4.8 Article

Bulky nanodiamond-confined synthesis of sub-5 nanometer ordered intermetallic Pd3Pb catalysts

Journal

NANO RESEARCH
Volume 15, Issue 6, Pages 4973-4979

Publisher

TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4138-4

Keywords

Pd3Pb intermetallic compound; bulky nanodiamond; strong metal-support interaction; alkynes semihydrogenation

Funding

  1. National Key Research and Development Program of China [2018YFA0702001]
  2. National Natural Science Foundation of China [22071225]
  3. Fundamental Research Funds for the Central Universities [WK2060190103]
  4. Joint Funds from Hefei National Synchrotron Radiation Laboratory [KY2060000175]

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The synthesis of small-sized Pd3Pb intermetallic nanocatalysts with improved catalytic performance is achieved by using a bulky nanodiamond-confined method. The resulting catalyst exhibits high activity and selectivity under mild conditions.
Modulation of geometric and electronic structures of supported Pd-based catalysts by forming atomically ordered intermetallic phases enables an effective way to optimize catalytic performance. However, the synthesis of small-sized Pd-based intermetallic nanoparticle catalysts with improved mass-based activity remains formidable challenges, since high-temperature annealing generally required for atom ordering inevitably leads to severe metal sintering and thus large crystallites. Here, we present a bulky nanodiamond-confined method to prepare sub-5 nm Pd3Pb intermetallic nanocatalysts by mitigating metal sintering at high temperatures, which is induced by the electronic interactions between metal and defect-rich graphene shells reinforced by diamond cores in the bulky nanodiamond support. The prepared small-sized Pd3Pb intermetallic catalyst displays a high activity with a turnover frequency of 932 h(-1) for the semihydrogenation of phenylacetylene under mild conditions (room temperature, 3 bar H-2), along with a high selectivity of > 96% to styrene near the complete conversion of phenylacetylene.

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