oxides offer new routes for improving catalytic performance and understanding catalytic activity.
  • The results below are discovered through our pilot algorithms. Let us know how we are doing!

    • 1 W. J. Linn and A. W. Sleight, J. Catal., 1976, 41, 134-139.
    • 2 J. L. Callahan, R. K. Grasselli, E. C. Milberger and H. A. Strecker, Ind. Eng. Chem. Prod. Res. Dev., 1970, 9, 134-142.
    • 3 S. Kowatsch, Formaldehyde, Springer, Berlin Heidelberg, 2010.
    • 4 G. W. Keulks, J. Catal., 1970, 19, 232-235.
    • 5 U. Chowdhry, A. Ferretti, L. E. Firment, C. J. Machiels, F. Ohuchi, A. W. Sleight and R. H. Staley, Appl. Surf. Sci., 1984, 19, 360-372.
    • 6 M. Bowker, R. Holroyd, A. Elliott, P. Morrall, A. Alouche, C. Entwistle and A. Toerncrona, Catal. Lett., 2002, 83, 165-176.
    • 7 M. Bowker, C. Brookes, A. F. Carley, M. P. House, M. Kosif, G. Sankar, I. Wawata, P. P. Wells and P. Yaseneva, Phys. Chem. Chem. Phys., 2013, 15, 12056-12067.
    • 8 C. Brookes, P. P. Wells, G. Cibin, N. Dimitratos, W. Jones, D. J. Morgan and M. Bowker, ACS Catal., 2014, 4, 243-250.
    • 9 C. Brookes, P. P. Wells, N. Dimitratos, W. Jones, E. K. Gibson, D. J. Morgan, G. Cibin, C. Nicklin, D. Mora-Fonz, D. O. Scanlon, C. R. A. Catlow and M. Bowker, J. Phys. Chem. C, 2014, 26155-26161.
    • 10 Y. Huang, L. Cong, J. Yu, P. Eloy and P. Ruiz, J. Mol. Catal. A: Chem., 2009, 302, 48-53.
    • 11 K. Routray, W. Zhou, C. J. Kiely, W. Gru¨nert and I. E. Wachs, J. Catal., 2010, 275, 84-98.
    • 12 M. R. Sun-Kou, S. Mendioroz, J. L. G. Fierro, J. M. Palacios and A. GuerreroRuiz, J. Mater. Sci., 1995, 30, 496-503.
    • 13 Y. Matsuoka, M. Niwa and Y. Murakami, J. Phys. Chem., 1990, 94, 1477-1482.
    • 14 C. J. Machiels, W. H. Cheng, U. Chowdhry, W. E. Farneth, F. Hong, E. M. Mc Carron and A. W. Sleight, Appl. Catal., 1986, 25, 249-256.
    • 15 C. Brookes, M. Bowker, E. K. Gibson, D. Gianolio, K. M. H. Mohammed, S. Parry, S. M. Rogers, I. P. Silverwood and P. P. Wells, Catal. Sci. Technol., 2016, 722-730.
    • 16 Y. Zheng, Y. Cheng, Y. Wang, F. Bao, L. Zhou, X. Wei, Y. Zhang and Q. Zheng, J. Phys. Chem. B, 2006, 110, 3093-3097.
    • 17 K. Sivula, F. le Formal and M. Gr¨atzel, ChemSusChem, 2011, 4, 432-449.
    • 18 A. Khelfa, V. Sharypov, G. Finqueneisel and J. V. Weber, J. Anal. Appl. Pyrolysis, 2009, 84, 84-88.
    • 19 G. Picasso Escobar, A. Quintilla Beroy, M. P. Pina Iritia and J. Herguido Huerta, Chem. Eng. J., 2004, 102, 107-117.
    • 20 R. M. Cornell and U. Schwertmann, The Iron Oxides: Structure, Properties, Reactions, Occurrences and Uses, Wiley, 2006.
