Letter | Published:

High-spatial-resolution mapping of catalytic reactions on single particles

Nature volume 541, pages 511515 (26 January 2017) | Download Citation


The critical role in surface reactions and heterogeneous catalysis of metal atoms with low coordination numbers, such as found at atomic steps and surface defects, is firmly established1,2. But despite the growing availability of tools that enable detailed in situ characterization3, so far it has not been possible to document this role directly. Surface properties can be mapped with high spatial resolution, and catalytic conversion can be tracked with a clear chemical signature; however, the combination of the two, which would enable high-spatial-resolution detection of reactions on catalytic surfaces, has rarely been achieved. Single-molecule fluorescence spectroscopy has been used to image and characterize single turnover sites at catalytic surfaces4,5, but is restricted to reactions that generate highly fluorescing product molecules. Herein the chemical conversion of N-heterocyclic carbene molecules attached to catalytic particles is mapped using synchrotron-radiation-based infrared nanospectroscopy6,7 with a spatial resolution of 25 nanometres, which enabled particle regions that differ in reactivity to be distinguished. These observations demonstrate that, compared to the flat regions on top of the particles, the peripheries of the particles—which contain metal atoms with low coordination numbers—are more active in catalysing oxidation and reduction of chemically active groups in surface-anchored N-heterocyclic carbene molecules.

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F.D.T. thanks the Director, Office of Science, Office of Basic Energy Sciences and the Division of Chemical Sciences, Geosciences, and Biosciences of the US Department of Energy at LBNL (DE-AC02-05CH11231) for partial support of this work. We thank the M. Raschke group at the University of Colorado for collaborating on the development of the SINS endstation. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract number DE-AC02-05CH11231. W.J.W. thanks the NSF for a predoctoral fellowship (DGE 1106400), and the Arnold Group (UCB) for use of their infrared spectrometer.

Author information


  1. Department of Chemistry, University of California, Berkeley, California 94720, USA

    • Chung-Yeh Wu
    • , William J. Wolf
    •  & F. Dean Toste
  2. Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, USA

    • Chung-Yeh Wu
    • , William J. Wolf
    •  & F. Dean Toste
  3. Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel

    • Yehonatan Levartovsky
    •  & Elad Gross
  4. The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel

    • Yehonatan Levartovsky
    •  & Elad Gross
  5. Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, USA

    • Hans A. Bechtel
    •  & Michael C. Martin


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E.G. and F.D.T. conceived the idea and co-wrote the paper. C.-Y.W. and W.J.W. prepared the carbene ligands and attached them to Pt and Au surfaces. Y.L. analysed the XPS measurements. H.A.B. and M.C.M. designed the SINS beamline and assisted in conducting the SINS measurements and analysing the data. E.G. performed the SINS experiments and analysed the data. All authors contributed to the overall scientific interpretation and edited the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to F. Dean Toste or Elad Gross.

Reviewer Information

Nature thanks C. Campbell, G. Rothenberg, F. Tao, B. Weckhuysen and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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