Influence of reduction conditions on the structure-activity relationships of NaNO3-promoted Ni/MgO dual function materials for integrated CO2 capture and methanation

Abstract

Integrated CO2 capture and utilization (ICCU) represents an innovative concept and technique for reducing industrial carbon emissions. Ni-MgO dual function materials (DFMs) promoted by alkali metal salt (AMS) for integrated CO2 capture and methanation (ICCU-M) is gaining increasing interest. The in-situ methanation performance depends heavily on the high-temperature NiO reduction process, while this might adversely affect CO2 adsorption due to loss of AMS. Herein, we investigated the effects of H2 concentration and reduction temperature on structure–activity relationships of AMS-promoted Ni-MgO DFMs for ICCU-M. The increase in H2 concentration and reduction temperature favors NiO reduction to metallic Ni0 and boosts oxygen vacancy concentration in the DFMs. Both CO2 uptakes and CH4 yield increase with the elevating H2 concentration, and CH4 yield also increases with the increasing reduction temperature, considering the increased metallic Ni0 content and oxygen vacancy concentration. CO2 uptakes of the DFMs decline with the increase in reduction temperature, due to the obvious loss in AMS. The bulk diffusion kinetics in CO2 adsorption stage will be improved under higher H2 concentration and reduction temperature, while the chemisorption kinetics will be weakened at elevating reduction temperature. The methanation kinetics will be enhanced when the DFMs are reduced under higher H2 concentration and temperature. The AMS-NM-100-450 DFMs reduced in 100 %H2 and 450 °C exhibit good ICCU-M performance with high CO2 adsorption capacity and CH4 yield of 6.46 mmol CO2/g and 0.85 mmol CH4/g. The results in this work enlighten that the ICCU-M performance of AMS promoted Ni-MgO DFMs can be tuned by regulating the operating parameters for catalyst reduction.