Can a Single Atom Serve as the Active Site in Some Heterogeneous Catalysts?

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• 作者：John Meurig Thomas (1)
  Zineb Saghi (1)
  Pratibha L. Gai (2)
  
• 关键词：Single Pt atoms ; Single ion catalysts ; CeO2 supports ; Single ; site heterogeneous catalysts ; Bimetallic nanocluster catalysts ; Oxyfunctionalization of alkanes
• 刊名：Topics in Catalysis
• 出版年：2011
• 出版时间：July 2011
• 年：2011
• 卷：54
• 期：10-12
• 页码：588-594
• 全文大小：696KB
• 参考文献：1. Thomas JM, Ducati C (2011) In: Che M, Vedrine JC (eds) Characterization of solid catalysts. Wiley––VCH, Weinheim
  2. Rim RT, Eom D, Liu L, Stolyarova E, Raitano JM, Chan S-W, Flytzani-Stephanopoulos M, Flynn GW (2009) J Phys Chem C 113:10198 CrossRef
  3. Fu Q, Saltsburg H, Flytzani-Stephanopoulous M (2003) Science 301:935 CrossRef
  4. Haruta M (1997) Catal Today 36:153 CrossRef
  5. Fierro-Gonzalez JC, Bhirud VA, Gates BC (2005) Chem Commun 42:5275 CrossRef
  6. Liu Z-P, Jenkins SJ, King DA (2005) Phys Rev Lett 94:196102 CrossRef
  7. Guzman J, Gates BC (2003) Angew Chem Int Ed 42:690 CrossRef
  8. Zhang X, Shi H, Xu B-Q (2005) Angew Chem Int Ed 44:7132 CrossRef
  9. Gai PL, Boyes ED (2009) Microsc Res Tech 72:153 CrossRef
  10. Zewail AH, Thomas JM (2010) 4D electron microscopy: imaging in space and time. Imperial College Press, London
  11. Thomas JM, Raja R, Lewis DW (2005) Angew Chem Int Ed 44:6456 CrossRef
  12. Thomas JM (2008) J Chem Phys 128:182502 CrossRef
  13. Wright PA (2008) Microporous framework solids. RSC Publishing, Cambridge
  14. Thomas JM, Raja R (2006) Top Catal 40:3 CrossRef
  15. Thomas JM, Raja R, Sankar G, Bell RG (1999) Nature 398:227 CrossRef
  16. Dugal M, Sankar G, Raja R, Thomas JM (2000) Angew Chem Int Ed 39:2310 CrossRef
  17. Raja R, Sankar G, Thomas JM (2000) Angew Chem Int Ed 39:2313 CrossRef
  18. Thomas JM, Raja R, Sankar G, Bell RG (2001) Acc Chem Res 34:191 CrossRef
  19. Cheetham AK, Eddy MM, Thomas JM (1984) J Chem Soc Chem Comm 20:1337 CrossRef
  20. Gomez-Hortiguela L, Cora F, Sankar G, Zicovich-Wilson C, Catlow CRA (2010) Chem Eur J 16:13618
  21. Ruddy DA, Tilley TD (2008) J Am Chem Soc 130:11088 CrossRef
  22. Abramo GP, Li L, Marks TJ (2002) J Am Chem Soc 124:13966 CrossRef
  23. Thomas JM, Catlow CRA, Sankar G (2002) Chem Commun 2921
  24. Dal Santo V, Liguori F, Pirovano C, Guidotti M (2010) Molecules 15:3829 CrossRef
  25. Argo AM, Odzak JF, Lai FS, Gates BC (2002) Nature 415:623 CrossRef
  26. Thomas JM, Adams RD, Boswell EM, Captain B, Gronbeck H, Raja R (2008) Faraday Disc 138:301 CrossRef
  27. Thomas JM, Raja R, Gai PL, Gronbeck H, Hernandez-Garrido JC (2010) Chem Cat Chem 2:402
  28. Haruta M, Yamada N, Kobayashi T, Iijima S (1989) J Catal 115:301 CrossRef
  29. Bond GC, Thompson DT (1999) Catal Rev–Sci Eng 41:319 CrossRef
  30. Hutchings GJ, Hall MS, Carley AF, Landon P, Solsona BE, Kiely CJ, Herzing A, Makkee M, Moulijn JA, Overweg A, Fierro-Gonzalez JC, Guzman J, Gates BC (2006) J Catal 242:71 CrossRef
  31. Bamwenda GR, Tsubota S, Nakamura T, Haruta M (1997) Catal Lett 44:83 CrossRef
  32. Valden M, Lai X, Goodman DW (1998) Science 281:1647 CrossRef
  33. Schwartz V, Mullins DR, Yan W, Chen B, Dai S, Overbury SH (2004) J Phys Chem B 108:15782 CrossRef
