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The effects of additives containing iron or nickel during chemical vapor deposition (CVD) on the growth of carbon nanotubes (CNTs) by methane decomposition on Mo/MgO catalyst were investigated. Ferrocene and nickel nitrate were introduced as deactivation inhibitors by in-situ evaporation during CVD. The precisely controlled in-situ introduction of these inhibitors increased the surface renewal of catalyst, and therefore prevented the catalyst from deactivation. Using this method, aligned multi-walled CNTs with parallel mesopores can be produced on a large scale.