One-step preparation of a N-CNTs@Ni foam electrode material with the co-production of H2 by catalytic reforming of N-containing compound of biomass tar

Abstract

Carbon nanotubes (CNTs) can be formed during catalytic reforming of hydrocarbons with H2 co-production over Ni-based catalysts. Normally, the formed CNTs need to be separated from original catalysts in order to be coated on the substrates to make high performance electrodes. To simplify the traditional preparation process, a novel one-step method for simultaneously producing a CNTs electrode material and H2 was proposed. A Ni-Fe modified Ni foam (Ni-Fe/NF) was chosen as both catalyst and electrode substrate to in situ grow nitrogen-doped carbon nanotubes (N-CNTs) during catalytic reforming of pyrrole. Pyrrole was selected as an N-containing model compound of biomass tar. The results showed that Ni-Fe nanoparticles on Ni-Fe/NF catalyst remarkably improved the H2 production and pyrrole conversion, which increased by more than 20 times than those of fresh Ni foam. Besides, a significant amount of multi-walled CNTs with more than 40 graphite layers grew on the surface of spent catalyst and their diameters were mainly from 10 nm to 20 nm. N element was detected on the formed CNTs and the Graphitic-N was the main type of N-doping. The spent catalyst (N-CNTs@Ni foam) can be directly used as a composite electrode material with high performance and stability. Its electrochemical capacitance reached 855 mF/cm2 at a current density of 5 mA/cm2 and remained over 95% after 10,000 cycles.