Microwave plasma-based high temperature dehydrogenation of hydrocarbons and alcohols as a single route to highly efficient gas phase synthesis of freestanding graphene

článek v časopise ve Web of Science, Jimp

angličtina

Understanding underlying processes behind the simple and easily scalable graphene synthesis methods enables their large-scale deployment in the emerging energy storage and printable device applications. Microwave plasma decomposition of organic precursors forms a high-temperature environment, above 3000 K, where the process of catalyst-free dehydrogenation and consequent formation of C-2 molecules leads to nucleation and growth of high-quality few-layer graphene (FLG). In this work, we show experimental evidence that a high-temperature environment with a gas mixture of H-2 and acetylene, C2H2, leads to a transition from amorphous to highly crystalline material proving the suggested dehydrogenation mechanism. The overall conversion efficiency of carbon to FLG reached up to 47%, three times as much as for methane or ethanol, and increased with increasing microwave power (i.e. with the size of the high-temperature zone) and hydrocarbon flow rate. The yield decreased with decreasing C:H ratio while the best quality FLG (low D/G-0.5 and high 2D/G-1.5 Raman band ratio) was achieved for C:H ratio of 1:3. The structures contained less than 1 at% of oxygen. No additional hydrogen was necessary for the synthesis of FLG from higher alcohols having the same stoichiometry, 1-propanol and isopropanol, but the yield was lower, 15%, and dependent on the atom arrangement of the precursor. The prepared FLG nanopowder was analyzed by scanning electron microscopy, Raman, x-ray photoelectron spectroscopy, and thermogravimetry. Microwave plasma was monitored by optical emission spectroscopy.

high temperature; dehydrogenation; graphene; growth mechanism; microwave plasma

JAŠEK, O.; TOMAN, J.; ŠNÍRER, M.; JURMANOVÁ, J.; KUDRLE, V.; MICHALIČKA, J.; VŠIANSKÝ, D.; PAVLIŇÁK, D.

10. 10. 2021

IOP Publishing Ltd

BRISTOL

1361-6528

Nanotechnology

32

50

Spojené království Velké Británie a Severního Irska

505608-1

505608-11

11

https://iopscience.iop.org/article/10.1088/1361-6528/ac24c3