  34. Date M, Okumura M, Tsubota S, Haruta M (2004) Angew Chem Int Ed 43:2129 CrossRef
  35. Carrettin S, Concepción P, Corma A, Nieto JML, Puntes VF (2004) Angew Chem Int Ed 43:2538 CrossRef
  36. Deng W, Frenkel AI, Si R, Flytzani-Stephanopoulos M (2008) J Phys Chem C 112:12834 CrossRef
  37. Deng W, Carpenter C, Yi N, Flytzani-Stephanopoulos M (2007) Top Catal 44:199 CrossRef
  38. Chen MS, Goodman DW (2006) Catal Today 111:22 CrossRef
  39. Meyer R, Lemire C, Shaikhutdinov SK, Freund HJ (2004) Gold Bull 37:72 CrossRef
  40. Shaikhutdinov SK, Meyer R, Naschitzki M, Baumer M, Freund HJ (2003) Catal Lett 86:211 CrossRef
  41. Giordano L, Pacchioni G, Goniakowski J, Nilius N, Rienks EDL, Freund HJ (2008) Phys Rev Lett 101:026102 CrossRef
  42. Fierro-Gonzalez JC, Gates BC (2004) J Phys Chem B 108:16999 CrossRef
  43. Hendricksen BLM, Bobaru SC, Frenken JWM (2004) Surf Sci 552:229 CrossRef
  44. Kwak JH, Hu J, Mei D, Yi C-W, Kim DH, Peden CHF, Allard LF, Szanyi J (2009) Science 325:1670 CrossRef
  45. Vaarkamp M, Miller JT, Modica FS, Koningsberger DC (1996) J Catal 163:294 CrossRef
  46. Yu R, Song H, Zhang X, Yang P (2005) J Phys Chem B 109:6940 CrossRef
  47. Thomas JM, Johnson BFG, Raja R, Sankar G, Midgley PA (2003) Acc Chem Res 36:20 CrossRef
  48. Uzun A, Gates BC (2008) Angew Chem Int Ed 47:9245 CrossRef
  49. Uzun A, Gates BC (2009) J Am Chem Soc 131:15887 CrossRef
  50. M?bus G, Saghi Z, Sayle D, Sayle TXT (2010) Adv Mater (in press)
  51. Aguilar-Guerro V, Gates BC (2008) J Catal 269:351 CrossRef
  52. Maschmeyer T, Rey F, Sankar G, Thomas JM (1995) Nature 378:159 CrossRef
  53. Zhai Y, Pierre D, Si R, Deng W, Ferrin P, Nilekar AU, Peng G, Herron JA, Bell DC, Saltsburg H, Mavrikakis M, Flytzani-Stephanopoulos M (2010) Science 329:1633 CrossRef
  54. Kwon O-H, Zewail AH (2010) Science 328:1668 CrossRef
  55. Thomas JM (2011) Angew Chem Int Ed 50:49
  
• 作者单位：John Meurig Thomas (1)
  Zineb Saghi (1)
  Pratibha L. Gai (2)
  
  1. Department of Materials Science and Metallurgy, University of Cambridge, Pembroke Street, Cambridge, CB2 3QZ, UK
  2. York JEOL Nanocentre, Helix House, University of York, Heslington, York, YO10 5DD, UK
  
• ISSN：1572-9028

文摘

We examine a number of distinct situations relating to heterogeneous catalysts where either a single atom (or ion), or a very small cluster of atoms functions as the locus of chemical turnover in various distinct kinds of conversion. There is little doubt that individual ions at certain crystallographic sites in nanoporous solids can indeed act as single-site catalysts. The situation concerning nanoclusters of pure metal (or bimetallic entities) is rather more ambiguous. What was hitherto thought to be an effective catalyst made up of a small cluster of Pt supported on γ-Al2O3 (for hydrogenation) now seems to be a single atom of Pt attached to a 5-coordinated AlIII ion. And in the case of Au or Pt on other supports, there is evidence that a single Pt atom, positively charged, but surrounded by alkali-metal ions, is a powerful catalyst for the water–gas shift (CO?+?H2O?→?H2?+?CO2) reaction. We also report interesting results concerning the mobility of CeO2 support material.