Relationship between dealloying conditions and coarsening behaviors of nanoporous copper fabricated by dealloying Cu-Ce metallic glasses

doi:10.1016/j.jmst.2017.11.043

Abstract

Abstract:

Monolithic nanoporous copper (NPC) with tunable ligament size (107-438 nm) was synthesized by dealloying a new Cu-Ce binary glassy precursor in dilute H₂SO₄ aqueous solution. The effects of the dealloying conditions on the morphologies of NPC were evaluated comprehensively. The results show that the ligaments of NPC can significantly coarsen with the increase of acid concentration, elevation of reaction temperature or prolongation of immersion time. These coarsening behaviors can be well described by a diffusion based growth kinetic model. Moreover, the surface diffusivity and activation energy for diffusion of Cu atoms were also estimated to investigate the formation mechanism of NPC, which is mainly governed by dissolution of Ce element in the glassy precursor coupled with nucleation and growth of Cu clusters via the precursor/solution interface. In the experiment of the degradation of methyl orange (MO) dye, the NPC fabricated by Cu-Ce metallic glasses exhibits superior sono-catalytic activity.

Key words: Cu-Ce metallic glasses, Nanoporous copper, Dealloying, Diffusion, Sono-Fenton-like

Ning Wang, Ye Pan, Shikai Wu. Relationship between dealloying conditions and coarsening behaviors of nanoporous copper fabricated by dealloying Cu-Ce metallic glasses[J]. J. Mater. Sci. Technol., 2018, 34(7): 1162-1171.

Figures/Tables 11

Fig. 1. XRD patterns of (a) Cu74Ce26 metallic glasses and (b) corresponding sample after dealloying in 0.1 mol L-1 H2SO4 aqueous solution at 333 K for 90 min.

Fig. 2. SEM images of samples by dealloying Cu74Ce26 metallic glasses at 333 K for 90 min in (a) 0.04 mol L-1, (b) 0.1 mol L-1, (c) 0.2 mol L-1, (d) 0.4 mol L-1 H2SO4 aqueous solution and (e) typical EDS spectrum of Fig. 2(b).

Fig. 3. SEM images of samples by dealloying Cu74Ce26 metallic glasses in 0.1 mol L-1 H2SO4 aqueous solution for 90 min at various temperatures: (a) 313 K; (b) 323 K; (c) 333 K.

Fig. 4. SEM images of samples by dealloying Cu74Ce26 metallic glasses in 0.1 mol L-1 H2SO4 aqueous solution at 333 K for various immersion time: (a) 90 min; (b) 120 min; (c) 240 min; (d) 270 min; (e) 360 min.

Fig. 5. (a) TEM and (b) HRTEM images of NPC by dealloying Cu74Ce26 metallic glasses in 0.1 mol L-1 H2SO4 aqueous solution at 333 K for 90 min. The insets in (a) and (b) show the corresponding selected area diffraction and fast Fourier transformation patterns, respectively.

Fig. 6. (a) Cross-sectional SEM image of NPC by dealloying Cu74Ce26 metallic glasses in 0.1 mol L-1 H2SO4 aqueous solution at 333 K and (b) EDS line scan of cross section.

Fig. 7. Schematic illustrations showing nucleation and growth mechanisms of NPC by dealloying Cu-Ce metallic glasses: (a) dissolution of Ce atoms; (b) agglomeration of Cu atoms; (c) formation of Cu ligaments; (d) coarsening of Cu ligaments.

Fig. 8. (a) Relationship between immersion time (t) and ligament size (d) of NPC by dealloying Cu74Ce26 metallic glasses and (b) plot of lnd vs. lnt for deriving coarsening exponent (n).

Fig. 9. (a) Relationship between temperature (T) and ligament size (d) of NPC by dealloying Cu74Ce26 metallic glasses, (b) plot of lnd vs. 1000/T for deriving the activation energy (Ea) and (c) Arrhenius plot of natural logarithm of surface diffusivity, lnDs vs. 1000/T.

Fig. 10. (a) Relationship between sulfuric acid concentration (c) and ligament size (d) of NPC by dealloying Cu74Ce26 metallic glasses and (b) plot of lnd vs. lnc.

Fig. 11. (a) Sonocatalytic degradation of MO versus reaction time, (b) linear transformation ln (C/C0) of the kinetic curves of MO degradation and (c) four recycling runs of NPC for degradation of MO.

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