    • 21 M. Hermanek, R. Zboril, I. Medrik, J. Pechousek and C. Gregor, J. Am. Chem. Soc., 2007, 129, 10929-10936.
    • 22 U. Schwertmann, R. Fitzpatrick, R. Taylor and D. Lewis, Clays Clay Miner., 1979, 27, 105-112.
    • 23 A. Zoppi, C. Lofrumento, E. M. Castellucci and P. Sciau, J. Raman Spectrosc., 2008, 39, 40-46.
    • 24 U. Schwertmann and R. M. Cornell, Iron Oxides in the Laboratory, Wiley, 2008.
    • 25 M. P. House, A. F. Carley, R. Echeverria-Valda and M. Bowker, J. Phys. Chem. C, 2008, 112, 4333-4341.
    • 26 R. Li, Q. Li, S. Gao and J. K. Shang, J. Am. Ceram. Soc., 2011, 94, 584-591.
    • 27 M. Wells, R. Gilkes and R. Anand, Clay Miner., 1989, 24, 513-530.
    • 28 R. Shannon, Acta Crystallogr., Sect. A: Cryst. Phys., Diffr., Theor. Gen. Crystallogr., 1976, 32, 751-767.
    • 29 L. Truffault, B. Choquenet, K. Konstantinov, T. Devers, C. Couteau and L. J. M. Coiffard, J. Nanosci. Nanotechnol., 2011, 11, 2413-2420.
    • 30 H. Liu, T. Chen, X. Zou, C. Qing and R. L. Frost, J. Raman Spectrosc., 2013, 44, 1609-1614.
    • 31 D. L. A. de Faria, S. Venˆancio Silva and M. T. de Oliveira, J. Raman Spectrosc., 1997, 28, 873-878.
    • 32 M. Hanesch, Geophys. J. Int., 2009, 177, 941-948.
    • 33 P. A. Redhead, Vacuum, 1962, 12, 203-211.
    • 34 R. L. Blake, R. E. Hessevic, T. Zoltai and L. W. Finger, Am. Mineral., 1966, 51, 123.
    • 35 A. P. V. Soares, M. F. Portela and A. Kiennemann, Catal. Rev.: Sci. Eng., 2005, 47, 125-174.
    • 36 M. P. House, M. D. Shannon and M. Bowker, Catal. Lett., 2008, 122, 210-213.
    • 37 W. McMaster, N. K. Del Grande, J. Mallett and J. Hubbell, International Tables for Crystallography, Mathematical, Physical and Chemical Tables, Compilation of X-Ray cross sections, Section III, Springer Science & Business Media, 1969.
    • 38 A. M. Beale, S. D. M. Jacques, E. Sacaliuc-Parvalescu, M. G. O'Brien, P. Barnes and B. M. Weckhuysen, Appl. Catal., A, 2009, 363, 143-152.
    • 39 A. M. Turek, I. E. Wachs and E. DeCanio, J. Phys. Chem., 1992, 96, 5000-5007.
    • 40 L. J. Burcham, L. E. Briand and I. E. Wachs, Langmuir, 2001, 17, 6164-6174.
    • 41 G. Busca, Catal. Today, 1996, 27, 457-496.
    • 42 L. J. Burcham, L. E. Briand and I. E. Wachs, Langmuir, 2001, 17, 6175-6184.
    • 43 M. P. House, Selective oxidation of methanol over iron molybdate catalysts, PhD Thesis, Cardiff University, 2007.
    • 44 K. Manseri, H. Hentit, E. H. Elandaloussi, B. Benaichouba and M. S. Ouali, Hyperne Interact., 2010, 198, 243-257.
    • 45 B. Benaichouba, P. Bussiere and J. C. Vedrine, Appl. Catal., A, 1995, 130, 31-45.
    • 46 A. S. Chellappa and D. S. Viswanath, Ind. Eng. Chem. Res., 1995, 34, 1933-1940.
    • 47 K. L. Madhok and K. P. Srivastava, Proc. - Indian Acad. Sci., Chem. Sci., 1981, 90, 527-535.
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