Abstract
The NiO-MgO solid solution has been proven to be an efficient catalyst for the carbon dioxide reforming of methane (CRM). However, the challenge is still there for the facilely controlled synthesis of the single-phase solid solution with the uniform composition, and the interactions between NiO and MgO are not consistently correlated with the CRM performance. To address these issues, in this work, the complex-decomposition method was applied to regulate the chemical and structural properties of NiO-MgO catalysts via simply changing the complexing agent, calcination temperature, and Ni/Mg molar ratio. The catalysts were comparatively evaluated for CRM under severe reaction conditions of 750 °C, 0.1 MPa, CH4/CO2 = 1, and a gas hourly space velocity of 60000 mL·g−1·h−1. Irrespective of the complexing agents investigated, NiO-MgO solid solution was exclusively formed. However, the structural and reductive properties of the NiO-MgO catalysts were strongly dependent on the complexing agent, which is reasonably explained as the varied coordinative capabilities of the complexing agent with the metal cations. Moreover, the highest CRM performance, i.e., the initial CH4 conversion of ~86% kept constant for a time-on-stream of 20 h, was achieved over the Ni0.1Mg0.9O catalyst by using glycine as the complexing agent and calcined at 800 °C. The characterization and CRM results vigorously confirmed that a good balance between the sintering and the in situ release of active metallic Ni under CRM reaction conditions was constructed over the NiO-MgO catalyst prepared using glycine as the complexing agent, leading to its highest stability. Considering the simple procedure of the complex-decomposition method and the convenient adjustment of the NiO and MgO interactions by simply changing the complexing agent and calcination temperature, the thus developed catalyst can be applied for extensive understanding the CRM mechanism, and extended for large-scale preparation.