Selective Propene Epoxidation on Immobilized Au6–10 Clusters: The Effect of Hydrogen and Water on Activity and Selectivity†
Sungsik Lee Dr.
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorLuis M. Molina Dr.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorMaría J. López Prof.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorJulio A. Alonso Prof.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorBjørk Hammer Prof.
iNano and Department of Physics and Astronomy, University of Aarhus, Ny Munkegade, 8000 Aarhus C (Denmark)
Search for more papers by this authorByeongdu Lee Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorSönke Seifert Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorRandall E. Winans Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorJeffrey W. Elam Dr.
Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorMichael J. Pellin Dr.
Materials Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorStefan Vajda Dr.
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Department of Chemical Engineering, School of Engineering & Applied Sciences, Yale University, 9 Hillhouse Avenue, New Haven, CT 06520 (USA)
Search for more papers by this authorSungsik Lee Dr.
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorLuis M. Molina Dr.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorMaría J. López Prof.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorJulio A. Alonso Prof.
Departamento de Física Teórica, Atómica y Óptica, Universidad de Valladolid, 47011 Valladolid (Spain), Fax: (+34) 983-423-013
Search for more papers by this authorBjørk Hammer Prof.
iNano and Department of Physics and Astronomy, University of Aarhus, Ny Munkegade, 8000 Aarhus C (Denmark)
Search for more papers by this authorByeongdu Lee Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorSönke Seifert Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorRandall E. Winans Dr.
X-ray Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorJeffrey W. Elam Dr.
Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorMichael J. Pellin Dr.
Materials Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Search for more papers by this authorStefan Vajda Dr.
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (USA)
Department of Chemical Engineering, School of Engineering & Applied Sciences, Yale University, 9 Hillhouse Avenue, New Haven, CT 06520 (USA)
Search for more papers by this authorWork supported by Spanish MEC (MAT2005-06544-C03-01) and JCyL (VA017A08) grants. L.M.M. acknowledges support from the “Ramon y Cajal” program. The work at Argonne National Laboratory was supported by the US Department of Energy, BES-Chemical Sciences, BES-Materials Sciences, and BES-Scientific User Facilities under Contract DE-AC-02-06CH11357 with UChicago Argonne, LLC, Operator of Argonne National Laboratory. S.V. gratefully acknowledges the support by the Air Force Office of Scientific Research. B.H. acknowledges financial support from the Danish research councils, FNU, DSF/NABIIT, and DCSC.
Abstract
Epoxidieren leicht gemacht: Subnanometergroße Goldcluster auf amorphem Aluminiumoxid sind ein hoch aktiver und selektiver Katalysator für die Epoxidierung von Propen. Am höchsten ist die Selektivität bei Gasmischungen, die Sauerstoff und Wasser enthalten, sodass der Einsatz von Wasserstoff vermieden werden kann. Ab-initio-Dichtefunktionalrechnungen lieferten Informationen über Schlüsselintermediate und Reaktionswege. Demnach beruht die Aktivität des Katalysators auf der Bildung von Propenoxid-Metallacyclen. Al grün, Au gelb, O rot, C grau.
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References
- 1T. A. Nijhuis, M. Makkee, J. A. Mouljin, B. M. Weckhuysen, Ind. Eng. Chem. Res. 2006, 45, 3447–3459.
- 2T. Hayashi, K. Tanaka, M. Haruta, J. Catal. 1998, 178, 566–575.
- 3P. Pyykkö, Angew. Chem. 2004, 116, 4512–4557;
10.1002/ange.200300624 Google ScholarAngew. Chem. Int. Ed. 2004, 43, 4412–4456.
- 4M. M. Schubert, S. Hackenberg, A. C. van Veen, M. Muhler, V. Plzak, R. J. Behm, J. Catal. 2001, 197, 113–122.
