Solvent-free microwave-assisted synthesis of tenorite nanoparticle-decorated multi-walled carbon nanotubes

doi:10.1016/j.jmst.2019.01.002

Abstract

Abstract:

Copper-decorated carbon nanotubes (CNTs) have important applications as precursors for ultra-conductive copper wires. Tenorite-decorated CNTs (CuO-CNTs) are ideal candidates and are currently developed using laborious processes. For this reason, we have developed a facile and scalable method for the synthesis of CuO-CNTs from copper acetate. It was found that the optimal loading of copper acetate onto the CNTs was 23.1 wt% and that three 1-minute microwave treatments were sufficient for the decomposition of copper acetate to copper oxide. The loading of copper oxide onto the nanotubes was confirmed using X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy and thermogravimetric analysis. The materials were characterised using X-ray diffraction and scanning electron microscopy.

Key words: Microwave-assisted synthesis, Multi-walled carbon nanotubes, Tenorite, Nanoparticle

Jennifer A. Rudd, Cathren E. Gowenlock, Virginia Gomez, Ewa Kazimierska, Abdullah M. Al-Enizi, Enrico Andreoli, Andrew R. Barron. Solvent-free microwave-assisted synthesis of tenorite nanoparticle-decorated multi-walled carbon nanotubes[J]. J. Mater. Sci. Technol., 2019, 35(6): 1121-1127.

Figures/Tables 12

Table 1 As-prepared loadings of copper acetate and copper in MWCNT samples. The amount of MWCNTs was fixed to 10 mg for all samples. Detailed calculations of Cu loadings are provided in Section 1 of the Supplementary Material (SM).

CuAc stock solution [mL]	CuAc loading [wt%]	Cu loading [Cu/(Cu + C) at. wt%]
9.0 (9.0 mg CuAc)	47.4	19.4
6.0 (6.0 mg CuAc)	37.5	14.6
3.0 (3.0 mg CuAc)	23.1	8.4
2.0 (2.0 mg CuAc)	16.7	5.9
1.0 (1.0 mg CuAc)	9.1	3.1
0.5 (0.5 mg CuAc)	4.8	1.6
0.1 (0.1 mg CuAc)	1.0	0.3

Fig. 1. A schematic representation showing the process of decoration of CNTs with tenorite nanoparticles. Blue spheres: CuAc; black spheres: CuO.

Fig. 2. SEM images of (a) MWCNTs decorated with CuO after three microwave treatments (CuAc loading 47.4 wt%) at low magnification, and (b and c) enlarged sections of image (a) showing individual nanoparticles of CuO.

Fig. 3. SEM images of (a) MWCNTs decorated with CuO after three microwave treatments (47.4 wt% CuAc initial loading) at low magnification, (b) enlarged section of image (a) with a tenorite nanoparticle. (c) EDX map superimposed on SEM image (b) showing the distribution of carbon, copper, oxygen, iron and indium, (d) EDX spectrum for the framed area in image (b), and (e-g) EDX individual maps for the carbon, copper, and oxygen, respectively.

Fig. 4. TEM images of tenorite nanoparticles decorating MWCNTs from (a) 9.1 wt% and (b) 47.4 wt% CuAc initial loading. Inset, higher magnification image of the CuO nanoparticle.

Fig. 5. Amount of copper acetate remaining unconverted on MWCNTs after an increasing number of 1-min microwave treatments. Comparison between two different initial loadings of CuAc: diamonds 47.4 wt%, squares 9.1 wt%.

Fig. 6. XRD patterns of MWCNTs with 47.4 wt% (red) and without (black) added copper acetate, after three microwave treatments. Miller indices refer to CuO (red) and MWCNTs (black) reflections.

Fig. 7. Copper loading in MWCNT samples measured using EDX plotted against the amount of copper from CuAc used during preparation (Table 1). Black circles and bars correspond to before microwave treatment, whilst red circles and bars are after three microwave treatments. The range bars represent the upper and lower limits of the spread of data. Each analysis is expressed as the average of three probed areas.

Fig. 8. (a) Representative Cu(2p) peaks from 90 wt% added CuAc sample after three microwave treatments, with fittings. (b) Representative C(1 s) peak from 30 wt% added CuAc sample after three microwave treatments with fitting.

Fig. 9. Copper loading in MWCNT samples measured using EDX (black circles) and XPS (red circles) after three microwave treatments plotted against the amount of copper from CuAc used during preparation (Table 1). For EDX, the range bars represent the upper and lower limits of the spread of data from at least three measurements. For XPS, one region scan was taken for each sample.

Fig. 10. TGA of pure copper acetate (black line), tenorite-decorated MWCNT samples after three microwave treatments (orange, green, and blue lines), and as received MWCNTs (red line).

Fig. 11. Copper loading in MWCNT samples measured using TGA after three microwave treatments plotted against the amount of copper from CuAc used during preparation (Table 1). The dashed diagonal line represents the expected copper loading when the only process occurring while microwaving is the conversion of CuAc to tenorite, without loss of carbon.

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