Display options
Cite
Riss A, Paz AP, Wickenburg S, et al. Imaging single-molecule reaction intermediates stabilized by surface dissipation and entropy. Nat Chem. 2016;8(7):678-83doi: 10.1038/nchem.2506.
Riss, A., Paz, A. P., Wickenburg, S., Tsai, H. Z., De Oteyza, D. G., Bradley, A. J., Ugeda, M. M., Gorman, P., Jung, H. S., Crommie, M. F., Rubio, A., & Fischer, F. R. (2016). Imaging single-molecule reaction intermediates stabilized by surface dissipation and entropy. Nature chemistry, 8(7), 678-83. https://doi.org/10.1038/nchem.2506
Riss, Alexander, et al. "Imaging single-molecule reaction intermediates stabilized by surface dissipation and entropy." Nature chemistry vol. 8,7 (2016): 678-83. doi: https://doi.org/10.1038/nchem.2506
Riss A, Paz AP, Wickenburg S, Tsai HZ, De Oteyza DG, Bradley AJ, Ugeda MM, Gorman P, Jung HS, Crommie MF, Rubio A, Fischer FR. Imaging single-molecule reaction intermediates stabilized by surface dissipation and entropy. Nat Chem. 2016 Jul;8(7):678-83. doi: 10.1038/nchem.2506. Epub 2016 May 02. PMID: 27325094.
Copy Download .nbib Format: NLM
Share it on

Nat Chem. 2016 Jul;8(7):678-83. doi: 10.1038/nchem.2506. Epub 2016 May 02.

Imaging single-molecule reaction intermediates stabilized by surface dissipation and entropy.

Nature chemistry

Alexander Riss, Alejandro Pérez Paz, Sebastian Wickenburg, Hsin-Zon Tsai, Dimas G De Oteyza, Aaron J Bradley, Miguel M Ugeda, Patrick Gorman, Han Sae Jung, Michael F Crommie, Angel Rubio, Felix R Fischer

Affiliations

  1. Department of Physics, University of California, Berkeley, California 94720, USA.
  2. Institute of Applied Physics, Vienna University of Technology, 1040 Wien, Austria.
  3. Nano-Bio Spectroscopy Group and ETSF, Universidad del País Vasco, 20018 San Sebastián, Spain.
  4. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
  5. Donostia International Physics Center, 20018 San Sebastián, Spain.
  6. Ikerbasque, Basque Foundation for Science, 48013 Bilbao, Spain.
  7. Centro de Física de Materiales CSIC/UPV-EHU-Materials Physics Center, 20018 San Sebastián, Spain.
  8. CIC nanoGUNE, 20018 San Sebastián, Spain.
  9. Department of Chemistry, University of California, Berkeley, California 94720, USA.
  10. Kavli Energy NanoSciences Institute at the University of California Berkeley and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
  11. Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany.
  12. Center for Free-electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany.

PMID: 27325094 DOI: 10.1038/nchem.2506

Abstract

Chemical transformations at the interface between solid/liquid or solid/gaseous phases of matter lie at the heart of key industrial-scale manufacturing processes. A comprehensive study of the molecular energetics and conformational dynamics that underlie these transformations is often limited to ensemble-averaging analytical techniques. Here we report the detailed investigation of a surface-catalysed cross-coupling and sequential cyclization cascade of 1,2-bis(2-ethynyl phenyl)ethyne on Ag(100). Using non-contact atomic force microscopy, we imaged the single-bond-resolved chemical structure of transient metastable intermediates. Theoretical simulations indicate that the kinetic stabilization of experimentally observable intermediates is determined not only by the potential-energy landscape, but also by selective energy dissipation to the substrate and entropic changes associated with key transformations along the reaction pathway. The microscopic insights gained here pave the way for the rational design and control of complex organic reactions at the surface of heterogeneous catalysts.

References

  1. J Am Chem Soc. 2014 Apr 16;136(15):5567-70 - PubMed
  2. Nano Lett. 2014 Nov 12;14(11):6127-31 - PubMed
  3. Nat Chem. 2010 Oct;2(10):821-5 - PubMed
  4. Nat Commun. 2013;4:2023 - PubMed
  5. Science. 2014 Mar 7;343(6175):1120-2 - PubMed
  6. Sci Rep. 2014 Jan 28;4:3899 - PubMed
  7. Nat Nanotechnol. 2007 May;2(5):285-9 - PubMed
  8. ACS Nano. 2013 Sep 24;7(9):8190-8 - PubMed
  9. Nat Commun. 2012;3:1286 - PubMed
  10. J Phys Chem A. 2007 Jul 5;111(26):5678-84 - PubMed
  11. Phys Rev Lett. 2014 Oct 31;113(18):186102 - PubMed
  12. Science. 2009 Aug 28;325(5944):1110-4 - PubMed
  13. J Am Chem Soc. 2013 Jun 12;135(23):8448-51 - PubMed
  14. Chem Commun (Camb). 2014 Aug 21;50(65):9034-48 - PubMed
  15. Nat Commun. 2014 May 30;5:3931 - PubMed
  16. Phys Rev Lett. 2014 Nov 28;113(22):226101 - PubMed
  17. J Am Chem Soc. 2015 Feb 11;137(5):1833-43 - PubMed
  18. ACS Nano. 2014 Jul 22;8(7):6571-9 - PubMed
  19. Science. 2012 Sep 14;337(6100):1326-9 - PubMed
  20. Science. 2013 Nov 1;342(6158):611-4 - PubMed
  21. J Am Chem Soc. 2014 Jan 29;136(4):1609-16 - PubMed
  22. Chem Commun (Camb). 2013 Apr 11;49(28):2900-2 - PubMed
  23. ACS Nano. 2014 Mar 25;8(3):3006-14 - PubMed
  24. Science. 2013 Jun 21;340(6139):1434-7 - PubMed
  25. Phys Rev Lett. 2000 Sep 25;85(13):2777-80 - PubMed
  26. Angew Chem Int Ed Engl. 2014 Apr 25;53(18):4721-4 - PubMed
  27. Nat Chem. 2011 Jan;3(1):61-7 - PubMed
  28. Angew Chem Int Ed Engl. 2013 Apr 2;52(14):4024-8 - PubMed
  29. Nano Lett. 2013 Oct 9;13(10):4840-3 - PubMed
  30. Nano Lett. 2014 May 14;14(5):2251-5 - PubMed
  31. ACS Nano. 2015 Mar 24;9(3):2574-83 - PubMed

Publication Types