A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
[Pt2Cu34(PET)22Cl4]2–: An Atomically Precise, 10-Electron PtCu Bimetal Nanocluster with a Direct Pt–Pt Bond (2021)


Lee, S., Bootharaju, M. S., Deng, G., Malola, S., Häkkinen, H., Zheng, N., & Hyeon, T. (2021). [Pt2Cu34(PET)22Cl4]2–: An Atomically Precise, 10-Electron PtCu Bimetal Nanocluster with a Direct Pt–Pt Bond. Journal of the American Chemical Society, 143(31), 12100-12107. https://doi.org/10.1021/jacs.1c04002


JYU-tekijät tai -toimittajat


Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Lee, Sanghwa; Bootharaju, Megalamane S.; Deng, Guocheng; Malola, Sami; Häkkinen, Hannu; Zheng, Nanfeng; Hyeon, Taeghwan

Lehti tai sarja: Journal of the American Chemical Society

ISSN: 0002-7863

eISSN: 1520-5126

Julkaisuvuosi: 2021

Volyymi: 143

Lehden numero: 31

Artikkelin sivunumerot: 12100-12107

Kustantaja: American Chemical Society (ACS)

Julkaisumaa: Yhdysvallat (USA)

Julkaisun kieli: englanti

DOI: https://doi.org/10.1021/jacs.1c04002

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Tiivistelmä

Heteroatom-doped metal nanoclusters (NCs) are highly desirable to gain fundamental insights into the effect of doping on the electronic structure and catalytic properties. Unfortunately, their controlled synthesis is highly challenging when the metal atomic sizes are largely different (e.g., Cu and Pt). Here, we design a metal-exchange strategy that enables simultaneous doping and resizing of NCs. Specifically, [Pt2Cu34(PET)22Cl4]2– NC, the first example of a Pt-doped Cu NC, is synthesized by utilizing the unique reactivity of [Cu32(PET)24Cl2H8]2– NC with Pt4+ ions. The single-crystal X-ray structure reveals that two directly bonded Pt atoms occupy the two centers of an unusually interpenetrating, incomplete biicosahedron core (Pt2Cu18), which is stabilized by a Cu16(PET)22Cl4 shell. The molecular structure and composition of the NC are validated by combined experimental and theoretical results. Electronic structure calculations, using the density functional theory, show that the Pt2Cu34 NC is a 10-electron superatom. The computed absorption spectrum matches well with the measured data and allows for assignment of the absorption peaks. The calculations also rationalize energetics for ligand exchange observed in the mass spectrometry data. The synergistic effects induced by Pt doping are found to enhance the catalytic activity of Cu NCs by ∼300-fold in silane to silanol conversion under mild conditions. Furthermore, our synthetic strategy has potential to produce Ni-, Pd-, and Au-doped Cu NCs, which will open new avenues to uncover their molecular structures and catalytic properties.


YSO-asiasanat: nanohiukkaset; nanorakenteet; metallit; molekyylit; kemialliset ominaisuudet


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OKM-raportointi: Kyllä

Alustava JUFO-taso: 3


Viimeisin päivitys 2021-11-08 klo 13:49