Pronounced interfacial interaction in icosahedral Au@C60 core-shell nanostructure for boosting direct plasmonic photocatalysis under alkaline condition

doi:10.1016/j.jmst.2021.02.062

Abstract

Abstract:

The unique hot carrier-driven direct plasmonic photocatalysis of coinage metal nanomaterials (NMs) via energetic localized surface plasmon resonance (LSPR) in visible-light region has been explored in recent years. However, the low photoinduced electron transfer efficiency and insufficient separation of electron-hole pairs would severely preclude their widespread practical applications. Herein, we demonstrate an interesting plasmonic photocatalyst based on the construction of icosahedral (Ih) Au@C₆₀ core-shell NMs, taking advantage of specific delocalized π electrons structure of a tight C₆₀ shell and enhanced LSPR property of Ih Au core. Then, the pronounced interfacial interaction at junction region endows the obtained Au@C₆₀ NMs with an outstanding photoinduced hot carrier-transmission during photocatalytic reaction, facilitating a remarkably higher (1.89 times) photocatalytic activity toward visible-light driven degradation of crystal violet (CV) dyes, as compared to bare Au NMs. Impressively, the photocatalytic activity of Ih Au@C₆₀ NMs can be effectively optimized by changing the pH value of reaction solution, with the kinetic rate constant reaching the maximum value of 0.179 min^-1 in pH₀ 11.4 solution, while 0.005 min^-1 at pH₀ 3.0. Moreover, due to the protection of a tight C₆₀ shell, the Ih Au@C₆₀ NMs also possess excellent photocatalytic stability/reusability in recycling runs, holding great potential for the design of robust and high-performance plasmonic photocatalysts in repeated practical applications.

Key words: Direct plasmonic photocatalysis, Icosahedral Au@C₆₀ core-shell nanostructure, Localized surface plasmon resonance, Delocalized π electrons;, Photocatalytic degradation

Yue Tian, Qingqiang Cui, Linlin Xu, Anxin Jiao, Shuang Li, Xuelin Wang, Ming Chen. Pronounced interfacial interaction in icosahedral Au@C₆₀ core-shell nanostructure for boosting direct plasmonic photocatalysis under alkaline condition[J]. J. Mater. Sci. Technol., 2021, 94: 10-21.

Figures/Tables 12

Scheme 1. Schematics of plasmon-induced generation of hot carriers on Ih Au@C60 core-shell NMs and the mechanism of charge separation and photocatalytic process under broad-spectrum light irradiation.

Fig. 1. (a, b) Low and enlarged magnification TEM images of spherical Au@C60 core-shell NPs. (c) The HRTEM image of an individual Au@C60 NPs.

Fig. 2. Morphology and structural characterizations of the obtained Ih Au@C60 NMs. (a, b) SEM and (c, d) TEM and HRTEM images. (e) SAED pattern. (f) Cross-sectional compositional line profile. (g) Raman spectrum of Ih Au@C60 NMs.

Fig. 3. (a) XRD patterns of Ih Au@C60 NMs, spherical Au@C60 NPs and Au NPs. (b) UV-visible absorption spectra of these three samples. (c) Down-converted photoluminescence spectra of C60. (d) Spectral overlap of C60 emission and Ih Au@C60 NMs absorption spectrum, both peaks are normalized.

Fig. 4. High-resolution XPS spectra of C1s on the surface of (a) C60, O1s on the surfaces of (b) Au NPs and (c) Ih Au@C60 NMs. (d) The detailed structure information of Au NPs and Ih Au@C60 NMs.

Fig. 5. (a) SERS spectra of 10-7 M CV adsorbed on Ih Au@C60 NMs, spherical Au@C60 NPs and bare Au NPs, respectively. The excitation wavelength is 633 nm. (b) FDTD calculations of near-field distributions for Au NPs and Ih Au with excitation of 633 nm. Einc is parallel to the y axis.

Fig. 6. (a) Temporal evolution of UV-vis absorption spectra of CV dyes during the photocatalytic degradation in the presence of Ih Au@C60 NMs under visible light irradiation. (b) Photocatalytic degradation of CV as a function of irradiation time, (c) kinetic linear simulation and (d) the corresponding rate constant (k) histogram of visible-light-driven photocatalytic performances in Ih Au@C60 NMs, spherical Au@C60 NPs and Au NPs systems.

Fig. 7. Based on the obtained Ih Au@C60 photocatalyst, the absorption spectra of CV dyes after photocatalytic degradation of 3 h by using three laser sources with wavelength of 532, 635 and 808 nm, respectively. (b) Degradation rate of CV dyes as a function of the laser wavelength. Overlaid (black line) is the UV-visible absorption spectrum of Ih Au@C60 NMs. FDTD calculations of near-field distributions of Ih Au nanostructure with excitation of 532 nm (c1), 635 nm (c2) and 808 nm (c3), respectively. Einc is parallel to the y axis.

Fig. 8. (a) Transient photocurrent responses of Ih Au@C60 NMs, spherical Au@C60 NPs and bare Au NPs in 0.1 M Na2SO4 under visible light irradiation. (b) The photocurrent density of three samples at 200 s.

Fig. 9. (a) The influence of different capture agents on photocatalytic performance of Ih Au@C60 NMs. (b) ESR spectra of the DMPO-•OH recorded on Ih Au@C60 NMs, bare Au NPs and original C60 powders under visible light irradiation.

Fig. 10. (a-c) Influence of pH0 on the photocatalytic degradation of CV dyes in the presence of Ih Au@C60 NMs. (d) High resolution XPS spectra of O1s region on the surface of Ih Au@C60 at pH0 11.4.

Fig. 11. Recycling runs of photocatalytic degradation of CV dyes under visible light irradiation at pH0 11.4 in the presence of Ih Au@C60 powders (a) and flexible film (c). (b) Digital photos of flexible Ih Au@C60 film and the mixed CV solution before and after a typical photocatalytic reaction. (d) The XRD pattern and (e) SEM image of Ih Au@C60 NMs after 10 cycles of repeated applications.

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Pronounced interfacial interaction in icosahedral Au@C₆₀ core-shell nanostructure for boosting direct plasmonic photocatalysis under alkaline condition

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