- 5A. Sanchez, S. Abbet, U. Heiz, W. D. Schneider, H. Häkkinen, R. N. Barnett, U. Landman, J. Phys. Chem. A 1999, 103, 9573–9578; S. Lee, C. Y. Fan, T. P. Wu, S. L. Anderson, J. Am. Chem. Soc. 2004, 126, 5682–5683; G. Pacchioni, S. Sicolo, C. Di Valentin, M. Chiesa, E. Giamello, J. Am. Chem. Soc. 2008, 130, 8690–8695.
- 6J. W. Elam, S. M. George, Chem. Mater. 2003, 15, 1020–1028.
- 7R. E. Winans, S. Vajda, B. Lee, S. J. Riley, S. Seifert, G. Y. Tikhonov, N. A. Tomczyk, J. Chem. Phys. B 2004, 108, 18105–18107; R. E. Winans, S. Vajda, G. E. Ballentine, J. W. Elam, B. Lee, M. J. Pellin, S. Seifert, G. Y. Tikhonov, N. A. Tomczyk, Top. Catal. 2006, 39, 145–149.
- 8O. P. H. Vaughan, G. Kyriakou, N. Macleod, M. Tikhov, R. M. Lambert, J. Catal. 2005, 236, 401–404.
- 9T. A. Nijhuis, T. Visser, B. M. Weckhuysen, Angew. Chem. 2005, 117, 1139–1142;
10.1002/ange.200462043 Google ScholarAngew. Chem. Int. Ed. 2005, 44, 1115–1118.
- 10L. M. Molina, B. Hammer, Appl. Catal. A 2005, 291, 21–31.
- 11S. P. Adiga, P. Zapol, L. A. Curtiss, Phys. Rev. B 2006, 74, 064204; S. P. Adiga, P. Zapol, L. A. Curtiss, J. Phys. Chem. C 2007, 111, 7422–7429.
- 12H. M. Ajo, V. A. Bondzie, C. T. Campbell, Catal. Lett. 2002, 78, 359–368; T. A. Nijhuis, E. Sacaliuc, A. M. Beale, A. M. J. van der Eerden, J. C. Schouten, B. M. Weckhuysen, J. Catal. 2008, 258, 256–264.
- 13M.-L. Bocquet, D. Loffreda, J. Am. Chem. Soc. 2005, 127, 17207–17215; S. Linic, M. A. Barteau, J. Am. Chem. Soc. 2003, 125, 4034–4035; D. Torres, N. López, F. Illas, R. M. Lambert, Angew. Chem. 2007, 119, 2101–2104; Angew. Chem. Int. Ed. 2007, 46, 2055–2058.
- 14A. A. Herzing, C. J. Kiely, A. F. Carley, P. Landon, G. J. Hutchings, Science 2008, 321, 1331–1335; M. Turner, V. B. Golovko, O. P. H. Vaughan, P. Abdulkin, A. Berenguer-Murcia, M. S. Tikhov, B. F. G. Johnson, R. M. Lambert, Nature 2008, 454, 981–983.
- 15L. M. Molina, M. J. López, J. A. Alonso, B. Hammer, unpublished results.
- 16B. C. Gates, Chem. Rev. 1995, 95, 511–522; A. M. Argo, J. F. Odzak, F. S. Lai, B. C. Gates, Nature 2002, 415, 623–626.
- 17S. Vajda, R. E. Winans, J. W. Elam, B. Lee, M. J. Pellin, S. Seifert, G. Y. Tikhonov, N. A. Tomczyk, Top. Catal. 2006, 39, 161–166.
- 18M. C. Payne, M. P. Teter, D. C. Allan, T. A. Arias, J. D. Joannopoulos, Rev. Mod. Phys. 1992, 64, 1045–1097.
- 19D. Vanderbilt, Phys. Rev. B 1990, 41, 7892–7895.
- 20J. P. Perdew, J. A. Chevary, S. H. Vosko, K. A. Jackson, M. R. Pederson, D. J. Singh, C. Fiolhais, Phys. Rev. B 1992, 46, 6671–6687.
- 21A. Alavi, P. Hu. T. Deutsch, P. L. Silvestrelli, J. Hutter, Phys. Rev. Lett. 1998, 80, 3650–3653.
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