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Issue 46, 2016
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Substrate co-doping modulates electronic metal–support interactions and significantly enhances single-atom catalysis

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Abstract

Transitional metal nanoparticles or atoms deposited on appropriate substrates can lead to highly economical, efficient, and selective catalysis. One of the greatest challenges is to control the electronic metal–support interactions (EMSI) between the supported metal atoms and the substrate so as to optimize their catalytic performance. Here, from first-principles calculations, we show that an otherwise inactive Pd single adatom on TiO2(110) can be tuned into a highly effective catalyst, e.g. for O2 adsorption and CO oxidation, by purposefully selected metal–nonmetal co-dopant pairs in the substrate. Such an effect is proved here to result unambiguously from a significantly enhanced EMSI. A nearly linear correlation is noted between the strength of the EMSI and the activation of the adsorbed O2 molecule, as well as the energy barrier for CO oxidation. Particularly, the enhanced EMSI shifts the frontier orbital of the deposited Pd atom upward and largely enhances the hybridization and charge transfer between the O2 molecule and the Pd atom. Upon co-doping, the activation barrier for CO oxidation on the Pd monomer is also reduced to a level comparable to that on the Pd dimer which was experimentally reported to be highly efficient for CO oxidation. The present findings provide new insights into the understanding of the EMSI in heterogeneous catalysis and can open new avenues to design and fabricate cost-effective single-atom-sized and/or nanometer-sized catalysts.

Graphical abstract: Substrate co-doping modulates electronic metal–support interactions and significantly enhances single-atom catalysis

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Publication details

The article was received on 27 May 2016, accepted on 06 Oct 2016 and first published on 07 Oct 2016


Article type: Paper
DOI: 10.1039/C6NR04292A
Citation: Nanoscale, 2016,8, 19256-19262
  • Open access: Creative Commons BY license
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    Substrate co-doping modulates electronic metal–support interactions and significantly enhances single-atom catalysis

    J. L. Shi, J. H. Wu, X. J. Zhao, X. L. Xue, Y. F. Gao, Z. X. Guo and S. F. Li, Nanoscale, 2016, 8, 19256
    DOI: 10.1039/C6NR04292A

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