Preparation of carbon nano-microcoils by Ni3S2-catalyzed pyrolysis of acetylene and its vapor-liquid-solid-solid growth mechanism

摘要

Carbon microcoils are generally prepared by catalytic chemical vapor deposition of acetylene, using Ni as the catalyst and thiophene as the promoter. In this work, Ni3S2 was chosen as the catalyst on purpose to avoid the introducing of noxious and unpleasant thiophene during the reaction process. The products obtained in the temperature range of 1013-1033 K were pure, regular and had perfect morphology. Using transmission electron microscope, Raman spectrometer and X-ray diffractometer, the microstructure of the as-prepared carbon microcoils were characterized, furthmore, energy dispersive spectrum and selected area electron diffraction analysis reveal that the growth of carbon microcoils is always accomplished with the transformation of the catalyst from Ni3S2 to Ni3C. We first observed that the fiber constructing the carbon microcoil is composed of three sub-fibers, which strongly supports the proposition of vapor-liquid-solid-solid growth mechanism. In this mechanism, every catalyst particle is in the state of the coexistence of solid and liquid. Carbon atoms firstly permeate into the liquid portion from gas, then disperse into the solid portion, and finally deposit from the catalyst grain to form the carbon microcoil.