Large-scale synthesis of multi-walled carbon nanotubes in a continuous inclined mobile-bed rotating reactor by the catalytic chemical vapour deposition process using methane as carbon source

Multi-walled carbon nanotubes (CNTs) were produced in a continuous inclined mobile-bed rotating reactor by the catalytic chemical vapour deposition of methane on a bimetallic Ni–Mo/MgO catalyst whose activity remains constant in the course of time. Measurements performed on the continuous reactor were validated to ensure that the installation worked correctly and that measurements were precise enough. The performance of the reactor was simulated using a model based on the chemical reactor engineering approach. Hypotheses of the model were verified, and a kinetic study was performed to obtain a kinetic rate expression and to determine the catalytic activity as a function of time. The purity level of produced CNTs depends on the desired properties of the product, so the operating conditions are linked to the purity level that is required. A minimal purity level corresponds to high carbon production, and a maximal purity level corresponds to high specific productivity. It was shown that operating conditions had to be fixed to reach a given specific productivity or a given carbon production, and the optimized operating conditions leading to those two opposite purity level objectives were established.

► Production of CNTs in a continuous rotating reactor by CCVD. ► Use of a catalyst that keeps its initial catalytic activity level during synthesis. ► This is a crucial point for industrial large-scale carbon nanotube production. ► Validation of performed measurements and modelling of the reactor. ► Determination of operating conditions relevant to a given purity level.