Catalytic performance of dioxide reforming of methane over Co/AC-N catalysts: Effect of nitrogen doping content and calcination temperature

摘要

The nitrogen doped activated carbon (AC-N) has been successfully prepared with commercial activated carbon as carbon material followed by a simple N-doping method using melamine as nitrogen sources. Using AC-N as the supports, cobalt supported on N-doped activated carbon (Co/AC-N) were developed and used as catalyst for dry reforming reaction (DRM). It was discovered that the Co/AC-N catalysts revealed much higher catalytic performance for DRM reaction in comparison to activated carbon supported cobalt catalyst (Co/AC). Moreover, the catalytic activity was influenced by preparation conditions of AC-N such as calcination temperature and the doping amount of nitrogen. The catalysts were characterized by BET, XRD, XPS, H-2-TPR, Raman spectroscopy and TEM. It was found that catalytic activities of the catalysts with different calcination temperature and nitrogen doping were influenced by catalyst surface defects and disorders, Co2+/Co3+ molar ratio, the content of nitrogen function groups (graphitic N, pyrrolic-N and pyridinic-N) and interaction between active metal and support. The Raman spectroscopy illustrated that the N-doped catalyst surface defects and disorders increased, which improved the performances of the Redox catalysts. The XPS valence band also revealed that higher Co2+/Co3+ molar ratio and nitrogen function groups was achieved by decreasing calcination temperature and increasing nitrogen doping. In short, the doping of nitrogen increased the structural defects and the interaction between active metals and supports, modified the surface electronic structure, which were facilitated the oxidation and reduction of methane and carbon dioxide. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.