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Towards stable catalysts by controlling collective properties of supported metal nanoparticles

Nature Materials volume 12, pages 3439 (2013) | Download Citation

Abstract

Supported metal nanoparticles play a pivotal role in areas such as nanoelectronics, energy storage/conversion1 and as catalysts for the sustainable production of fuels and chemicals2,3,4. However, the tendency of nanoparticles to grow into larger crystallites is an impediment for stable performance5,6. Exemplarily, loss of active surface area by metal particle growth is a major cause of deactivation for supported catalysts7. In specific cases particle growth might be mitigated by tuning the properties of individual nanoparticles, such as size8, composition9 and interaction with the support10. Here we present an alternative strategy based on control over collective properties, revealing the pronounced impact of the three-dimensional nanospatial distribution of metal particles on catalyst stability. We employ silica-supported copper nanoparticles as catalysts for methanol synthesis as a showcase. Achieving near-maximum interparticle spacings, as accessed quantitatively by electron tomography, slows down deactivation up to an order of magnitude compared with a catalyst with a non-uniform nanoparticle distribution, or a reference Cu/ZnO/Al2O3 catalyst. Our approach paves the way towards the rational design of practically relevant catalysts and other nanomaterials with enhanced stability and functionality, for applications such as sensors, gas storage, batteries and solar fuel production.

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Acknowledgements

H. Meeldijk, M. Versluijs, R. van Zwienen and A. van der Eerden (Utrecht University) are acknowledged for high-angle annular dark-field STEM/energy-dispersive X-ray spectroscopy analysis, in situ XRD measurements, assistance with the high-pressure catalytic set-up and discussions on the X-ray absorption spectroscopy data, respectively. M. Watson, L. van de Water and C. Ranson (Johnson Matthey Catalysts) are thanked for the N2O reactive frontal chromatography measurements. The electron tomography study was carried out in the 3D Electron Microscopy group of Utrecht University headed by W. Geerts and J. A. Post. Beamline C at Hasylab (Hamburg) is acknowledged for the beam time allocated (project I-20110876 EC). This material is largely based on work supported as part of the Center for Atomic-Level Catalyst Design, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001058; further support from NRSCC and NWO is acknowledged.

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Affiliations

  1. Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, NL-3584 CG Utrecht University, The Netherlands

    • Gonzalo Prieto
    • , Jovana Zečević
    • , Krijn P. de Jong
    •  & Petra E. de Jongh
  2. Laboratory of Materials and Interface Chemistry, Eindhoven University of Technology, NL-5600 MB Eindhoven, The Netherlands

    • Heiner Friedrich

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Contributions

P.E.d.J. and K.P.d.J. conceived and coordinated the research. G.P. contributed to research conception, catalyst synthesis and methanol synthesis experiments. J.Z. recorded the TEM tilt series. J.Z. and G.P. reconstructed the electron tomograms and carried out image segmentation with guidance from H.F. G.P., with help from P.E.d.J., designed the routines and performed the particle growth simulations. The manuscript was primarily written by G.P. and P.E.d.J. All authors contributed to discussions and manuscript review.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to Krijn P. de Jong or Petra E. de Jongh.

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DOI

https://doi.org/10.1038/nmat3471

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